EPA-650/2-74-046-0
June 1974
Environmental  Protection  Technology Series
                                   I

                                                           LU
                                                           a

                                                                04 6

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                                          EPA-650/2-74-046-Q
DEVELOPMENT OF  A  GAS  LASER SYSTEM


         TO MEASURE TRACE  GASES


                BY  LONG PATH


         ABSORPTION TECHNIQUES:

       VOLUME I - GAS LASER SYSTEM  MODIFICATIONS

                FOR OZONE MONITORING

                     FINAL REPORT


                         by

                  S. E. Craig, D. R. Morgan,
               D. L. Roberts, and L. R. Snowman

                     General Electric
                  Electronic Systems Division
                    100 Plastics Avenue
                Pittsfield, Massachusetts  01201
                   Contract No. 68-02-0757

                     ROAP No. 26ACX

                 Program Element No. 1AA010
              EPA Project Officer: W.A.McClenny


               Chemistry and Physics Laboratory

              National Environmental Research Center

            Research Triangle Park, North Carolina 27711
                      Prepared for


             OFFICE OF RESEARCH AND DEVELOPMENT

            U.S. ENVIRONMENTAL PROTECTION AGENCY

                  WASHINGTON, D.C. 20460



                       June 1974

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This report has been reviewed by the Environmental Protection Agency
and approved for publication.  Approval does not signify that the
contents necessarily reflect the views and policies of the Agency,
nor does mention of trade names or commercial products constitute
endorsement or recommendation for use.
                                  11

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                               TABLE OF CONTENTS

                                                                       Page No.

A.  INTRODUCTION  	,....  1
B.  SIGNAL PROCESSOR  	  2
    1.  Introduction 	  2
    2.  Mini Computer Processor  	  5
             Interface Subsystem 	  6
             Central Processor Subsystem	  6
             Program Input and Data Logging Subsystem	8
    3.  Logic Block Diagram	9
    4.  Software 	  13
             Operational Modes	  13
             Collection Mode	  14
             Data Reduction and Display Mode	15
             Program Structure	16
    5.  Interface Unit	  21
C.  SPECTRAL STUDIES	  25

    1.  Introduction	  25
    2.  Spectral Data	,	28
             Introduction and Summary ,	  28
             Ozone (O )  	  34
                     3
             Carbon Dioxide (CO )	  36
                               £t
             Water Vapor (HO)	39
                           tt
             Ethylene (C H )	42
                       ti  4
             Ammonia (NH )	46
                         u
    3.  Wavelength Selection 	46
                                       III

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                            TABLE OF CONTENTS (Cont'd)
                                                                       Page No.
    4. Linear Weight Computation (MFIL)  	51
    5. Factor Analysis of Drift	55
D.  SPATIAL FILTER 	58
E.  SEALED E3OTOPIC LASER DESIGN	64
    1. Introduction	„	64
    2. Laser Plasma Tube Design Considerations	67
    3. Stability Considerations	72
    4. Intracavlty Windows	.72
    5. Spectral Tuner Design	74
    6. Sealed Laser Design Considerations	79
    7. Proposed Sealed Laser Design	84
F.  REFERENCES	87
                               APPENDICES

A.  INTERFERENCES	A-l
B.  OPTIMUM LINEAR WEIGHTS  	B-l
C.  WAVELENGTH SELECTION	C-l
D.  LWSP - LASER WAVELENGTH SELECTION PROGRAM	D-l
                                      Iv

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                                LIST OF ILLUSTRATIONS
                                                                           Page No.
Figure 1 - Signal Waveforms	  2
Figure 2 - Signal and Gating Waveforms	  4
Figure 3 - Data Collection and Reduction System	  7
Figure 4 - Logic Block Diagram  	   9
Figure 5 - Program Modification  	  12
Figure 6 - Sequence of Events	  23
Figure 7 - Composite Spectral Absorption In 9.4ji CO  Band	  31
                                                2
Figure 8 - Composite Differential Spectral Absorption In P-Branch	33
             of 9.4ji  CO  Band
Figure 9 - Ozone Absorption Coefficient Data Comparison in 9.4/i CO Band 	35
                                                               Lt
Figure 10 - CO  Coefficient Data Comparison	37
             A
Figure 11 - Comparison of the Continuum Absorption Coefficient at Three	41
             Temperatures
Figure 12 - Representative Spectrum of HO Between 800 and 1250 cm    	44
                                      Lt
Figure 13 - Spectrum of 383 Meters of Room Air at 750 Torr on a Rainy Day	45
Figure 14 - Resultant Line Selection From a 25 Iteration LWSP Run	48
Figure 15 - CMFIL Output Listing	  49
Figure 16 - Signal to Noise Ratio	50
Figure 17 - Spatial Filter Experiment Layout	  60
Figure 18 - Amplitude and Power Distribution of the Gaussian Fundamental Mode ... 61
Figure 19 - Contours of Equal Power Density	!	  63
Figure 20 - CO  Laslng Lines  	65
             2
Figure 21 - Calculated CO Isotope Band Centers	  66
Figure 22 - Radial Gain Profile	69
Figure 23 - Unsaturated Gain of a CO   Laser at a J-40 Transition	  70
                                 Lt

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                         LIST OF ILLUSTRATIONS (Cont'd)
                                                                         Page No.
Figure 24 - Layout of Laser Optical System	79
Figure 25 - Manifold for High Vacuum Fill Station	 82
Figure 26 - Proposed Sealed Isotoplc Laser Design  	 85

                             APPENDICES
Figure A-l Detector Noise Versus Frequency	A-"3
Figure A-2 Optical Scintillation Noise Versus Frequency	A-3
Figure B-l Possible Transmission Patterns for Single Absorbers	B-3
Figure B-2 Possible Transmission Patterns for Mixtures of Absorbers	B-3
Figure B-3 Possible Patterns for the Natural Log of the Transmission	B-5
Figure D-l Flow Chart of LWSP Program	D-?

                              LIST OF TABLES
Table I Absorption Coefficients for 00°1 - 02°0 (9.4 Micron) CO9 Band	29
Table TI Absorption Coefficients for 00°1 - 10°0 (10.4 Micron) CO2 Band	30
Table HI Relative CO  Absorption Coefficient Variation with  Pressure	38
                   Li
              and Temperature
Table IV Partial Tabulation of  HO Vapor Line Data	43
                              It
Table V Absorption Coefficients and CL Variance of Atmospheric Species	52
Table VI Linear Weights and SNR's for Atmospheric Species	 53
Table VH Cross Response of Linear Weights	54
Table VIII Eigenvector/Eigenvalue Analysis of Data Record  	56
Table DC Comparison of Factors and Atmospheric Species	57
Table X Losses Versus Mirror Tilt for a Confocal Resonator	71
Table C-l CMFIL Input Data	^-7
                                         vl

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A.  INTRODUCTION
       The Final Report of EPA Contract 68-02-0757, Development of a Gas Laser
System to Measure Trace Gases by Long Path Absorption Techniques consists of
two (2) volumes:
       I  Gas Laser System Modifications for Ozone Monitoring
      n  Field Evaluation of Gas Laser System for Ozone Monitoring
       The work reported here stems from development activity begun in 1966 at
GE's Electronics Laboratory.  Under this contract, a breadboard laser long path
monitor called ILAMS (Infrared Laser Atmospheric Monitoring System) was modified
to improve its sensitivity as indicated by previous field experience. System parameters
were selected to optimize system performance for ozone monitoring.  A field
evaluation of the modified system was conducted.
       In this volume of the Final Report,  the work of ILAMS modification and the
selection of system parameters, lasing wavelengths and linear weights,  is reported.
Significant system modifications included introduction of a spatial filter In the laser
output beam. In addition,  a digital signal processor was Incorporated In the system,
replacing an analog device.  The problems associated with Incorporating a sealed,
Isotoplc fill CO  laser were studied and a laser design proposed.  The selection of
              £t
the four laser wavelengths were preceded by extensive spectral  data collection to
determine the infrared absorption characteristics of target gases and expected Inter-
ferences. The selection process was facilitated by a previously developed computer
program. Similarly,  the calculation of linear weights was done on an existing computer
program.
       The change to digital processing was particularly important in the evolution of the
ILAMS design.  It greatly enhanced the flexibility of the system, offering significant
advantages over the analog approach as discussed in the next section.

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B.  SIGNAL PROCESSOR
1.  INTRODUCTION
      The spectrally scanning CO laser periodically steps through a number of
                               Lt
lasing modes. In each mode, the laser generates a quantity of energy at a par-

ticular wavelength.  Figure la.  Illustrates the energy output of the laser in time where

x (t) is the energy generated of wavelength,A   and  7"is the period of one scan.
 K                                        K y
     a. Laser Energy
        Output
« *"
X](t)


X2(t)




X3(t)


Xi(t+r)

x2l
_T
     b. Signal
        Return
        Energy


     c. Reference
        Preamp
        Output
     d. Return  K  T  X, (t)
        Signal       s\  KB T2 X2 (t)
                             KBT3X3(t)
Signal
Preamp
Output
     e. Normalized
        Return    ^
        Signal
         -d/c
                             KT2
                                                    T2 X 2 (t +T)
                               (K= KB/KA)
                                                                  TIME
                      Figure  1.  SIGNAL WAVEFORMS

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      This energy is transmitted over a path in which a spectral attenuation takes
 place that is dependent upon the nature of the medium.  Figure Ib.  illustrates the
 energy after passing through a medium where T  is the transmission of the medium
 at wavelength,
               'k.
      The desired information consists of the transmissions T   T   T
                                                           1,   2,  3, 	
 which characterize the  medium.  As shown in Figure la., the laser output at each
 wavelength is generally not constant from wavelength to wavelength, or even from
 period to period.  This problem necessitates the use of a  reference that directly
 senses the output of Figure la.  Conversion of the optical  energy  to an electrical
 signal is accomplished  with a suitable  IR detector followed by a preamplifier.  If
 the return signal, Figure Id. is  divided by the reference signal, Figure Ic., the
 desired information is obtained, as in  Figure le.

      Information is extracted at each wavelength by synchrounous demodulation
 which is performed by filtering or integrating gated portions of the signal.  Typical
 signal waveforms and gating signals are shown  in Figure 2. A null gate is also
provided in order to derive  a zero energy reference for dc restoration since the
 signal is ac coupled through the preamp.

      The normalization division process may take place before or after synchronous
demodulation as long as the reference signal-to-noise-ratio is large enough.
Division before synchronous demodulation requires a fast, stable divider and
necessitates state-of-the-art hardware for precision measurements.  On the other
hand, division after synchronous demodulation requires a  relatively slow separate
divider for each wavelength and twice as many synchronous demodulators.

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a.) Analytic Signal
b.) Reference Signal
c.) Null Gate
d.) Signal Gate

e.) Signal Gate #2  °
f.) Signal Gate #3 0





g.) Signal Gate ^4 0
JLJLJLJl
       ,  Figure 2. SIGNAL AND GATING WAVEFORMS

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      For large absorptions, logarithmic processing is desirable in order to
linearize the exponential transmission-concentration characteristic exhibited
by gases. Again, there is some choice as to where this transformation is applied.
If the signal-to-noise-ratio (SNR) is very high, then log processing can be accom-
plished before synchronous detection without any degradation in performance.
However, in general, it is preferable to do as much filtering as possible  before
the log conversion in order to maintain reliable performance.

      Linear weighted sums of the filtered log transmission measurements are then
derived in order to estimate the concentrations of particular atmospheric gases.
This technique is discussed in detail in Appendix B.

 2. MINI-COMPUTER PROCESSOR

       The mini-computer signal processor includes a general purpose (stored
 program) mini-computer and appropriate interface electronics.  The collection
 and reduction of data is entirely under computer,  i.e., program control; results
 are displayed on simple displays incorporated in the equipment, and on an optional
 teletype, which need not be used (or even be connected) during field or test range
 exercise of the  system.

       The use of the stored program control and data reduction means:
       •  changes in  system design, or variations in data reduction algorithms,
          may be accommodated without alteration of the data collection or re-
          duction hardware; only changes in the control program will be required.
       •   modification of signal processor parameters such as number of wave-
          lengths (up to 8), gate locations, system response time,  weighting
          factors, etc., do not  even require software changes,  these parameters
          are  expediently entered by the teletype input.
       •  the precision of data processing may be made as accurate as desired;
          similarly the impact of imprecise calculations may be assessed by direct
          simulation for purposes of evaluating future low cost special purpose
          instruments.

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       •  additional data, e.g., environmental conditions, time,  date, signal
          variability, laser parameters, etc., may be measured and recorded
          without modification of or addition to the  existing system hardware.
       •  the performance of one or more data processing and display systems
          can be directly analyzed, e.g., data from several ozone monitors
          could be crosscorretated and recorded.
       The data collection and reduction system is sketched in Figure 3.  A Digital
Equipment Corporation PDF 11/05 is used for the central processor.  The data
collection and reduction equipment in Figure 3 consists of three major subsystems:
Interface Subsystem
       The Interface Subsystem is composed of an 8 input analog  signal multiplexer,
which is followed by a  sample-and-hold amplifier and an analog-to-dlgital converter
at 10-bit precision.  (The analysis path detector preamplifier output is connected to
one multiplexer input,  the reference path to a second multiplexer input, the  re-
maining 6 are available for sensing other voltage levels of interest). Additional
subsystem elements include an AGC attenuator,  a wheel position counter and
demultiplexer/storage capability for analog data displays like the meters shown
in Figure 3.
Central Processor Subsystem
       The central processor and its own control panel form this subsystem.  Power
supplies  for this equipment are contained within the CPU cabinet proper.  The
central processor control panel  ordinarily is disabled during operation.

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Analysis Path
Amplifier Output

Reference Path
Amplifier Output

Chopper  Wheel
Encoder Timing ••
Signals
                       Interface
Multiplexer,
Sample and
Hold, A/D
AGC
Attenuators,
D/A Converter
Storage Registers
        	I
Teletype and Paper Tape Reader
(Teletype Not Required for Equipment
Operation;  May Be Removed After
Control Program Has Been Loaded
                       Meters
                                                  Central Processor
                                                  POP 11/05
                                                       CPU
                                                         Program Input and
                                                         Data Logging
                     Data Display
                                                Fiaure 3.  DATA COLLECTION AND REDUCTION SYSTEM

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Program Input and Data Logging Subsystem
       A Teletype Corporation ASR-33 teletype with appropriate interface circuits
constitutes this subsystem.  As indicated,  it plays two roles.  First, it permits
entry (ordinarily via paper tape) of the control program.  Second, it permits detailed
reporting of directly measured quantities,  or derviced (computed) quantities.
       The central processor is designed so that programs stored in its core memory
may be caused to remain  intact during periods of no primary power.  This option
is exercised,  so that once a control program has been entered in the CPU, it
need not  be reentered until there is a need to change it,  regardless of whether the
CPU remains  energized or not.  The control program is designed so that it will
run properly regardless of whether the teletype is connected or not.  Thus the
teletype unit is an optional data display device, not an essential component of the
system once the control program has been entered.
       Details of the mini-computer signal processor are described in the following
sections.
3.  LOGIC BLOCK DIAGRAM
       A logic block diagram of the complete system is shown in Figure 4.  The
analysis  path or analytic detector is followed by a preamplifier which generates a
10 mV -  10 V  signal level depending upon path attenuation.   In this diagram a wide-
band analytic detector is shown. However for the modified ILAMS system, a thermistor
bolometer detector with equalization will be alternatively used.

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                                             METE*

                                            OUTPUTS

                                              iUi
                                                                                                                           •ll
                                                                                                                           *. 3
                                                                                                                             *
                                                                                                                              i


                                                                                                                             J
CD
                                                               Figure 4.  LOG.'C 8LOCK CTiaG

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      A digitally-controlled amplifier, using a multiplying D/A converter (MDAC),
automatically controls this signal level to about 10 V in order to limit the dynamic
range requirements of the A/D converter.  The mini-computer generates a feedback
signal to control the gain of this circuit and also performs the  required filtering
necessary to realize a given loop response time which is usually set to about 1 second.

      A single pole low-pass filter preceeds the A/D converter in order to limit the
bandwidth and thereby establish the required sampling rate. The cutoff frequency
is chosen large enough in order to limit the interpulse interference  to an acceptable
level.  An analysis of bandwidth, sampling time,  and  interpulse interference as
well as other effects appears in Reference 1.

      For the ILAMS system,  the reference detector is followed by  a similar pre-
amplifier, equalizer, and filter.  However, no gain control is  necessary for this
channel.

      An A/D converter and multiplexer alternately samples the analytic and reference
channels at a rate  compatible with the signal bandwidth.

      A digital shaft encoder which is attached to the laser wavelength selector
wheel is used with a counter in order to provide the synchronous gating information
shown in Figure 2.  This arrangement provides an 8-bit number which determines
the wheel position  at any instant in time.   The lowest  order bit is also used to control
the A/D converter and multiplexer so that the samples are synchronized  with the
waveforms.
                                     10

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      Each data collection cycle consists of serially reading a signal and wheel
position sample into the DR11-A interface unit.  The samples for each analytic
and reference wavelength and nulls are accumulated in separate registers according
to wheel position.  This performs the synchronous demodulation of the signals.

      Digital filtering of the data is done in two steps.  In the first step, samples
are accumulated for l/4s at each analytic and reference wavelength.  A null is
also accumulated for analytic and reference.  Both accumulated nulls are
appropriately weighted and subtracted from the corresponding accumulated wave-
length samples.  The  null weight for each wavelength is determined so as to
account for the different number of samples accumulated in the wavelength and null
accumulators over one scan; i.e.
                   nbr of samples in wavelength accumulator in one scan
                   nbr of null samples in one scan

      The second step consists of low pass filtering the  l/4s sequences to obtain the
desired system response time.  This approach allows a quasi-continuous readout of
all monitoring  signals.  In addition,  the l/4s signal sequences can also be filtered
for AGC  feedback with arbitrary response time.

      The factor E shown in Figure 5 controls the system response time
       T -  (1 - In E)/4 seconds
      where  E  is a positive number less than one.
                                     11

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1 *
2 ^
u3 p
U4 »

5 *

U6 *


v2 *
^
^3 >
i. ^
v4 *
V5 ^
V6 P





DIVIDER
X Ui
xi 	
f













X]
y _
A2
X0
3
X4
X5
X4






XA
M -

1













NAA;
i













t

< f,.
IA

































2")






















































LOW
PASS
FILTER

Yp(l-E)*Xi
+ E Y|

t
1






Yl
— T~+
Y2 .

3 M
Y4
YS k
Yrt k














LOG
i log Y;





FigureS.  PROGRAM MODIFICATION

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      A "geometric" integrator is used for AGC feedback filtering.  The error signal
is derived in such a manner as to maintain each analytic level at less than or equal
to half of its respective reference level, on the average.  For this arrangement,
the response time of the AGC loop is dependent upon the reference level.  However,
an improved design which eliminates this dependency as well as simplifies the
computations is shown in Figure 5.  This version will probably be adopted in any
future generation software.

      After  the final low-pass filtering, the log ratios of the 1/4 second analytic and
reference samples are computed. A balance register is provided at this point in
order to initially calibrate the instrument for a zero output in the absence (hopefully)
of any absorbing gas.

      The normalized log  ratios are then weighted, scaled and outputed to the
teletype unit as the final concentration estimates.  A later modification also
provided meter readouts.  A threshold feature  Is also included In order to signal
exceptionally large concentration levels.

      An existing analog signal simulator (Reference 2)  is being used to generate arbitrary
absorption patterns and thereby checkout the entire signal processor in the laboratory.

4.  SOFTWARE

Operational  Modes

      The system normally operates in either one of two modes:  collection,  and data
reduction and display.
                                      13

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Collection Mode
         In this mode repeated measurements of the analysis path signal and
reference path signals are made and recorded.  Additional measurements
on the behavior of other system elements also may be made before, during or
immediately after the repeated transmission measurements.

         The output of the analysis path detector amplifier is connected to one
of the multiplexer inputs indicated in Figure 3; the output  of the reference
path amplifier is  connected to a second multiplexer input.

         The chopping wheel,  which both modulates the laser beam output and
controls the laser wavelength, is driven by a motor which is monitored by
a digital shaft encoder.   The net effect of this apparatus is to generate a binary
number which reports the position of the wheel and thus laser wavelength  and
modulation.  The wheel position is reported to 1 part in 256, i.e., to about 1.4
precision.  One can think of a 256 tooth gear or index on the chopper wheel.  The
wheel rotates about 3000 rpm, or 50 revolutions/second,  so that the wheel
advances one "tooth" every 78 microseconds.   (In  reality, the binary counter
advances 1 count  each 78 microseconds.)  At each new count, the CPU is  in-
terrupted and the present reading of the counter and one A/D converter reading
are transmitted to the computer.  The  counter reading is  interpreted to deter-
mine the nature and proper disposition of the A/D  converter reading;  that dis-
position  is  made and the processor then waits for another interrupt.   (Typical
data dispositions  are the addition of a current reading to the previously
                                    14

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 accumulated sum for that wavelength and that path,  or ignoring the reading
 because it is the transition interval between "on" and "off".)

         At preset intervals, e.g., once every N cycles of transmissivity
 data collection, the normal data collection sequence may be altered to
 measure any other parameter of the system which is connected to one of the
 multiplexer ports.  Each of these measurements may be  recorded separately
 if the total number is small (e.g., 100), or averaged.  Each measurement
 would require 50 to 100 ps to complete.  Upon completion of the measure-
 ment, data collection would continue as before, picking up again at the next
 full revolution of the chopper wheel.

         At the conclusion of a preset  number (e.g., M) of transmission
 observations, operation in the data collection mode is terminated.

         The parameters M and N are stored in the processor at some
 previous time,  either by teletype,  or by use of the numeric input controls
 of the operator control subsystem.

 Data Reduction and Display Mode

        The second mode of operation is data  reduction and display.

        At the  conclusion of a data collection sequence, signal measurements
have been accumulated on each of typically 4 wavelengths, at both the reference
and analysis paths.  The transmission measurements consist of both "peak"
                                  15

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      measurements at each wavelength and "valley" measurements made during
      the off period between open shutter intervals.  In all, for 4 wavelengths,  10
      quantities will be available,  (4 reference paths, 4 analysis paths, reference
      amplifier null and analysis amplifier null).

               The data reduction program now operates on this data, reporting,
      for example, relative transmission at each wavelength or estimated con-
      centration of each of one or more gases.

               The first two results might best be reported via the teletype; the
      latter results might be reported both via the teletype and via the simpler
      displays  included in the  operator control subsystem,  (As indicated earlier,
      the teletype system and  software are configured so that the absence of
      the instrument does not prevent successful computation and presentation of
      the results intended for  display on the operator control  subsystem.)

              It may be noted that the only hardware that would have to be changed
      to accommodate the use  of any reasonable number (say  up to 10) different
      wavelengths of laser radiation would be the  chopper wheel.  The "data dis-
      position" table stored in the processor would have to be changed, but this is
      merely a matter  of reading a paper tape.  A few additional memory locations
      would be  needed for the accumulation of transmission measurements, but the
      22  accumulators  required for 10 wavelengths are readily available.

Program Structure

      Software  of the ILAMS system is  composed  of one  real time analysis program
and two non-real time  support programs that modify tables used in the analysis
                                        16

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program.  The functions of each program are:
      •  Real-time Analysis Program - a)  collect  real time laser out-
        puts and compute a series of measurements for printing on the
        teletype, b) monitor and feedback of AGC.
      •  Parameter Entry Program - supplies and modifies, via the tele-
        type keyboard, various weighting factors, integration constants,
        time constants,  scaling factor, etc.
      •  Channel Assignment Program - builds tables of values which are
        used to assign individual  data samples to specific input channels.
      Instructions for Operating Real-time Analysis Program

              These instructions apply when the analysis program and required
      support programs are already loaded into memory.  For instructions on the
      loading of programs, see Chapters 2 and 6 of the "PDP-11 Paper Tape Soft-
      ware Programming Handbook".  Steps required to  start program are:
              1.  Turn console power key to ON.
              2.  Turn teletype console switch to LINE position.
              3.  Depress ENABLE/HALT switch.
              4.  Enter start location 12400  in the Switch register.
                                         8
              5.  Depress LOAD ADRS switch.
              6.  Lift ENABLE/HALT switch.
              7.  Depress START switch.

              The above starting point will cause the  AGC value to be initialized
      to the minimum gain setting.  An alternate restart location of 12414g  will
      leave the AGC at its last computed value.
                                         17

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       The program may be stopped at any time by depressing the
 ENABLE/HALT switch.


 Program Output

       a) A set of eight measures are printed on the teletype for
         approximately every 16th set of data gathered.

       b) A new AGC value is computed and transmitted for every
         set of data gathered.

       c) Eight meter outputs are transmitted for every set of data gathered.

 Program Input - Keyboard

       The depression of selected keys on the teletype allows the user to
 alter the flow of the analysis program.

       Key        Reaction

      "B"        Program performs the balancing function and then
                 continues with normal processing.

      "U"        Program performs an unbalancing function and  then
                 continues with normal processing.

      "T"        Control  is transferred to the channel assignment
                 program which prints a "K" when ready to receive
                 data.  Restart at !2414  is necessary to  return  to
                 analysis program.

      "P"        Control  is transferred to the parameter entry program
                 which prints a "$" when ready to receive data.  Restart
                 at 124148 is necessary to return to analysis program.

Parameter Entry Program

      Various parameters used by the program are stored  in an 12 x 8 array
which may be altered by the parameter entry program.  The array structure and
contents are as follows:
                                         18

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Array Location    Parameter
1.1
2,1
3,1
4,1
 1,4
•2,4
•3,4
• 4,4
5,1 — 5,4
6,1 -—6,4
7,1 — 7,4
8,1 -—8,4
9,1
9,2
10,1
10,2
11,1—11,8

12,1 —12,8
Measure 1 weight
Measure 2 weights
Measure 3 weights
Measure 4 weights
Measure 5 weights
Measure 6 weights
Measure 7 weights
Measure 8 weights
E
1-E
F
AGC value
Scaling constants
(Multiply results by
2n where n = 1—15)
Meter offsets
Range
-1.0—1.0
-1.0—1.0
-1.0—1.0
-1.0 —1.0
-1.0 -*1.0
-1.0—1.0
-1.0 —1.0
-1.0—1.0
0 — < 1
0-^1
0 ^( 1
0—7777
8
1-15
Maximum
Input Units
± 250
± 250
± 250
± 250
± 250
± 250
± 250
fc 250
32767
32767
32767
4095
15
Input
Units
± 1/250
± 1/250
± 1/250
± 1/250
-t 1/250
± 1/250
:t 1/250
± 1/250
1/32768
1/32768
1/32768
1/4095
1
                                       63   64
1/64
       The parameter entry program may be started by depressing the "P" key
while the analysis program is running - or - starting at 14000 .  The program
                                                         o
will print a "$" when ready to accept data.
                  Input format:
                  x, xbnnnnn(CR)
                                (CR) is a return
       where
       Examples:
                  b - blank
                  x, x - signifies the array coordinates
                  nnnnn - any value up to 5 digits - may be preceded by a
                         minus sign to signify a negative value
                  1, lb!25(CR) - Value of 1/2 entered for set 1 weight 1
                  3, 7b-10(CR) - Value of -1/2 5 entered for set 3 weight 3
                  5,lb32767(CR) - Value of l-2~15 entered for E
                                           19

-------
Channel Assignment Program


        This program is used to assign data samples (as designated by

wheel position count) to specific input channels.  Channels are numbered:
        01
        02
        03
        04
-Analytic
09
10
11
12
>  Reference
        07  Analytic nulls         15    Reference nulls
The channel assignment program may be started by depressing the "T" key

while the analysis program is running - or - starting at 7000  .  The program

will print a "K" when ready to accept data.
         Input format:
         xxbnn,nnn	n(CR)
                      Examples

                      03bl7,19,123,7(CR)
                      04bl24(CR)
                      etc.
         where
             b - blank

             xx - is a two digit channel number

             n or nn or nnn - is the wheel position count

         Notes: 1.  00 - as a channel entry will clear the channel
                   assignment table.

                2.  Wheel position counts are separated by commas
                   with the last one followed by a return.
                                                               8
    3.  Any positive octal value placed in location 7446
        will be added to the wheel positions as they
        are entered.  Truncation at 256 is performed by
        the program (256 = 0, 257= 1, etc.).
                                   20

-------
5.  INTERFACE UNIT

      The Interface Unit conditions the analog signals from the reference and
analytic detectors and the signal from the shaft position encoder, converts them
to digital form, and makes them available in the proper sequence as inputs to the
computer.  The capability for automatic gain control (AGC)  is provided for the
analytic signal channel.  In addition the Interface Unit  Includes storage elements
and digital-to-analog  converters for output indicators such as meters or chart
recorders.  Up to eight values can be indicated or recorded simultaneously,  and
the eight quantities to be displayed can be selected by the computer program.

      The Interface Unit is assembled in an aluminum enclosure measuring
approximately 28 X 18.7 X 18.7 cm.  It consists  of a socket panel which holds
most of the analog and digital circuitry,  a Data Acquisition System, and power
supplies.  The power supplies allow the unit to operate directly from the 117 V
AC line. They also furnish power for the shaft position encoder and the preamplifier
for the analytic detector.

      The Data Acquisition System is a modular unit made  by  Datel Systems,  Inc.
(Model DAS-16-L10B).   It has a 10-bit analog-to-digital  converter, a sample-and-
hold circuit,  and  an analog multiplexer,  connected to allow either random or
sequential digitizing of up to  8 analog voltages.  The Interface Unit uses only two
of the eight inputs - one  for the analytic signal and one for the reference signal.
These two inputs  are  sampled and digitized  alternately.
                                          21

-------
      The functional elements of the Interface Unit are shown at the left side of
the signal processor block diagram, Figure 4. The detectors and their pre-
amplifiers,  and the shaft position encoder, are not physically a part of the Inter-
face Unit.

      The AGC circuit makes use of a multiplying D/A converter (MDAC)  in the
feedback path of an operational amplifier.  The closed-loop gain of this amplifier
is inversely proportional to the value of a 12-bit binary number that  is applied to
the MDAC, except that the gain cannot exceed 39. Since the AGC control  comes
from the mini-computer,  the algorithm used and  its response time are the choice
of the programmer.

      The shaft position encoder is of the incremental type with a zero index.  It
produces 1024 pulses per revolution on one output, and one pulse per revolution
on the other.  The 1024 pulse output clocks a 10-bit binary counter,  which under-
goes a complete cycle once per revolution.  The index resets the counter  to insure
that it always starts from exactly the  same shaft  position.  In this way,  the 10-bit
number furnished by the counter indicates the position of the  chopper wheel with an
accuracy of about 0.1%.

      Figure 6  shows the  sequence  of events and their  relative  timing during a con-
version cycle.  A time equivalent to 1/256 of a wheel  revolution, or  78 p.sec. at
3000 rpm,  is allowed for  this cycle.  The first four lines in Figure 6 show the logic
states of the four least significant bits of the wheel position counter.  The 128-count
line is used to switch the  analog multiplexer  in the Data Acquisition System, so that
                                         22

-------
 1024
r~L
  512
  256
     l_
  128
     1_
 CONV CMD
to
co
 CONV BSY
 REQ B
 DATA TRANS
 POSAAL
                          -78//SEC
                                   Figure 6. SEQUENCE OF EVENTS

-------
 the analytic channel and the reference channel are sampled and digitized  in
 alternate cycles.  After this multiplexer switches, a period of about 9.8 ^scc.
 is allowed for settling before an A/D conversion is initiated by the negative
 transition of the "Convert Command11 line.  The A/D converter's "busy"  line
 stays high while the conversion is taking place, and then goes low.  At that point
 the "Request B" line goes high to indicate to the computer that data is ready for
 input.  This data passes through a digital multiplexer which selects between the
 wheel position counter and the  A/D converter. Initially,  this multiplexer,
 controlled by the "Position/Value" line, is switched toward the counter.

       When the computer has read in the wheel  position, it sends a "Data
 Transmitted" pulse to the Interface Unit.  This pulse terminates the "Request
 B" and changes the digital multiplexer to the A/D converter.  The  computer then
 reads the digitized input value  and returns another "Data Transmitted" pulse.
 (The Interface Unit does not use this second pulse.)

      Since the A/D conversion requires only about IS^tsec. , the time available
for the computer to read both the shaft position and signal values is about 65 ^scc.
Only the  eight most significant bits of the  wheel position counter are furnished to
the computer, since that is sufficient to give each conversion cycle a unique wheel
position value.
                                       24

-------
C.  SPECTRAL STUDIES

1.  INTRODUCTION

       ILAMS measures directly the transmission (T1§ T2>  Tg, T4>
of the sample region between the transmitter and the retroreflector at four wave-
lengths.  Assuming that the line width of the resonance absorption is broad
compared to the transmitted laser line width, and assuming also that there is no
saturation in the absorbing media,  then, for a uniform concentration of the absorber
over the path, the transmission at each discrete wavelength is of the form,  T^  =
exp (-A  C L): where A   is the absorption coefficient of absorber A at wavelength
  v v   m A            m
m, C  is the concentration of absorber A over the total optical path, and L is the
     A
total optical path through the  sample region.  If the concentration is non-uniform
over the path, as is the more usual case, then CAL can be replaced by the integrated
concentration over the path or, more simply, let CA represent the average concentra-
tion over the path.

      Typically, C has units of grams/liter or atmospheres of partial  pressure, and
L is in centimeters.  A   is in units to make A  C L dimensionless.
                      m                     m  A

      If a second absorber B with absorption coefficients B   is introduced into  the
region, the net transmission will be the product of the transmission due to each
absorber.
                                                                       (1)
                          -  A CAL+ B  C^L
                              m  A     m  B
                   T  = e
                    m

      If the natural log of the transmission at each wavelength is taken elec-
tronically, then

                   S  =  InT  --(A  CAL+B  C_L)                     (2)
                    m       m     m  A      m  B

and the resulting signals have two convenient properties:
                                      25

-------
      1)  System response to any absorber is a linear function of the
         quantity (concentration x path) present
      2)  System response to several absorbers is the sum of the
         responses to the individual absorbers.
Therefore, it the system can be designed to give a zero response to spectrally
interfering absorbers, the system will respond only to the pollutant to be measured,
and the response will be proportional to the quantity present.

      Speaking more generally,  the above properties define a linear 4-dimensional
vector space.  Each gas is represented by a vector in this space whose length is
proportional  to the concentration.  This formalization permits  the application of
known mathematical and statistical techniques.

      Using decision theory and multivariate statistical analysis, it can be shown
that the optimum signal processing involves the use of single or multiple linear
weights.  Application of a single linear weight, W, means taking n  linear sum of the
signals S  S  ... S  to give a new signal, S = W^ + W^ +  ...  W^.  The
quantity of absorbers present can be accurately determined by examining the magnitude
of such linear sums.

      Techniques may also be applied for choosing linear weights to accurately
measure the quantity of a given pollutant in the presence of known interfering
spectral absorbers, random spectral absorbers,  scintillation, and other "noises".
A definitive study on spectral absorption pattern detection and  estimation techniques
using linear  weights appears in Reference 3.  A  summary of the applicable results
are given in Appendix A and B.
                                         26

-------
      For the CO laser, there Is a large number of lines from which the
                 ^
 4 wavelengths can be selected.  On the basis of both analytical and experimental
 work, several basic conclusions about wavelength selection can be drawn.  These
 are:
       1)   The relative success of a group of wavelengths depends directly
           on the measurement problem.  The pollutants to be measured,
           pollutants and absorbers to be ignored, expected quantities of
           absorbers and the system noise levels, all affect the choice of
           wavelengths.
       2)   For a given problem, there will be an optimum set of wavelengths.
           Increasing  the number of pollutants  to be estimated or ignored will
           tend to increase the optimum number of wavelengths to be used;
           i.e., the more complex the environment, the more wavelengths
           are necessary.
       3)   The finer the spectral structure of an absorber,  the fewer number
           of wavelengths  areneeded to best measure the quantities of it
           present.  The laser system is not limited to detecting pollutants
           with fine structure such as ammonia and ethylene. In fact, it does
           remarkably well in detecting or rejecting absorbers with rather
           smooth spectral characteristics.
       4)   On the basis of past experience, four wavelengths have done an
           excellent job in handling spectral recognition problems in environ-
           ments representative of the real world.

       The primary target gas considered in this program was ozone.  Secondary
targets, which are also, to some extent,  interferences for the primary target as well
as between themselves, were ethylene  (C H ) and ammonia (NG ).  The general
                                      &  4                  O
topics of Interferences and Optimum Linear Weights are discussed, respectively, in
Appendices A  and B. A systematical approach  to the wavelength selection problem
using mathematical and computer techniques is presented in Appendix C.
                                        27

-------
2.  SPECTRAL DATA





Introduction and Summary



       In this section, absorption coefficient spectral data from a variety of


sources is presented.  This data was subsequently used for wavelength selection


and linear weight computation as described in the following sections of the report.



       Much difficulty was experienced in  reconciling laser measurements with


high resolution spectrometer measurements.  In general,  the adage of using only


laser absorption measurements for designing a laser system has been reaffirmed.



       The molecular species considered for this contract were ozone (O ),  carbon
                                                                      O

dioxide (CO ), water vapor (HO), ethylene (C H ),  and ammonia (NH ).  Reliable
           L                L>               £> 4                    o

data was obtained for all of these gases except for water vapor.  This absorber is


especially difficult to characterize because of the predominant self-broadening


that occurs.



       Tables I and  II give a tabulation of the summarized absorption coefficient data. *


A composite  spectral plot that illustrates the data  in the 9. 4 micron CO band is shown


in Figure 7.  Two considerations must be taken into account when attempting to


interpret  this plot.   First, only the deviation from a horizontal line is significant since


neutral attenuation is rejected.  The second consideration is that only deviations from


the mean concentration are significant because the instrument is  initially balanced.  For


example,  if the CO   concentration only varies 32 ppm from the nominal 320 ppm
                  £

shown in the plot, then the actual interference level would be reduced by an order of


magnitude from the nominal curve shown.
*Blank spaces between data are linearly interpolated; blank

spaces outside of the data range are set to zero.
                                        28

-------

J
Value
P40
P38
P36
P34
P32
P30
P28
P26
P24
P22
P20
P18
P16
P14
PI2
PIO
P8
P6
P4
R4
R6
R8
RIO
R12
R14
R16
R18
R20
R22
R24
R26
R28
R30
R32
R34
R36
R38
R40

Wavelength
Microns
9.733474
9.713998
9.684831
9.675971
9.657416
9.639166
9.621219
9.603573
9.586227
9.569179
9.552428
9.535972
9.519808
9.503937
9.488354
9.473060
9.458052
9.443325
9.428886
9.367339
9.354414
9.341758
9.329370
9.317246
9.305386
9.293786
9.282444
9.271358
9.260526
9.249946
9.239615
9.229530
9.219690
9.210092
9.200733
9.191612
9.182725
9.174070
Wave
Number
CM"'
1027.382
1029.442
1031.478
1033.488
1035.474
1037.434
1039.369
1041.279
1043.163
1045.022
1046.854
1048.661
1050.441
1052.196
1053.924
1055.625
1057.300
1058.949
1060.571
1067.539
1069.014
1070.4efficient

                                                                   H20*



                                                                1.430E-04
   The H2O absorption coefficient is proportional to H2O
   partial pressure (see text).  The values listed in the table
   are for 100% relative humidity at 23 degrees C (73 degrees F)
   which is equivalent to 19.8 torr.
** See text.
                                                                1.390E-04
                                                                1.360E-04
ATM'1 CM'1

      C2H4
                                                                                 400E 00
                                                                                 900E-01
                                                                                 400E 00
                                                                                 600E-01
                                                                                 500E-01
                                                                                 600E-01
                                                                               9.000E-01
                                                                               4.400E-OI
                                                                               8.700E-01
                                                                               2.200E-01
                                                                               1.500E-01
                                                                               1.800E-01
                                                                               4.600E-01
                                                                               2.400E-01
                     Table I   Absorption Coefficients for 00°1 - 02°0 (9.4 micron) CO2 Band

                                                      29
NH3
                   3.400E-01
                   9.000E-02
                   6.000E-02
                   l.OOOE-01
                   4.700E-01
                     800E-01
                     580E  00
                     600E-01
                     200E-01
                   3.400E-01
                   I.030E 00
                   3.900E-01
3.600E-01
9.000E-02
8.000E-02
3.100E-01
6.700E-01
1.900E-01
1.100E-01
2.000E-01
1.200E-01
5.000E-02
2.600E-01
3.700E-01
7.200E-01
**1.050E 01
1.400E-01
3.000E-02
.7.800E-02
7.000E-02
1.200E-01
4.200E-01

-------

J
Value
P40
P38
P36
P34
P32
P30
P28
P26
P24
P22
P20
P18
P16
P14
P12
PIO
P8
P6
P4
R4
R6
R8
RIO
R12
RI4
R16
R18
R20
R22
R24
R26
R28
R30
R32
R34
R36
R38
R40

Wavelength
Microns
10.8)1105
10.787380
10.764052
10.741113
10.718560
10.686386
10.674586
10.653156
10.632090
10.611385
10.591035
10.571037
10.551387
10.532080
10.513114
10.494484
10.476187
10.458220
10.440579
10.365168
10.349277
10.333696
10.318424
10.303458
10.288797
10.274438
10.260381
10.246625
10.233167
10.220006
10.207142
10.194574
10.182301
10.170323
10.158637
10.147246
10.136146
10.125340
Wove
Number
CM-1
924.975
927.009
929.018
931.002
932.961
934.895
936.804
938.689
940.549
942.384
944.195
945.981
947.743
949.480
951.193
952.882
954.546
956.186
957.801
964.770
966.251
967.708
969.140
970.548
971.931
973.289
974.623
975.931
977.215
978.473
979.706
980.914
982.096
983.253
984.384
985.489
986.568
987.621
                                                            Absorption Coefficient -  ATM"'  CM"1
                                                  co2


                                               5.3981-04
                                               7.037E-04
                                               8.651E-04
                                               1.099E-03
                                               1.303E-03
                                               1.539E-03
                                               1.834E-03
                                               2.052E-03
                                                  278E-03
                                                  500E-03
                                                  731E-Q3
                                                  756E-03
                                                  786E-03
                                                  736E-03
                                                  595E-03
                                                  335E-03
                                               1.984E-03
                                               1.580E-03
                                               1.091E-03
                                               2.725E-03
                                               1.870E-03
                                               2.301E-03
                                                  608E-03
                                                  867E-03
                                                 978E-03
                                                 050E-03
2.
2.
2.
2.
2.
2.
2.
2.
                                               3.019E-03
                                               2.870E-03
                                               2.708E-03
                                               2.449E-03
                                               2.211E-03
                                               1.955E-03
                                               1.667E-03
                                               1.412E-03
                                               1.157E-03
                                               9.449E-04
                                               7.581E-04
                                               5.879E-04
* The H2O absorption coefficient is proportional to
  partial pressure (see text).  The values listed in the table
  are for 100% relative humidity at 23 degrees C (73 degrees F)
  which is equivalent to 19.8 torr.
                   H20*
   C2H4
                 1.800E-04
                 8.000E 00
2.400E 00
1.200E 00
1.800E-00
3.600E 00
5.000E 00
3.200E 01
0.
                  Table  II  Absorption Coefficients for 00°1 - 10°0 (10.4 micron) CO, Band


                                                    30

-------
 0.15
 0.10
u
«
n
h-
C
                                           	 O3 - McClenny, EPA
                                                CO2 -SRI
                                           	C2H4 - McClenny, EPA
                                           	 H2O - Burch, Long
                                                NH3 - McClenny, EPA
                 320 ppm
                  C02
                               H2O 50% RH @ 23°C
36    32   28    24
20
                                  16    12 RIO   P1012    16
                                   00° 1 -02°0 (9.4p Band)
                Figure 7.  Composite Spectral Absorption in 9.4/j
                                       31
20    24
                                                                CO2 Band
                                                                       28

-------
 A more refined plot showing only the deviation about the mean for water vapor and
 carbon dioxide in the P branch is shown in Figure 8.  As can be seen, water vapor
 is a serious interferent and its characterization is critical in detecting trace con-
 centrations of ozone.
      Observed stability of the monitoring system that uses linear weights derived
 from this spectral  data has been poor under some conditions which are suspected
 to be attributable to relative humidity variations.  Other sources of data noted in the
 following discussion of water vapor absorption coefficients also suggest significant
 departure from the assumed linear continuum as well as a bizarre interrelationship
 with aerosols.  In Section C.5 a  factor analysis of the system noise also points the
 finger of suspicion in this direction.
       In particular, it is now believed that the R14 line that was used Is sitting
almost on top of a water vapor absorption line.  At the writing of this report the
number 1  system wavelength has been moved from the R14 line to the R16 line and
operation under this modification is being evaluated.
       For  all of the above reasons,  a water vapor laser measurements program is
recommended for future air pollution monitoring systems that utilize laser absorption
measurements in this spectral region.  A research facility such as the 980 m cell
at Ohio State University Electroscience Lab now operated by Dr. R. K. Long and
associates would be ideal  for this purpose.  This particular facility is the one which
was used in the past for obtaining the only reliable water vapor absorption laser
measurements known to exist (Reference 4).
       Some spectral instability  can be attributable to variation in the CO   absorption
                                                                      £t
coefficient with temperature.  For  the lines and linear weights that were used with the
present system, a 40 degree F change in temperature causes an apparent change  in
ozone level  of about 2. 3 ppb.  This level of unstablllty is not a limiting factor for the
present system.
                                        32

-------
    0.015
    0.010
u
a
n
H
T
        0
                                                        1	j—	1
                P10    P12    P14   P16    P18    P20   P22    P24   P26    P28   P30    P32
                                             9.4fj Band
           Figure 8.  Composite Differential Spectral Absorption in P-Branch of 9.4yu CO2 Band
                                               33

-------
However,  if desired, this variation could be eliminated by changing linear weights
as a function of ambient temperature or by considering the first order temperature
variation as an additional interferent to be discriminated against.

       A large absorption coefficient for ammonia was discovered in the 9.4 micron
CO  band by direct laser absorption measurements performed by  W.A. McClenny.
   L*
This behavior  has been previously unnoticed with spectrometer measurements which
have obscured the true peaks because of resolution limits.  In  fact, this absorption
coefficient is larger than the one in the 10.5 micron band which was heretofore thought
to be the largest available.

Ozone (O )
        O
       Ozone absorption coefficient data was obtained from direct laser measurements
(References 5 and 6) high resolution spectrometer (Reference 7) and theoretical
computations (Reference 8) using line strength data (Reference 9).  Figure 9 illustrates
a comparison of the data which demonstrates very good consistency.  In all cases,
the measurements were made at standard temperature and pressure. *  Because of the
inherent accuracy of the laser measurements and good repeatability, McClenny's
measurements were used as a basis for the ozone data and were transcribed onto our
computer spectral library tape as listed in Tables I and  H.
*It was subsequently determined that all of McClenny's measurements (References 5
 and 12) were converted to 0 degrees C reference temperature by using the T 1/2
proportionality law for the line half-width.  It is noted that this scaling law is only
appropriate at a line center.  Moreover, the temperature dependence of the line intensity
must also be taken into account (Ref. 9 (eq. 3) and (Ref. n (ecu 77)).  In anv case, the
difference is probably small compared to the spread of the other data.  In addition,  all
of the wavelength selection and linear weight algorithms are more dependent on the
relative ratios of absorption coefficients between wavelengths rather than the absolute
magnitude.
                                          34

-------
 0)
E
15
                                                     00° 1 -02°0 Band
                   Figure 9.   Ozone Absorption Coefficient Data Comparison in 9.4}} CC>2 Band
                                                     35

-------
Carbon Dioxide (CO )
                  
-------
                  5x10
co
                  4x10
                  3x10
                o
                1
                "o
                  2x10
                   1x10
                              R14    R16    R18   R20   P12    PU    P16   P18   P20    P22   P24    P26    P28   P30
                                                                 9.4jj Band
                                             Figure 10.  CC>2 Absorption Coefficient Data  Comparison

-------
CO
oo

Temperature
Degrees F
70
70
70
50
70
90
Pressure
Bars
1.003 !(-!%)
1.0132(nom)
1.0233(+1%)
1.0132
1.0132
1.0132
Relative Absorption Coefficient
Wavelength - microns
9.305386
(RH)
1.106621
1.106 650
1.106678
1.106080
1.106650
1 .107 239
9.503937
(PI 4)
1 .000 000
1 .000 000
1.000000
1 .000 000
1 .000 000
1 .000 000
9.586227
(P24)
0.841 477
0.841 471
0.841 464
0.816962
0.841 471
0.864891
10.532080
(PI 4)
0.747 132
0.747 138
0.747 143
0.731 860
0.747 138
0.761 726
10.674586
(P28)
0.500629
0.500720
0.500809
0.468 236
0.500720
0.532764
10.718560
(P32)
0.355 691
0.355 710
0.355 729
0.327 494
0.355 710
0.384 019
                               Table III.  Relative  CO^ Absorption Coefficient Variation with Pressure and Temperature

-------
 Water Vapor (HO)
                Lt	
        In the 8-14 micron water vapor window, the absorption is a  relatively smooth
 function of wavelength.  This continuum is believed to be mostly due to the extreme
 wings of strong collison-broadened absorption lines centered more  than 10-20 cm"1
 away (Reference 13).  However, the effects of pressure induced  absorption resulting
 from forbidden transitions of unperturbed molecules and the possible existence of the
 water dimmer (^0:^0) have also been suggested  (References 9 and 14).
        The absorption coefficient due to the continuum  can be written as (References
 9 and 13).

                   R = CsP + CbPb                                  (3)

 where Cg is the self-broadening coefficient, Cb is the foreign gas broadening co-
 efficient, p is the partial pressure of the species, and pb is the foreign gas partial
 pressure.  As  can be seen from (3), for small p, the absorption coefficient is nearly
 constant which is usually the case for most atmospheric gases.  On  the other hand,
 for large p, the first term dominates and the absorption coefficient is proportional to
 p.  In this case, the log transmission is proportional to -p2.  It has  been experimentally
 demonstrated that the latter situation occurs for atmospheric water  vapor absorption
 under normal relative  humidity conditions (Reference 4).
       In the SRI computer study, (Reference  8) the water vapor absorption due to the
 superposition of many  lines was computed. However, the effects of  self-broadening,
which is predominant for water vapor, were neglected and so these results were not useful.
                                      39

-------
        Figure 11  shows the spectral dependence of C  for water vapor continuum
 absorption for three temperatures that has been experimentally determined by
 Burcli (Reference 1-1).  n'he ratio of the coefficients at the f).rir,:> micron  and lO.ri!'!
 micron C()i?  P20 lines is seen to be about O.S which is in good agreement \\iih
 McCoy,  (Reference 4).  After a suitable  conversion of units (2. C9 x 10 '   mnl/cm"
 ] atm - 7(10 tori1),  the absolute value of the 10.591  micron coefficient indicated in
                            -I      -2    -1
 Figure 11 is about ll.fi .x ]0   torr    Ian   at 23 degrees C which is at.  variance
                          -4     -2    -1
 with the  value of S. :;<) x  10   torr  km   reported by McCoy.  In  a  recent  report
 by Trusty, (Reference 11)  spcctrophone measurements of water vapor absorption
 nt this .same line were noted to be about SO1/? higher than McCoy's measurements,
 thus giving more credibility to Burch's measurements.
       The C  value for nitrogen  has been measured to be C   0. 00.") C   at mom
             n                                            b         s
 temp(jrauire  by McCoy (Reference 4) and Burch (Reference  9) considers  this to be
 a reliable measurement.
       The data in Figure 11  was used  as a basis for the water vapor absorption
 coefficients.  The values listed in Tables I and  n were computed from (:j) and
 Figure 11 for a  relative humidity  of 100^ and at a temperature  of 2.'J  degrees C (?:}
 degrees F), i.e. ,  for a 19.8 torr partial pressure of water  vapor.   For other partial
 pressures, the absolute value of the coefficients will be scaled  accordingly, however,
 the relative absorption coefficient pattern will be invariant.
       The wavelength selection and linear weight computations described in Sections
 C.3 and C.4 were based upon the  continuum values  derived from Figure  11 (originally
 obtained from Reference 9)duo to the unavailability of  any other data at that time.
Since  then, additional data concerning the line structure has  been uncovered.
                                      40

-------
    10
      -21
E
"o
E   in'22
o   ID
o
    10
      -23
                     1200
                                                    Ref.  11
                                                                                   296 K
                                                                                                  K
1000
Wavenumber (cm"')
800
600
                                                  10

                                                 Wavelength (microns)
                                         14
           Figure 1 1 .  Comparison of the continuum absorption coefficient at three temperatures.  (From Ref.  14)

-------
       Table IV lists some of the more significant water vapor line data that were
used in the SRI study (Reference 8).  This data was obtained from a magnetic  tape
described in Reference 9.  Figures 12 and 13 show measured water vapor absorption
spectra, from Burch (Reference 13) and Hanst (Reference 7) respectively, winch
are in remarkable agreement with Table IV.  It is especially noted that the R14
(1074. G5 cm"1) CO laser line that was used in the present monitoring system is
sitting almost directly on top of the 1074.430 cm"1 water vapor line.  This could
explain some of the unstability that was noted.
       In Reference 11,  CO  laser measurements with  a spectrophone have demon-
strated a 2:1 variation in the water vapor absorption coefficient from  PS (954.54 cm  )
to P36 (929.02 cm"1). These measurements are plotted in Figure 11 and show a
significant deviation from Burch's continuum.
        Another source of anomoly has been suggested by Carlon (Reference 15) which
attributes additional broadening to  inelastic collisions involving water aerosols.
This effect has been experimentally verified and  has been used to reconcile apparent
 inequalities of absorptance and emittance in atmospheric field measurements.
        In view of all  of the uncertainties mentioned above, a water vapor laser
 measurements program would be highly  desirable for future work in  this area in
 order to pin down the true behavior of water vapor.
 Ethylene (C)
        The absorption coefficients for ethylene listed in Tables I and II were obtained
 by direct laser absorption measurements (Reference 12) and represent the most
 reliable  information to date.  The maximum absorption coefficient of 32 at the PI4
 (10.532 micron) line agrees favorably with the value of 36 measured by Hanst (Reference.7).
                                      42

-------
Wavenumber
cm
922.142
924.988
948.260
976.012
1066.200
1074.430
1091 .240
Linestrength

1 .690E-23
9.730E-24
1 .980E-23
7.700E-24
3.730E-23
1 .350E-23
2.040E-23
Halfwidth
cm'1
0.048
0.050
0.038
0.040
0.047
0.050
0..056
Table IV. Partial Tabulation of H20 Vapor Line Data (From Ref. 8)
                             43

-------
100
                                                       1000
                                                    Wavenumber (cm   )
                                                                    P14
                                                        Wavelength  (microns)
             Figure 12.   Representative spectrum of H?O between 800 and 1250 cm  .   The sample is pure
                                                                            0*7             O
                         at 14.2 torr;  path length is 1185 meters; u = 5.48 x I0'z molecules/err/;  temperature is 296K.
                         The  spectrum contains a few lines due to a trace  of ammonia in the sample;  some of the stronger
                         lines are indicated.  The ammonia lines  can be accounted for by comparing the spectrum with
                         one  of pure ammonia.  (From Reference  13).

-------
  1.1
    c
    o
    VI
Oi
          900
                                      P14
        1000
Wavenumber - CM"
P24   P14
                                                                                                           P14
                               11GX
                        Figure 13.  Spectrum of 383 meters of room air at 750 torr on a rainy day (March. 31,  1972)
                                   in Research Triangle Park,  N. C.  Recorded on the digital FTS system at 0.5 cm~'
                                   resolution using a Hg-Cd-Tel detector.. .(From Hanst, Ref. 7).

-------
Ammonia (NH )
       	o
       The absorption coefficients listed in Tables I and II were also obtained by
direct laser absorption measurements (Reference 12).  The P32 (10.7186 micron)
absorption coefficient of 8.0 is lower than the value of 32 previously measured by
Hanst (Reference 15).   However, at that time, the wavelength of the P32 line was
not accurately known and the absorption coefficient was measured at 10. 717 microns.
In addition, the resolution  of the spectrometer used by Hanst was not fine enough to
adequately measure the fine line structure of ammonia.
        The surprising  feature of the data is the large absorption coefficient (2.58)
 in the 9.4 micron band at the P20 (9.5524 micron) line.  A narrow  peak has been
 previously noted with high resolution spectrometers at that wavelength, however,
 the magnitude of the fine structure was not evident.
        It was recently  determined that the ammonia coefficients shown in the R-branch
 of Table I are displaced one J value too high, e. g.,  the R12 value listed is really the
 RIO value.  In addition, remeasurement of the true RIG coefficient has given a value of
 14. 0 rather than the value of 10.5 indicated by the table.   However, for consistency,
 the values listed in Table  I are shown as they were used in the subsequent wavelength
 selection and linear weight computations.
 3.  WAVELENGTH SELECTION
        In Appendix C, the philosophy and methodology of wavelength selection  is
 delineated as a two step process.  First a preliminary wavelength selection is used
 to reduce the number of potential lines (74) to a manageable number (say 10) by using
 a computer program called LWSP.   This program eliminates wavelengths of low
 information by an iteration process of adjusting the power allocation.  The second step
                                        4fi

-------
 in the selection process involves a combinatorial evaluation of the reduced set by
 which all combinations are ranked in accordance with their performance in measuring
 ozone. An existing program (MFIL) was modified to perform this operation and is
 called CMFIL.
        A 25 iteration LWSP run resulted in the line selection illustrated in Figure 14.
 The solid lines  in this figure represent the linear weights applied to each wavelength
 and their length is indicative of the relative importance of each line.   The X's
 designate normalized ozone absorption coefficients and the  +'s designate the average
 interferent noise level.
        The top  9 wavelengths from the LWSP output were combined with the PI4
 (10. 5321 micron) ethylene line to form the basis set for CMFIL.  Combinations of
 this set were then evaluated and ranked using CMFIL and the output listing is shown
 in Figure 15. As expected, the P12 and P14 (5 and 6) lines, which correspond to the
 peak ozone  absorption, appear in all of the highest rankings.  The RIG,  R14, and P24
 (3, 4,  8) lines also predominately appear in all of the highest rankings and are therefore
 indicated as good reference lines.
        The combination 4, G,  8, 10 (R14,  P14, P24, P14) was selected  as the com-
 bination that gave the highest signal-to-noise-ratio (SNR) while retaining the ethylene
 line.  In retrospect,  this may have been a bad initial choice since the  R14 line has been
 shown in Section C 2 (water vapor) to fall right on top of a water vapor absorption line.
 Using the RIG line instead of the R14 line would result in  the 3, G, 8,  10 combination
 which,  as can be seen from Figure 15, is only slightly inferior to the  4, 6, 8, 10
 combination.

        The  effect of the number of lines used to detect ozone has also been determined
 and is  illustrated in Figure 16.  As can be seen, a 3 wavelength system  (which we
essentially have at the present due to the retention of the  10. 5321  micron ethylene
line) provides near optimum performance with a minimum of complexity.  A two-
wavelength ozone system results in about 1/2  the sensitivity.
                                         47

-------
              o
              CN
                        TARGET  1
                                                             Time  10.41

                                                             Date  091173
              o
              CO
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                                                                                    o)
oo
           o_

           o
              8
           o  9
           OJ
              o
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              GO
, ^V^S. sr\ ^p s\ s{




 -h  -hT ^ -h
   •f  4-

J-  '     +     +
                                                                                                  t  -1-
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                                                                                                                             _c



                                                                                                                             O)
9.12
                             9.20
9.28
              9.36
     9.44

Wavelength
     9.52
9.60
9.68
9.76
                                          Figure 14.  Resultant Line Selection From a 25 Iteration LWSP Run

-------
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                                Flfur. 15.  CMFIL OUTPUT LISTING

-------

0
                            2           3
                        Number of Wavelengths
   Figure 16.   Signal-to-noise ratio as a function of the number of
               wavelengths used for the measurement of ozone.
                                50

-------
4.  LINEAR WEIGHT COMPUTATION (MFIL)
       After the four wavelengths were selected, the optimum linear weights for
measuring each species were computed using the MFIL program.  The absorption
coefficients  for these lines (R14, P14, P24,  P14) from Tables I and II are shown in
Table V.  For lack of any better data at that time, the same variances listed in
Table C-l in Appendix C were assumed and are also listed in Table V .  As more
field data is accumulated, these estimates can  be revised and more accurate linear
weights can  be computed.
       Table VI lists the linear weights and relative SNR's that were computed by
MFIL using  the input data listed in Table V.  The relative SNR's shown in Table VI
are computed for  an optical thickness of CL = 0.1.  Therefore, the noise equivalent
concentration (NEC) is given by
          NEC - (10 L SNR   f1                                        (4)

where L is the path length in cm.  For example, the present system monitors over
a 1. 34 km folded path.  The NEC for ozone is then
          NEC    = (10 x 1. 34 x 105 x 305. 9)"1  =  2. 5 ppb
               3
for the assumed noise variances.
       The cross response of the linear weights in Table VI to 0.1 CL of each
species  is shown  in Table VII.  These responses have been scaled so that the
background noise  level is unity.  Therefore,  the diagonal terms are the same as
the SNR's listed in Table VI.
                                   51

-------
en
to
Species
03
CO2
C2H4
NH3
H2O
Neutral
Absorption Coefficient - ATM"1 CM"1
R14
0.
4. 052363 E-03
9. 032525 E-02
3. 698675 E -01
1.379555E-04
1. 000000 E 00
P14
1 . 265892 E 01
3.661722E-03
1. 500705 E-01
3.416207E-01
1.407015E-04
1. 000000 E 00
P24
6.918318E-01
3.082101E-03
4.607009E-01
4.698566E-01
1.417035E-04
1. 000000 E 00
P14
0.
2. 7361 21 E-03
3. 197261 E 01
8.535154E-04
1 . 737966E-04
1. 000000 E 00
Variance (CL)
25 X 10"6
10.0
25 X 10"6
25 X 10"6
106
1.0
                          Table V.  Absorption Coefficients and CL Variance of Atmospheric Species

-------
en
Species
°3
co2
C2H4
NH3
H2O
Linear Weights
R14
-0.4745
0.9302
0.6508
-0.9171
-0.9469
P14
1.0000
0.0559
0.0520
-0.0619
-0.0519
P24
-0.5286
-1.0000
-1.0000
1.0000
1.0000
P14
0.0029
0.0145
0.2962
-0.0212
0.0000
Relative SNR
305.8907
0.0175
110.3722
1 . 7920
0.0001
                                          Table VI.  Linear Weights and SNR's for Atmospheric Species

-------

Li osor
Weight

°3
co2
C2H4
NH3
H2O
Response to 0. 1 CL


03
305.8907
0.28537E 00
-0. 40088 E 00
-0.1 4985 E 00
0. 60282 E 00

CO2
0.29339E-02
0.0175
0. 67632 E-02
-0.1 5042 E-01
-0.1 6402 E-01

C2H4
-0.10789E 01
0.17755E 01
110.3722
-0. 50682 E 01
0.63966E 01

NH3
-0.20457E 01
-0.19995E 01
-0.25674E 01
1 . 7920
0.17689E 01

H2O
0.21 225 E-04
-0.56256E-04
0.83622E-04
0.4564 IE -04
0.0001


Neutral
-0.29074E-02
0.99228E-02
-0.11857E-01
-0.34612E-02
0.21823E-01
Table VII. Cross Response of Linear Weights

-------
5.  FACTOR ANALYSIS OF DRIFT
       An attempt was made to characterize the spectral nature of the drift/noise
associated with the monitoring system.  A teletype output chart was examined for
the date of Saturday, 20 October 1973 between the hours of about 1535 PM to 1G05 PM.
During this period, the weather conditions were damp and overcast and the drift/
noise of the  system was similar to the erratic behavior experienced in the mornings
of clear days.  A total of 68 data points was selected out of this record  and the effects
of printout round off error were minimized by sampling only nfter the last digit of
most of the channels changed simultaneously  in  the positive direction.
       A sample covariance matrix was computed from the data and  an eigenvector/
eigenvalue analysis was performed using the  FACD program (Reference 17).
Eigenvectors and eigenvalues are listed in Table VIII.  The eigenvectors, or factors,
represent an optimal basis for representing the spectral data in the sense of
minimizing the rms  reconstruction error for the ensemble, and the associated eigen-
values are a measure of the importance of each factor in this representation.  The
rms reconstruction error for the ensemble depends on how many factors are used and
is numerically equal to the square root of one minus the sum of the normalized (by G8
in this case) eigenvalues.  This error, of course, diminishes to zero for four factors
since that is the dimensionality of the space.
       In order to remove the effects of neutral attenuation, the factors listed in
Table vm were projected onto the neutral hyperplane, (1, 1,  1,  1),  by subtracting 1/4
of the sum of the components from each vector.  These vectors were then normalized
to unit length and are listed in Table DC. The absorption coefficients of known atmospheri
species were also projected and normalized in  the same manner and are listed in
Table K for comparison.
                                       55

-------
Ul
No.
1
2
3
4
Eigenvalue
6.298509E 01
3. 534071 E 00
1.051795E 00
4.290484E-01
RMS
Error
27.1%
14.8%
7.9%
0
Eigenvector
R14
-4.6076
-4.7461
-4.3835
0.1213
P14
1.3684
-1.2651
-0.0751
-0.2355
P24
-0.2501
-0.1220
0.3697
-0.9153
P14
-0.1778
-0.2743
0.4917
0.2837
                                    Table VIII.  Eigenvector/Eigenvalue Analysis of Data Record

-------
Factor/
Species
Fl
F2
F3
F4
°3
co2
C2H4
NH3
H2O
Wavelength
1
(R14)
-.295
.757
-.023
-.407
-.310
.659
-.296
.212
-.368
2
(PI 4)
-.329
-U646
.117
-.559
.865
.274
-.291
.127
-.266
3
(P24)
-.240
-.012
.653
.647
-.245
-.299
-.279
.494
-.232
4
(PI 4)
.864
-.099
-.748
.320
-.310
-.633
.866
-.833
.862
                Table IX.  Comparison of Factors and Atmospheric Species
       Examination of Table IX reveals a similarity between the dominant factor and
both ethylene and water vapor.  Since the presence of ethylene on that particular clay is
unlikely, the finger of suspicion is pointed in the direction of water vapor as a
possible atmospheric interferent.  The uncertainties of the water vapor absorption
coefficients have been previously mentioned in Section C.2. However,  any con-
clusions at this point would be premature considering the limited amount of statistical
data processed.
       If repeatable factor analysis of data taken on other days was obtained, a
linear weight could be computed to reject this source of spectral interference no
matter what its underlying source is.
                                         57

-------
 D.  SPATIAL FILTER
        Experiments performed under Contract EHSD 71-8 showed that substantial
 improvement in system performance could be expected from the introduction of a
 cleanup aperature or spatial filter in the output beam of the laser.  These results led
 to incorporation of a spatial filter in the laser under this contract.

      In terms of optical theory, the function of the clean up aperture (spatial filter)  is
 to filter the higher spatial frequency variations in the transmitted laser output beam
 particularly in the far field pattern.  We can visualize the far field as the Fourier
 transform of the near field and vice versa. A small  aperture located in the far field
 provides an abrupt cutoff of the spatial frequency of the near field and at the same time
 edits  any  non-uniform clutter in the far field.  An aperture  with a two-dimensional
 gaussian amplitude distribution would be a better solution, but more difficult to
 fabricate.

       For the purposes of this experimental program,  it was decided to use a
near-circular aperture like an iris in the far  field. In the application of this device
 it must be kept in mind that the near field will be a classical Airy disk pattern
      2
 (J  /x)  which is the two-dimensional Fourier transform of the uniformly illuminated
  x
 circular cleanup aperture.  This Airy disk pattern is characterized by fringes in  the
 shape of rings that do not carry a large percentage of the laser power but are important
 in shaping the far field pattern that is formed on the retroreflector.  If a larger
 percentage of the power in the rings is collected then the far field pattern formed upon
 the retroreflector will be a disk with sharp edges  (a true image of the clean up
 aperture). Because the beam expander will not collect all the  power exiting from the
 clean up aperture then the illumination of the  disk in  the far field will be non-uniform
 especially near the edges.  The more of the rings or fringes from the clean up
 aperture that are collected by the beam expanding optics the more uniform  the disk
 pattern and the less the effect of incoherent illumination. The tradeoff between
 aperture configuration and beam expander size was a fundamental objective of
 the experiment.
                                       58

-------
       The spatial filter was introduced to the CO^ laser breadboard system at :i
point between the coupling mirror and the beam  splitter.  The layout is shown in
Figure 17. The single mode beam diameters from the laser for this particular laser
design configuration are indicated on the figure.  Note that the beam diameter, \v, at
the spatial filter is 0.67 mm.  This is the nominal beam diameter, w,  which is the
                                                                  2
distance between the 60 percent power point or the half-width to the  1/e  power point.
Figure 18 describes the amplitude and power of a Gaussian beam0 This optical con-
figuration was designed with the assistance of a computer simulation of the optical
elements and the diffraction limited Gaussian beam.

       Ten optical apertures were made from 5 mil stainless steel sheet, ranging
in size from 0.1 mm to 2. 0  mm.  The beam  intensity at the exit of the 122 mm beam
expander was observed for each of these apertures. Some improvement was
obtained as the aperture diameter was decreased down to 1 mm.  Smaller diameters
than that showed no measurable improvement in the uniformity of the beam at the
beam expander exit.   Figure 19 shows the map of the beam intensity at the beam
expander exit for the two extremes.  There is some spreading as well  as smoothing
of the beam at the aperture.
      The solid lines in the figure are a map of the beam expander output at a single wave-
length without a spatial filter.  The dashed lines are the same plot using the 1 mm aperture.
The observed improvement in the beam pattern is responsible for the majority of the
improvement in the signal-to-noise and drift of the system, over that during the previous
study  program.

       The original intent of the spatial filter was to place the aperture at a focal
point  that represented the far field pattern of the laser,  i.e., the pattern that would be
                                    o
formed at a plane located  more than  w /X from the  coupling mirror of the laser,  [f
one places a short focal length lens at the exit of a laser with a near-collimated output.
beam, then the far field pattern will  occur at the point where the beam diameter is
minimum (the waist) which would also coincide with the focal point of the lens. In the
more usual case as in the ILAMS,  none of these points coincide.  A  waist is formed
within the 762 mm long portion of the laser cavity between the coupling mirror and

                                       59

-------
                           SPATIAL FILTER DIA. - 1 mm
              SIGNAL
              OUTPUT
OS
o
                                                                                  25 mm
                                                                                  DOUBLET
                                                            TO
                                                            REFERENCE
                                                            APERTURE
                                                  Figure  17.  Spatial Filter Experiment Layout

-------
                        E
 a. AMPLITUDE DISTRIBUTION OF THE FUNDAMENTAL BEAM
/
i

p
1
/
1
1
f
1
0 I
1
1
1
1
\ ^




1 K
\
I
1
\ f


w
k
1


    b. POWER DISTRIBUTION OF THE FUNDAMENTAL BEAM
Figure 18. AMPLITUDE & POWER DISTRIBUTION OF THE
          GAUSSIAN FUNDAMENTAL MODE
                           61

-------
                                          WITH CLEANUP APEKTIWE

                                          WITHOUT CLEANUP APEKTUKK
Figure 19. CONTOURS OF EQUAL DENSITY AT X = 9.504pn WITH
          AND WITHOUT A CLEANUP APERTURE
                            62

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the concave mirror at the vertex of the "V".  The design called for this waist to be
positioned midway between the two mirrors, but it actually lies closer to the coupling
mirror.
       The true position of the waist (364 mm from the coupling mirror)  was determined
by computer simulation of the laser  cavity and confirmed by measurement of the
exit beam.   A new waist is formed by the first lens following the coupling mirror and
then again by the doublet as indicated in Figure  17.  The position of these new waists
does not coincide with the position of the real1 image of the waist of the beam within
the laser cavity, but this fact does not reduce the effectlvenss  of a clean  up aperture
located at a particular waist. The aperture will strip off any undesirable side lobes
in the diffraction pattern that represent high frequency clutter  in the near field.  Tho
ideal optical configuration following  the clean up aperture is a  large transmitting
telescope that would pick up the major side lobes of the diffraction pattern of the
clean up aperture itself yielding good image of the clean up aperture on the retroreflector.
                                       63

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 E.  SEALED ISOTOPIC LASER DESIGN



 1.  Introduction



      An isotopic CO^ laser in ILAMS offers additional pollutant detection capability


 compared to the natural isotope, flowing CO laser In current use.  Figure 20 illustrates

                                      13   16
 its greater spectral coverage.   Use of C  C>2  In the plasma tube adds, among others,


 HNO ,  PAN.and PBzN to the system's list of potentially detectable pollutants.  With

  12  18
 C  O2   in the plasma tube a suitable absorption coefficient for long path monitoring of


 SO  has been reported. (Reference 18)



      The C02 laser produces high CW power at high efficiency, i.e.,  more than 1  kw


 at up to 15% efficiency.  Patel (Reference 19) demonstrated CO lasing at approximately
                                                           £1

 10.6 and 9.6 microns and, subsequently, Moeller and Rigden (Reference 20) demonstrated


 CO2 lasing at approximately iO. 6 and 9.6 microns and,  subsequently, Moeller and


 Rigden (Reference 19) demonstrated lasing in both the P and R branches of the rotational


 lines up to J values of over 50.   Figure 20a shows the wavelengths at which lasing has


 been achieved by the investigators cited.



      The use of the heavier, stable isotopes of carbon and oxygen shifts the energy


levels of the CO2 molecule.  Figure 20c shows the predicted lasing wavelengths for


the isotopic form of carbon dioxide, C13O l6.  These predictions were based on
                                       Li

measurements of the molecular vibration levels of carbon  dioxide  by infrared
                                         64

-------
                                                                                                 CI2<46 CALCULATED
                                                                                                'AND MEASURED
                                                                       12
                                                                                                     6- c1 V
                                                                                                'MEASURED
Ul
                                                                                                      CALCULATED
                     r
 ~t  .
9

•P
                   f
            r—
           9.0

9.5
10.0              105

WAVELENGTH (MICRONS)
                                                11.0
                                    II 5
                                                                                                 a
                                                                                                 ~
-------
 CI202'8
 CI20217
 c'2ol7o'8
 CI20I6018
 c'W7
 CI202'6
CI30218
CI30I60I8
CI30I6017
c'6
                                                                 10
                                                                                                                       II 7
                                                     WAVELENGTH.   MICRONS
                                 Figure 21.  CALCULATED CO9 ISOTOPE BAND CENTERS

-------
 spectroscopy.  Verification of these predictions has been achieved using a mixture

              1 Q   1 f*               1 9   1 fl

 of 55 to 60% C O    and 40 to 45% C  O   .  Spectral measurements of these lines
                 2                     2

 with an infrared monochrometer were made at a resolution of +0.01 micron.  Figure


 20g indicates  the spectral region spanned by the laser using the isotopic mixture

  12  18      n   16
 C  O    and C  O   .  Note that lasing  is occurring at the allowed transitions for
     Z            £t

 both isotopes.  Figures 20f and 21 show the band centers for several isotopic forms of


 carbon dioxide for both the 00 1 - 02 0 and the 00  1 - 10 0 transitions.  Figure 20e

                                                12   18
 shows measurements made of the lasing  lines of C  O    providing further verification
                                                  £t

 of the validity of the analytical results, Figure 20d.  These results indicate that the IR


 spectrum from 8.5 to 12 microns can be swept with a CO  laser filled with appropriate
                                                     1*

 isotopes.



 2.  LASER PLASMA TUBE  DESIGN CONSIDERATIONS



       The primary objective in the design of the plasma tube is high  gain. The


 requirement for spectral lines corresponding to remote "J"  values of  150  or more


using mixtures of  isotopes in a sealed CO  laser demands high optical gain of the
                                       &

working plasma.  In addition, the long path length (to maintain closely-spaced


longitudinal modes) with multiple path folding plus  a lossy spectral tuner within the


 optical cavity  of the laser produces losses that must be compensated for  with gain.



       Since the gain of the plasma in a CO  laser is exceptionally high,  laser


designers are usually more concerned with output power and efficiency for a given


working volume.  Power output is usually obtained through the use of large fundamental


 mode diameters and correspondingly large tube diameters.  Coupling  coefficients are


optimized for  maximum power output at the  P-20 line of the  laser.  For the scaled


laser designed for this laser system, the power output  of 1/4 watt is more than adequate.



       The "V" laser concept is designed to take advantage of the fact that the gain


of a laser is inversely proportional to the tube diameter.  The stable mode diameter


for the TEM QO traverse mode is proportional  to the square root of the distance


between curved mirrors for near confocal systems.  The advantage of the zig-zag


folding configurations of which the "V"  laser is the simplest example,  is that a  curved


mirror can be placed at each vertex and the beam diameter (and thus the tube diameter)


can be kept to  a minimum.




                                        (57

-------
       Once the smallest possible fundamental mode diameter is established,  llicn
the tube diameter can be chosen.  In general,  the gain increases for decreasing
plasma tube diameter until diffraction losses are introduced which exceed the  in-
crease in gain.  These diffraction losses are not introduced by the tube walls directly,
but by  the fact that the gain of the pumping plasma falls off near  the walls.  This
effect is  shown in Figure 22 to be a function of the exciting current.  In order  to
establish the optimum size the laser on-axis gain was measured in an experimental
setup as  a function of nominal beam diameter and plasma tube diameter for the case
of optimum plasma excitation  (determined experimentally during each run). During
each experimental run,  gain was measured with  a circular mode stop in place to
confine lasing to a fundamental mode.  A variable iris was used  as a mode stop and
was set at the largest aperture size that would constrain operation to the TEM QQ mode.
       The tube diameter for  maximum gain was found to correspond to 1. 532 times
the stop size that would produce 0.1B diffraction loss. This stop size  can  be
calculated using the curves of Kogelnik and Li (Reference  21). The advantage of a
folded  plasma tube configuration such as the "V" laser is  illustrated in Figure  23.
Note that a gain of 6.3dB may be obtained with two, 100 centimeter tubes,  whereas
a single, 200 centimeter tube  produces about 4.5 dB of excess gain.  The improve'ment
in gain is 1. 85 dB while incurring an additional loss of 0.1 dB because of the extra
folding mirror.  Aberration losses (coma) due to off-axis operation of the confocal
mirror at the vertex are negligible because of the small beam diameter (low f number)
within  the plasma tube.
       Because the glass  envelope of the plasma tube is highly reflective at grazing
incidence it is unfortunately easy for lasing to occur over paths not anticipated in
the original design.  To inhibit these "whisper"  modes constrictions are introduced

-------
                                                   TUBE WALLS
Oi
to
                                          r  I   I   r  I-  I   I,  i   ii  '•
                                        1.0  .8. .6 .4  .2 0  .2  .4  .6 .8 1.0.

                                              RADIAL POSITION ~ CM
                   Figure 22.  RADIAL GAIN PROFILE FOR A MIXTURE OF 1.8 TORR CO 2, 2.0 TORR N2
                             AND 4..6 TORR He AT WALL TEMPERATURE OF 13° AND DISCHARGE CURRENTS

                             OF : a.10 mA; b.20 mA; c.30 mA; d.50 mA

-------
     EXTRAPOLATED
     EXPERIMENTAL
     GAIN/METER
                     TUBE DIAMETER
                     FOR MAXIMUM GAIN
                                              OPTIMIZED GAIN
                                              OF SINGLE CONFOCAL CAVITY
      50         75         100         125         150         175

            LENGTH OF CONFOCAL CAVITY  (~ CENTIMETERS)

Figure 23. UNSATURATED  GAIN OF A CO2 LASER AT A J-40 TRANSITION
          CAVITY VS LENGTH ASSUMING THE TUBE DIAMETER IS OPTIMIZED
         FOR MAXIMI IM r;AIN

-------
in the glass tubing every few Inches.  These rings in the glass have an internal diameter
of one or two millimeters less than the I. D. of the bulk of the tubing; however they do
not increase diffraction losses because they are spaced too far apart to shrink the
diameter of the active plasma in the tube and are large compared to the mode stops
deliberately introduced to inhibit higher order modes.
3.  STABILITY CONSIDERATIONS
       Laser stability places a limit on the system performance.  Angular riucliiMtions
and frequency fluctuations produced by changes in the plasma or in the option I
alignment introduce spectral effects and measurement errors.
       Dimensional changes in the laser cavity are introduced by temperature .md
mechanical vibration.  These changes shift the laser's frequency, amplitude, ;md modi
pattern.  The percent change in laser frequency Is proportional to the percent change
in cavity length which is small (a few parts in 10 ) compared to the spectral bandwidth
of the gases we are trying to detect.  Amplitude fluctuations produced by changes in
alignment,  however, arc of major concern when they lead to mode hopping that mny
occur at some spectral lines and not others.  Table X gives some indication of the
alignment tolerances that must be maintained to achieve satisfactory mode stability.
Mirror Tilt
Milliradians
-
0.16
0.33
0.66
1.64
TEM QQ % Losses
2, 3%
2.5%
4.0%
6. 8%
35.0%
TEMQ1 % Losses
28%
28%.
32%
40%
75%
TEMnj Rejection Mode
12:1
1 1:1
8:1
6:1
2:1
            Table X.  Losses versus Mirror Tilt for a Confocal Resonator
                                     71

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       Frequency and gain can also be influenced by the excitation; however, the
effects on frequency stability as a result of changes in plasma current are con-
siderably less than that contributed by other sources.  The CO  laser will have a
                                                           Ci
frequency drift in the range of 0.5 to 0.9 MHz per milliamp change in excitation
current.   A typical current for a cooled laser is about 30 ma; thus, for a frequency
tolerance of 0.5 MHz the required regulation on the source current would only be
about 3.7%.  A typical setup for lasers uses large series ballast resistors.  Prior
to firing, the voltage at the electrode exceeds the maximum value needed for
ignition;  however, as current begins to flow, the voltage drop across the ballast
resistor  increases  rapidly thereby lowering the voltage across the electrodes to the
appropriate operating level.  The ballast resistor is chosen to accommodate the
desired voltage and is  very much larger than the dynamic impedance  of the laser (a
factor which improves current regulation by causing the voltage source and the
resistor  to appear as a current source across the laser electrodes).  If the use of
ballast resistors  is objectionable, because of power dissipation  in the ballast or
because of stability requirements, then an active current regulation system may be used.
4.  INTRACAVITY WINDOWS
       Practical  design considerations make necessary at least one window within  the
laser optical cavity to  seal off the plasma portion of the laser from the spectral tuner.
Considerable effort in  this design study was expended on the Brewster window problem.
The requirement  for wide spectral range tunability from the laser means that neither
anti-reflection coated windows nor Fabry  Perot etalons will suffice as a  window.  Metal
halides having adequate transmission  at 10.5 micrometers are unsatisfactory because
they are hydroscopic,  birefringent, and have been found to have poor surface quality.
Germanium and gallium arsenide have been the choice as Brewster windows to date,
but they have some disadvantages.  The index of refraction of these materials is high
(4.0 and 3.28 for Ge and GaAs respectively).  They are opaque to visible light.
                                      72

-------
The absorption of laser radiation is sufficiently high that the change of index ol n>~
 I'rnction with temperature distorts the beam as the laser conies up i.o a stable*
operating temperature.
        Until recently we felt that thin GaAs windows offered the best compromise.
 These windows can be polished to one (1) mm thickness maintaining a wedge angle of less
than 40 arc seconds between the front and back surfaces.  In practice they were cemented
to a kovar flange which was then cemented to the borosilicate glass laser tubing rut ;ii
the Brewter angle.  The kovar steel flange serves as a he:it sink to mmimi/e the
thermal gradients across  the window  which produce defocussing of the beam.  Kovar
was chosen because its thermal coefficient of expansion lies  midway between that ol
gallium arsenide and borosilicate glass.  Thermal flexing is the major source of |xist
sealing leaks in the laser  system.  The-sealing material  was Torseal high vacuum
epoxy which was then overcoated with General Electric HTV-lls.  The RTV is  used us
insurance against hairline cracks that may develop in the seal with very large arnbimi-
temperature changes.
       The recent introduction of vapor-deposition-fabricated /inc selonido windows
has changed our philosophy somewhat with respect to sealed laser system design  for
spectrally tunable CO  lasers.  The alignment procedure, which requires that all ihr
mirrors be lined up within one-half milliradian before lasing can occur, is quite
complicated when using an opaque Brewster window with even small  \vodftv angles.
However,  in the proposed  design, zinc sclenide windows which transmit in the visible,
and a coupling mirror external to the  laser plasma tube will allow relatively easy
alignment with a HeNe (G328A) laser.  The index of zinc sclcnido is  2.4 and  its
absorption  coefficient is lower by more than 4:1 than cither germanium or gallium
arsenide.   The smaller index yields a smaller Brewster angle and thereby somewhai
lowers the  tolerances on the optical surface  flatness.
                                         73

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 5.  SPECTRAL TUNER DESIGN
        Because of its high dispersion, relatively low losses, and easy maintainability,
 the reflectance diffraction grating has been the choice as a spectral tuning element
 for use within  the laser cavity.  Other possible approaches such as metal halide
 prisms, Fabry-Perot etalons and dielectric fibers have been evaluated under earlier
 study programs (Reference 22).
        Used as an end mirror in the laser cavity,  a blazed reflectance diffraction
 grating designed for 10 microns has a dispersion of approximately 100 milliradians/
 micron. The measured reflection efficiency of a Bausch and Lomb aluminized replica
 grating, to CO^ laser radiation at ten microns, was 95 percent at the proper polarization.
 There is some change in properties with temperature at moderate  power levels near
             2
 100 watts/cm  .tending to increase losses.
        The  efficiency of a blazed, reflection, diffraction grating varies as a function
 of wavelength and angular orientation of the grating with respect to the incident radiation.
 Except for approximately 3% absorption and scattering losses (using a gold overcoat)
 all the losses from the first order reflection go into the  zero order reflection.  (The
 direction of the zero  order  reflection is such that the angles of incidence and reflection
 are equal about the normal to the grating surface). This zero order out-coupling can
 be adjusted by  selection of blaze angle, grooves per mm, and angle of orientation, and
 varies strongly with wavelength.
       The grating must be oriented with the grooves horizontal (with path folding
 in the horizontal plane) so as to minimize the zero  order reflection losses for both
 ingoing and outgoing reflections.  The first  order reflections from  the grating arc
dispersed in elevation with wavelength. The shorter  wavelengths,  for example, are
directed slightly downward (the grating is facing  slightly downward) and the longer
                                      74

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 wavelengths reflect upward.  The separate beams are collected in groups by the Hat
 mirrors and redirected through the chopper wheel In a convenient orientation for
 sequential shuttering.  The shorter wavelengths strike the lower mirrors and the
 longer wavelengths reflect off the upper mirrors.  Because of the redirection ol' tin-
 beams by mirrors, the position of the beams at the chopper and the wavelength
 separation end mirrors  is not proportional to wavelength.  The number and location
 of the mirrors following the diffraction grating and the respective position of the holes
 in the chopper wheel both depend upon the wavelengths selected for the particular
 target detection problem.
        The optical design  of the laser cavity to  include the grnting clement as a
 spectral tuner involves several,  sometimes conflicting, requirements:
        1. High spatial resolution between adjacent spectral lines at  the end
          mirrors so that adjacent spectral lines may be used in the same
          laser system.
        2. Large angular resolution between adjacent spectral lines so that un-
          wanted spectral  lines may be tuned out by angular alignment of the
          end mirror.
        3. Low aberration losses  from curved folding mirrors which must be
          operated off axis.
        4. Small losses from the grating which must also be operated off axis.
                                2
       5. Less than 100 watts/cm  power density on the grating surface.
       The spatial resolution of the spectral tuner is dependent primarily upon the
diameter of the laser beam incident upon the grating and the dispersion of the grating.
Spatial resolution is measured by the spacing between adjacent spectral  lines
( A^ =  0.007 to 0.026 urn)  in spot diameters at the end mirrors.   If  the grating has
a dispersion ft  then the resolution  is given by:
                                          75

-------
          R -  /$ 7/w      diameters/micrometer                       (5)
                  A
where w is the nominal diameter of the beam at the  diffraction grating.  For
example,  if the spectral separation between two lines at 9.2 micrometers is
0.01 micrometers and ^3= 0.1 radians/micrometer, then in order to get a spectral
separation of four diameters, the beam diameter on the grating must be:

               4 A	     4 x 0.0092 mm
     w=  	= 	 =11.1 mm          (6)
             0.1 if x .01               .OOlrr                            v  '

In order for the grating to accommodate this beam without introducing appreciable
diffraction losses within the laser cavity,  it should be four diameters wide, which
is 46. 8  mm or 1. 84 inches in diameter.
       The use of a large beam on the grating poses another difficulty.  Because the
surface of the reflectance grating is inclined with respect to the vertical, beams with
high numerical apertures (small f numbers) introduce large aberration losses.  For example
the "V" laser used in this program uses a spherical mirror of one meter focal length
to focus the beam on the end mirrors via the grating.  The beam diameter at the
grating  is 2. 9 mm yielding a numerical aperture of  NA = 1/2 x 2.1/1000 = .00145 for
which the  losses are negligibly small.  However,  in order to obtain the  resolution
indicated above, the numerical aperture for the same focal length mirror would be:
          NA = 1/2 x 46. 8/1000 = . 0234                                   (7)
Measurements with the laser system using just this numerical aperture on the
diffraction grating resulted in diffraction losses in excess of 3dB making the laser
virtually inoperable for this configuration on any but the strongest transitions.
       In  addition to the requirement for spatial resolution, it is necessary for the
spacing from the  grating to the end mirrors to be large in order to preserve the
angular resolution.  The angular  resolution is given by:
          R = p  (1 -a/F)                                                (8)
                                    76

-------
 where
        p is the dispersion of the diffraction grating
        a  is the spacing from the grating to the last concave mirror
          or focusing mirror, and
        F is the focal length of the mirror.
        The  conflict between requirements is indicated in Figure 24.  The nngle, A,
 between mirrors Ml and M2 should be kept small to minimize  zero order losses
 from the grating and the angles C and D at the mirrors must be minimized Lo reduce
 off axis aberration.  The off axis image is degraded by coma,  which is given by:
         a  =   6
           T   16       (f No.)2                                         (9)

where aT is the third-order tangential coma expressed in the snmc units of angle
as u,  which is the semi-field angle.  Note that for a given f number the coma increases with
the square of the  beam diameter and linearly with the off axis (semi-field) angle.
The only way to reduce "C" and "D" is to reduce the beam diameter and make
dimension "a" small.  The beam diameter is set by'the requirement for sprttinl
resolution, and "a"  is necessarily small because mirror  M2 must intercept all the
spectral lines dispersed by the grating.  Alternate approaches are:
       1.  Forego the use of spectral lines that are closely spaced in wavelength
          and use small diameter beams of low numerical aperture at the
          diffraction grating.  This  approach is used in the General Electric
          ILAMS  System.
       2.  Use off axis parabolas with  long focal length (greater than 2.5 meters) in
          the configuration shown in Figure 24.  This will permit the dimension "a"
          to become as large as  O.G meters and keep angle "A"  small.  The  axial
          image formed by a paraboloid is well known to be free  of geometric
          aberrations.  This method is recommended for the proposed sealed
          system design.  f
                                      77

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-0
00
                                                               LASER BEAM
                                                               FROM PLASMA TUBE
               ,/xBBB	
          WAVELENGTH
          SELECTION
          END MIRRORS
                                    "CHOPPER WHEEL
                                       Figure 24. LAYOUT OF LASER OPTICAL SYSTEM

-------
 6.  SEALED LASER DESIGN CONSIDERATIONS




        The problem of building a CO  laser using the less common isotopes of
                                   £t

 carbon and oxygen is to construct a sealed plasma tube that will last from two to


 five thousand hours without serious degradation in gain.  The techniques for


 accomplishing this require a marriage of the arts of vacuum technology and


 laser physics.




        Because of the high cost of carbon-13 and oxygen-18, the COf laser must


 be operated as a sealed (non-flowing) system.  The gain, power output, and life


 time  of a sealed CO  Jaser are a function of the gas mixture,  the tube diameter,
                   L*

 the proximity of the path taken by the laser beam to the walls,  the means of


 excitation and the electrode structure  and materials.  The sealed CO  laser shows
                                                                 &

 a gradual decay in gain and hence in power output with operating life,  m order to


 have  an operating laser detection system, the gain within the plasma envelope must


 be kept greater than the optical cavity's  fixed losses  and including those of the output


 coupling mirror, while maintaining an internal power density compatible with the


 desired output power.   This minimum  gain requirement  must be  met throughout the


 operating life of the plasma tube  and at the weakest laser transitions that are to be


 used  for gas  detection.




       This program included a detailed study  and experimentation of the effects


 of gas fill mixtures, plasma tube configuration and  excitation on la.ser performance


 and lifetime.  A large background of work has already been accomplished by a variety


 of investigators in the areas of laser gain and lifetime using the most common isotopic


form  of carbon dioxide, i.e., C   O 1U (References  23,  24,  25, 2f>, 27 and 28).
                                 £1


Witteman (Reference 23) achieved 10,000 hours of continuous operation


with a forty watt CO  laser operating at 10. G micron  wavelength.  The results of this


work  have been extremely  valuable to us, but there are significant differences


between the 10. G micron laser and the  laser designs being considered.  The isotopic
                                       79

-------
 CO  .aser must maintain high gain over a large number of wavelengths at high J

                         12   18
 values.  The purchased C  O    isotopes will necessarily be contaminated with
                            Lt


 more than ten percent CO     .At each wavelength corresponding to energy
                           z

 transitions in both of the  CO gases, the gain-saturation characteristic is
                           u

 different.  The gain-saturation characteristic at a wavelength corresponding to on


 energy transition  in one of the isotopic forms is influenced by the presence of


 other species because of  the competition effects.  The optimum ratios of carbon


 dioxide to the other gases in the system are not the same for all isotopes of mixtures


 as for ordinary CO .
                  &


       The lifetime of the CO  laser is directly related to the gas mixture, the
                            Lt

 cleanliness of the  internal surfaces of the plasma tube and the flow rate from out-


 gassing and leaks. A gas filling station must be used to bake out the plasma tube


 under high vacuum, to fill the plasma tube with the desired mixture of the isotopic


 forms  of CO ,  N  , He, Xe, and HO, and to monitor the partial pressure of each
            L*   &                £t

 gas.  (See Figure  25).




       When direct current excitation of the plasma is used the electrode  material


 and the configuration of the electrodes are extremely important to the laser lifetime.


 The electrode material may act as a sponge to some of the gases in the laser,  it


 may act as a catalyst for  the production of undesirable compounds and it may sputter


 away material from the cathode which may  in turn react with  the gases in  the laser


 or batter  them against the glass walls of the tube.  Platinum is  one of the  better


 choices as an anode material because it does not encourage the  production of


 compounds (carbonyls,  etc.) that  Interfere  with lifetime, nor does it oxidize to use


 up the  oxygen in the CO . However, platinum is a notorious sputterer and therefore
                      £

not suitable as a cathode material.  Cathodes  made from high purity nickel and


 designed to operate at from 300  to 500 degrees Centigrade have been tested and found


 to be acceptable.
                                        80

-------
oc
                                                                   LASER
                                                                         FLEXIBLE
                                                                         COUPLING
                    ULTRA-HI VACUUM
                    BAKEABLE VALVES
                                                                              CAPACITANCE
                                                                              MANOMETER
                                                                                     TO
                                                                                     ROUGH
                                                                                     PUMP
                                                                               ABSOLUTE
                                                                               PRESSURE
                                                                               MILLIMETERS
                                                             ION
                                                             GAG!
                                                             TUB!
                                                                       TO
                                                                       ION GAGE
                                                                       CONTROLS
STAINLESS STEEL
FLEX TUBE
                                                                                   NUPRO
                                                                                   BELLOWS
                                                                                   VALVES
                         SI L1C ON h
                         RUBBER
                         SEPTUM?
                                                                           TO DIFFUSION
                                                                           *.-  ROUGH VACUUM
                                                                           PUMPS
               \VATEK
               INJECT
                                              Figure 25.  MANIFOLD FOR HIGH VACUUM FILL STATION

-------
       Another essential ingredient for long lifetime in a sealed laser is to maintain
a partial pressure of approximately 1.5 torr of water vapor in the gas mixture.
Because the electrodes and the glass walls tend to absorb HO, it is necessary to
                                                       u
add to the laser several times the amount of water needed to fill the plasma tube
volume  to 1.5 torr.  The water vapor is introduced  into the plasma tube through a
double septum of silicon rubber with a rough vacuum held between the two septums.
This approach prevents the introduction of atmospheric gases into the plasma tube.
The system is allowed to come to stable equilibrium with the water vapor following
each injection and  the amount of injected  HO is adjusted for peak laser power output.
                                        £
A small container of Linde 4-a Molecular Sieve material Is tied to the plasma tube
as a reservoir of water vapor to compensate for any long cleanup by the electrodes
and the glass walls.
       A second reservoir consisting of a large bottle attached to the laser plasma
tube is used simply to increase the total gas mixture volume available to maintain
maximum sealed lifetime.  If the gain of  the laser falls below threshold because of
normal  degradation of the fill gas mixture then the refilling process can be  accomplished
fairly quickly at the gas filling station. If a  leak is  the cause for laser failure, however,
then the internal surfaces will have absorbed gases  from the air which will  have to be
removed by bakeout of the glass  and high temperature bakeout of the  electrodes with
an induction heater.  The bakeout process requires  several days.
       Determining the laser gas mixture for optimum unsaturated gain is a tedious
business because of the large number of variables.  The optimum mix determined
             12   18
for use  with C  O     is:
                                 Torr
          Carbon Dioxide         4.5
          Helium                 9
          Nitrogen                2
          Xenon                  1
          Water Vapor            1. 5
                                        82

-------
                                                                      12   18
Given this mix as a starting point, the optimum mix using ninety percent C  O

             12   16                                                      ^
ten percent C  O    can be determined by trial and error monitoring output power.
                jL




 7.  PROPOSED SEALED LASER DESIGN



        The critical elements in this sytem are the seals, reservoirs,  and the gas


 fill mixture.  Bakeout with a good, high-vacuum filling station is essential.  The


 proposed sealed system design is illustrated in Figure 2f>.  It is a water-cooled "V"


 shaped plasma tube with two Brewster windows.  The coupling mirror will not be


 connected directly  to the plasiiia tube as in the present ILAMS system  laser. This


 avoids the problems associated with a flexible seal between the coupling mirror and


 the plasma tube, which was necessary in order to obtain adequate  alignment of the:


 optics. Such  a seal presents a high vacuum problem and must be. insulated against


 the high voltage between the plasma tube and the support frame. The tube is necked


 down by two millimeters at regular intervals to inhibit whisper modes  from developing.



        The Brewster windows are of zinc selenide and are cemented directly to


 the laser tube with  high vacuum  epoxy Torseal.  The epoxy is then over-coated


 with RTV-118 as a  seal against hairline cracks that may appear in the  epoxy as :i


 result  of age or large temperature changes.  The laser tube and associated glass


 plumbing is made of pyrex type borosilicate glass (Glass Code Number 7740).  At


 the two ends where the Brewster windows are sealed this glass is graded to a soda


 lead glass (Number 0120) which  is a better match for the thermal coefficient of


 expansion of  zinc selenide.  The glass is cut to the approximate Brewster angle


 and then hand ground to meet the Brewster angle and to provide a smooth,  flat


 mating surface for the window.




       The length of the tube is approximately 1.1 meters with a convex one-meter


 radius-of-curvature gold mirror at the vertex. The glass tubing at the vertex is cut


;md hand ground to prealign the mirror which is cemented directly to the glass.  This
                                       83

-------
2-
         CONCAVE MIRROft
         SEALED TO GLASS
                                              XENON RETURN
                                                   NECKDOWN
                                                   EVERY 30 cm
	PLATINUM
\ANODE
                                                                                LINDE
                                                                                4-a RESERVOIR
                                                                                                                                           22.6  ANGLE
                                                                                                                                           FOR BREWSTE
                                                                                                                                           WINDOW
                                                     Figure 26.  Proposed Sealed Isotopic Laser Design

-------
again, is to avoid sealing and high voltage problems.  Water cooling of the tubes out
beyond the electrodes provides sufficient temperature stability so that alignment is
maintained.  A circular metal aperture is cemented to the center of this mirror as a
stop for higher order modes.
       Xenon being a heavy molecule tends to drift in the plasma toward the cathode
so a return or bypass is provided for each leg of the "V".  This bypass must have
smaller diameter and/or longer length than its associated plasma tube  in order to
prevent the discharge from firing along the bypass.
       A gas reservoir is attached to one of the legs of the "V" and the inlet valve is
in turn connected to the reservoir.  This is a high vacuum bellows type valve with
sufficiently high conductance to allow bakeout of the system in less than a week at
temperatures of 250 degrees Centigrade.  A second reservoir of molecular sieve
material is used to keep the water vapor concentration fixed in spite of the clean up
effects of the internal surfaces of the system.  The capacity of the molecular sieve
material is large compared to that of the inner surfaces at the same vapor pressure.
       The anode is platinum and the cathodes are made from Number 270 Nickel.
They are 6 mm cylinders with a 2.6 mm hole drilled in one end.   The other end is
welded to a kovar wire for the glass seal.
                                         85

-------
                                  REFERENCES
 1.   L. R. Snowman and D.R. Morgan, "Studies on An Isotopic CO  Laser LOPAIR
                                                           £t
     System," Department of the Army Edgewood Arsenal DDEL, First Quarterly
     Report, Contract DAAA15-72-C-0359,  February 1973.

 2.   L.R. Snowman, D.A. Ware, and D.R. Morgan, "Gas Laser Detector", Air Force
     Armament Lab., Eglin AFB, Florida,  Ftnal Report, Contract F08635-68-0116,
     September 1969; also, General Electric Company, Electronics Laboratory, Syracuse,
     New York, Report No.  R69ELS-1, September 1969.

 3.   D.R. Morgan and D.A. Roberts,  "Computer Signal Processing Study",  Dept. of
     the Army, Edgewood Arsenal DDEL, Final Report, Vol.  1: Analytical Results,
     DAAA15-71-C-0186,  September 1972.

 4.   J.H.  McCoy, D.B. Rensch and R.K. Long, "Water Vapor Continuum Absorption of
     Carbon Dioxide Laser Radiation Near IQn" Applied Optics Vol. 8, No. 7, pp 1471-
     1478, July 1969.

 5.   W.A. McClenny,  EPA,  Private Communication, August 1973.

 6.   E.H.  Christy, Tulane University, Private Communication, June 1973.

 7.   P.L.  Hanst, EPA Research Triangle Park, North  Carolina,  Private Communication, 1972

 8.   L. Gaslorek, Stanford Research Institute, Private Communication, August 1973.

 9.   R.A.  McClatchey, et al., "AFCRL Atmospheric Absorption Line Parameters Comp-
     ilation", Air Force Research Laboratories, Bedford, Massachusetts, AFCRL-
     TR-73-0096, January 1973.

 10.  R.K.  Long, Ohio State University, Electroscience Laboratory, Private Comm-
    unication,  September 1973.

 11. G. L.  Trusty, "Absorption Measurements of the 10.4 Micron Region Using a CO
                                                                           Lt
    Laser and a Spectrophone" Air  Force Avionics Laboratory, Wright-Patterson AFB,
    Ohio,  AFAL-TR-72-413, January 1973.

12. W.A.  McClenny, EPA Research Triangle Park,  North Carolina,  Private Comm-
  .  unicatlon,  September 1973.

13. D.E.  Burch, "Semi-annual Technical Report; Investigation of the Absorption of
    Infrared Radiation by Atmospheric Gases" Phllco-Ford Corporation, Aeronaut-
    ic Division, Contract No. F19628-69-C-0263,  U-4784, January 1970.
                                      86

-------
14. D. E.  Burch, "Radiative Properties of the Atmospheric Windows" Conference on
    Atmospheric Radiation, pp 61-68, August 7-9, 1972, Fort Collins, Colorado;
    published by AMS,  Boston, Massachusetts.

15. H. R.  Carlon, "Model for Infrared Emission of Water/Aerosol Mixtures" Applied
    Optics, Vol.  10, No. 10, October 1971.

16. P. L.  Hanst,  NASA Electronics Research Center, Cambridge, Massachusetts,
    Private Communication, 1970.

17. D. R.  Morgan and D.A. Roberts, "Computer Signal Processing Study" Final Report,
    Vol. 2: Computer Programs, Dept. of the Army,  Edgewood Arsenal, Contract
    No. DAAA-71-C-018G,  September 1972.

18. R. T.  Menzies,  "Remote Detection of SO  and CO  with a Heterodyne Radiometer"
                                        2       2
    Appl. Phys. Letters, Vol. 22,  No. 11, p592,  1973.

19. Patel, Phy.  Rev. 136, 5A, November 1964, pAH87.

20. G. Moeller and J. Ridgen, Appl. Phys. Letters Vol. 8, No. 3, p 68, 1966.

21. H. Kogelnik and T. Li, "Laser Beams and Resonators" Proceedings of the IEEE,
    Vol. 54, No.  10, October 1966.

22. L. R.  Snowman, "Laser Coincidence Absorption Measurements",  General Electric
    Co., Electronics Laboratory Report No.  R72ELS-15, March  1972.

23. W.J.  Witteman, "Sealed-off High-Power CO  Lasers"  Phillips Technical Review,
    Vol. 28, Nov. 10, 1967.

24. R.J. Carbone, "Characteristics of a Single-Frequency Sealed-off CO  Amplifier"
    IEEE  Journal of Quantum Electronics, January 1969.                2

25. V. Hoffman and P.  Toschek,  "One-year Operation of Sealed-off CO   Laser"
    IEEE  Journal of Quantum Electronics, November 1970.

26. R.J. Carbone, "Continuous Operation of a Long-lived CO  Laser Tube" IEEE
    Journal of Quantum Electronics, March 1968.           2

27. H.W.  Mocker and H. A. Gustafson, "New  Contender for Space Communication"
    Laser Focus, October 1970.
                                   87

-------
28. W. J. Wltteman and H. W. Werner,  "The Effect of Water Vapor and Hydrogen on
    the Gas Composition of a Sealed-off CO Laser" Physics Letters, Vol.  26A,  No.
    April 10, 1968.

29. M.M. Whatiey and D.A. Smity "Atmospheric Effects on Digitally Modulated Laser
    Transmission" U.S. Army Electronics Command, Fort Monmouth, New Jersey,
    Tech. Rep. ECOM-3005, July 1968.

30. R. Paulson, E. Ellis and N. Glnsburg,  "Atmospheric Noise Measurements" Air
    Force Cambridge Research Laboratories, Tech.  Rep.  AFCRL-62-869,
    AD 287 517, August 1962.

31. W. L. Wolfe, Handbook of Military Infrared Technology, Office of Naval Research,
    Dept. of the Navy, Washington, D.C., 1965.
                                   88

-------
                             APPENDIX A
   INTERFERENCES

      Anything that frustrates the detection of the  IR absorption pattern associated
with  a particular gas is considered as a source of interference.

   System Noise

      System noise is composed of detector, optical, and other noise-
sources that arise in the measuring apparatus. This type of noise usually consists
of fairly rapid zero-mean fluctuations of the received energy.

      An actual instrument will time-average the  demodulated signal.   Therefore,
if response time is not a consideration, then the effect of system  noise may be
reduced to an arbitrarily small level by choosing a large enough integration time.
Of course, any real-time measurement problem does necessitate a finite response
time and so there are limitations on how much noise reduction may be  attained  in
this  manner.
                                       A-l

-------
      Detector noise is additive and usually uncor related between wavelengths for
 a scanning-type system.   The amplitude distribution of detector noise is Gaussian
 and its variance depends on the particular type of detector that is used.  The spectrum
 of the noise usually consists of a uniform thermal noise components and a  1/f
 "flicker noiseM component that dominates at lower frequencies.   Detector noise will
 be negligible if the source strength is large enough.

      Optical noise or "scintillation" is a modulating type of noise that results from
 inhomogeneities of the index of refraction in the atmosphere. ; This type of noise
 is strongly correlated between wavelengths over a large  range because the refractive
 index does not vary much with wavelength.   The amplitude  distribution of optical
 noise is log-normal (Reference 29) and its  variance is a function of aperture, range,
 and meteorological factors (Reference 30).  Its spectrum shape  is of a 1/f  nature
 (Reference 28) although the exact value of the exponent varies, depending on conditions.
 Unlike detector noise, the relative magnitude of scintillation noise does not depend  on
 Lht: source strength, since it is a multiplicative type of noise.

      Laser systems may be either optical  or detector-noise-limited.  Past experience
 indicates that, in most cases where a  cooperative reflector is used,  enough laser
energy is available so that detector noise can be neglected. Under these circumstances,
the laser system is optical noise limited.  Typical detector and scintillation noise
densities as a function of frequency are plotted in Figures A-l, and A-2, respectively.

      For a system corrupted by additive detector noise and multiplicative  optical
noise,  the  measured absorption at wavelength i is given by:
                                    -
                     A. --•- -log(MP.e  i   + N) + log P.                (A-!)
                                      A-2

-------
   100
                        Detector
 >
 c
0)
in
'5
Z
o
0>
   10
     10
                   Preamp
-1	1	L.
                  I _ I _ I  • I
                          Frequency - Hz

          Figure A-l. DETECTOR NOISE VERSUS FREQUENCY
                                                    IK
                           3 Mile Path
                           6" Aperture

                 "Optical Noise Measurements, " Report #AD 287517,
                 U .S .  Dept of Commerce
                              =    5.4
                                  f 1.25
                                 100
                         Frequency - Hz
                                                   IK
  Figure A-2. OPTICAL SCINTILLATION NOISE VERSUS FREQUENCY
                               A-3

-------
 where P. is received power,<*. the absorption coefficient at wavelength i and CL
 is the optical thickness or mass per unit area of target gas.  The optical modulation
 noise M is assumed to be distributed log-normal with unit mean and variance  cf   2
                                                                             M
 cycle of bandwidth.  The detector noise N is assumed to be Gaussian distributed and
 is specified by the noise equivalent power NEP of the detector which is defined as the
 amount of optical power necessary to produce a signal-to-noise-ratio of one at the
 detector output in a bandwidth of one Hz.  Here, the svstem is assumed to have been
 initially balanced by adding the quantity log  P. corresponding to CL = 0.

      If detector noise is  small, then for small  absorptions, (A-l) reduced to:

              A  =o-CL - log M - N/MP.,   (1 - 0" )  P »   NEP   (A-2)
               11                   i         M   i  '              '
 Each noise component in (4) is now additive and linear mean-square estimation
 theory can be applied.

      If detector noise is  not negligible, then some pre-log integration (filtering)
 is necessary in order to reduce the noise level  so that the approximation in  (A-2)
 can be made.

      The first noise component in (A-2), log M, is now zero-mean Gaussian-distributed
                       2
with variance log (1+0'M )•  The second noise term is somewhat more unwieldy in
 distribution.  However, if <7   ^» NEP and the second noise
 term can be neglected.
                                     A-4

-------
     Specific  Interferents
       An interfered is defined as any spectral absorber that may be present in
  sufficient quantity as to interfere with the detection of the target gas absorption
  pattern.  Unlike system noise, this type of  interference does not necessarily consist
  of rapid fluctuations and therefore  is not  appreciably reduced by increasing the
  integration time of the measurement.
       Neutral Attenuation
       One of the most dominent interferents in any system is neutral attenuation.
 This effect is caused by:
       1)  Unfavorable atmospheric conditions such as rain or fog,
       2)  Changes in the transmission or reflectivity of optical components
           (e.g. , dust accumulation on mirrors), and
       3)  Gain variations of electronic components (e.g. , respr.nsivity variations
           of a thermistor bolometer due to ambient temperature changes).

      An  automatic gain control (AGC) amplifier is used in the system to control
 large average variations  of signal level  and thereby reduce the dynamic range
 requirements of the signal processor.  However, neutral attenuation must still be
 considered as an interfered since it perturbs the absorption pattern.  Specifically,
 the effect of the  AGC amplifier is to adjust the system gain so that the average
 signal  level is constant.   For example if there is a 4% absorption at A  , then the
 AGC will  boost the average signal which will result in a 3% absorption at A  and
a -1% absorption at A 2> Agi and  ^   This effect is equivalent to the combination
of the 4% absorption at  A 1 and a -1% neutral attenuation.
                                     A-5

-------
      Other Specific Interferents

      The amount of an interferent that is present may be' regarded as a random
quantity.  The absorption pattern of a particular interferent is of the form:
                S. = I. CL,  i = 1, 2, ...,  n                           
where I. is the absorption coefficient of the interferent at the i  wavelength and C
is the average concentration of the interferent over the path length L.  This inter-
ferent constitutes a noise source whose covariance between wavelengths is given by:
                cov (S.S.) = I.I. var (CL)                             /A_4)

In the absence of detailed statistical information, the variance of the CL factor
may be bounded by the square of the largest CL factor that has been observed in
the field.  The danger in using such coarse statistical measures is that the actual
probability distribution is obscured.  This leads to difficulties if the system is
optimized by treating system noise and interferent noise on an equivalent rms
statistical basis, that is, by summing their covariances.  A more detailed discussion
is given In Appendix B.

    Random Interferents
      Besides the known interferents, there may be certain other intcrferents of
an unknown absorption pattern.  One  model that is both intuitively appealing and
mathematically tractable assumes a Poisson distribution of Lorentz-broadened lines
(Reference 31).
                                     A-6

-------
      It is shown in Appendix A of Reference 2 that the spectral autocovarianec
of such a model is given by
                                   C(0)                                  (
where C(0) is the variance of the noise, and a is the half width of the lines.   At
atmospheric pressures, a is on the
to some extent on the absorbing gas.
atmospheric pressures, a is on the order of 0. 1 cm  ,  although the value
      Thus, the random interference model is equivalent to a for related noise- soui-rc-
and can be lumped together with the other sources of noise.

    Other Interferents
      If a particular interferent is not well-defined or is of an unstable nature,  for
example, dependent upon meterological and/or environmental conditions, then a
factor analysis of this behavior pattern must be performed.  This implies that am
particular variation of the interferent ensemble can be suitably approximated by a
linear combination  of a set of factors.  Each factor is in turn considered as in
interferent in its own right and is used in the design of the linear spectral weights.
To the extent that the subspace spanned by the factors represents the interferent
ensemble, a design based upon such an approach will be  successful in rejecting this
interferent.

      Such an approach was taken in a previous  study (Reference 2) in which  dust
particulates were a serious source of interference.  For the present program it
appears that water  vapor may be of such a nature as to require a similar treatment.
This will depend  a great deal on the  results of the SRI simulation study which are
expected shortly.
                                     A-7

-------
                                 APPENDIX B





     OPTIMUM LINEAR WEIGHTS






     Introduction and Notation






       In this Appendix, techniques for the design and evaluation of optimum linear


weights for detecting and estimating quantities of spectral absorbers and discussed.


They are a summary of the results derived in Reference 2.  The purpose of


determining optimum systems is to establish a theoretical limit on the performance


that may be obtained.   This limit can then be used as a goal in the design of actual


systems,  that is, a frame of reference by which tradeoffs between  complexity and


performance  may be reasonably conducted.  In addition, optimum solutions often


serve as a guide in designing an actual system.   If a solution is arrived at by this or


any other means and it is close to optimum, then there is no need to search further.





       Spectral information will be contained in the transmission values  T , T ....  T
                                                                     12       n

 where n is the total number  of wavelengths used.  If a single absorber is placed in the


 sample region, the transmission at each wavelength will be of the  form
                      •

                                                                        (B-l)
                        T  =exp  (-A.C  L) , i = I, 2	n
                         1         L f\


 where A  is  the absorption coefficient  of absorber A at wavelength i, C   is the
                                                                   f\

 average concentration of absorber A over the total optical path,  and L is the total


 optical path  through the sample region.  Typically, C has units of  grams/liter or


 atmospheres of partial pressure,  and  L is in centimeters.  A is in units to make  A
 _                                                        i                    i

 C  L dimensionless.
  /\


       In vector notation, eq. (B-l) becomes
                                                                       (B-2)


                        T= exp(-A CL)
                                       B-l

-------
 where A - (A   A ,...,A  )' and T = (T   T  ... ,T )' are n-dimensional column
             i   ^       n           i    L       n

 vectors representing the absorption coefficients of absorber A and the transmission


 values of the sample region, respectively, and the prime (') denotes transpose.  If


 a second  absorber B with absorption coefficients J3 is introduced into the region, the


 net transmission will be the product of the transmission due to each absorber;  thus:



                       T = exp (-A C  L - B C_L).                     (B-3)
                                   A       B


      First, some discussion of possible patterns is necessary.  Figure B-.1 shows


 possible transmission patterns for an  absorber A  characterized by absorption co-


 efficients, A^^ = 1 liter/gm-cm and A  =  5 !iter/gm-cm, and a second absorber B


 characterized by absorption coefficients,  B = B  = 1 liter/gm-cm.  Transmission
                                         .L.    4J

 patterns are plotted  for various amounts of each single absorber.  Some mixtures


 of the two absorbers are shown in Figure B-2.  All possible mixtures of A and B will


 be a smooth distribution lying between the contours for each pure absorber.  For


 small absorptions, i.e., 1- T.   «   1, eq.  (B-3) becomes



                        T=1-ACL-BCL,                     (B-4)



where 1 - (1,  1	1)'.



If the measured transmission is subtracted from a reference level at each wavelength,


the signal is




                       S= 1 -  T~AC  L4 BC_L.                   (B-5)
                           -         t\    —  D


Under these circumstances, the absorption coefficients add vectorially and a linear


space is defined.






     Another method of displaying transmission patterns is to plot the natural  logs


of the transmissions.  Let  S = -In T.   If T is due to several  absorbers,  then



                       S = A  CL+ B CL+  ...                        B-<1
                                     B-2

-------
                                     A] = 1 liter/gm-cm
                                     A2 = 5 liter/gm-cm
                                     B] = 1 liter/gm-cm
                                     CL = 0, 1, 2, 3 gm-cm/lifer
   Figure B-l .  POSSIBLE TRANSMISSION PATTERNS FOR SINGLE ABSORBERS
Figure B-2.  POSSIBLE TRANSMISSION PATTERNS FOR MIXTURES OF ABSORBERS
                                   B-3

-------
which is the exact version of eq.  (B-5).  Figure B-3 is the equivalent of the patterns
of Figure B-2.  For this method of display, a linear space is defined for all
absorption levels, and so the vector for each absorber is constant in direction,
has a magnitude proportional to CL, and obeys vector addition.  Visualization of
possible transmission patterns is also easier in this manner.

      The linear model adequately represents the actual process and hereafter,
it is assumed  for this discussion  that the linear vector space model adequately
represents the actual process over the range of interest either by  virtue of small
absorptions or by a log transformation.  The system can therefore be considered
as a black box with an output column vector X that is composed of the sum of a
signal vector  A and a noise component N that represents all sources of  interference.
The signal vector represents the  absorption coefficients of the target gas over a
selected set of wavelengths.

      A detailed mathematical derivation of optimum linear weights is given in
 (Reference 32) and the major results are summarized in this section.  The optimum
linear weights maximize the  signal-to-noise-ratio
                       0 - W'A/(Var W'X) 1/2                     (B~7)
for various constraints.

    Unconstrained Weights

      The direction of the optimum unconstrained weight for a single target in a field
of correlated  noise is derived as
                 W = Z  ~1A                                      
                                      B-4

-------
                0
Figure B-3. POSSIBLE PATTERNS FOR THE NATURAL LOG OF THE TRANSMISSION
                                  B-5

-------
 where E  is the covariance matrix of the noise vector and A is the signal vector
 which represents the absorption coefficients of the target gas.   The optimum signal-
 to-noise  ratio is given by
                        t     MA'E'
                         max   -      -
                                                 2
 If the noise is uniform and uncorrelated.then £ =0  1 and W is the "matched filter"
 for the signal vector.
      The composition of C takes into account the interferents as well as other
 sources of correlated or uncorrleated noise.  If an interferent is of the form P \
 where/»is a random variable and T = (I   I     . ,i ) is a fixed pattern vector,  then
                                       i  L.      n
 its contribution to the total covariance matrix is
                      O" .. = 11. var (P\                                (B-10)
                         i]    ij
 For a spectrally absorbing interferent gas, the quantity/? represents the CL factor
 or mass per unit area.  In addition,  the covariance matrix provides a convenient
 means of handling random interferents since  this is just another correlated noise
 source.  A detailed description of interference was covered in the Appendix A.

      The disadvantage of a signal-to-noise optimization is that all interferences arc
 characterized only by second-order statistics.  This leads to difficulties if system
 noise and interferent noise are treated on an  equivalent rms statistical basis, that is,
 by summing their covariances.  The reason for this is that while the system noise
probability distribution is fairly well-defined, an interferent distribution may  be of a
very non-stationary and erratic nature; e.g., a passing truck stirring up a dust cloud.
 For these reasons, it is often desirable  to design a system in which certain "well-
behaved" interferents are described by the covariance matrix and a null response  is
required for the more irregular distrubances.
                                      B-6

-------
    Orthogonal Weights






      Orthogonality constraints of the type




                    W. J. =0, j = 1, 2,...,  m <  n                          (B-li)



 are now considered.  That is,  a zero response is required for certain interferents


 of a perverse nature.  It is shown that the direction of the optimum weight is given


 by



                     W =  PA                          .                       



 where

                     P = E    I I - Q(Q' £ ~ Q)  Q1 £ ~



 and


                    Q= (I., L	I  )                                       (R-14)
                          i   ^      m




 is an  n x m partitioned matrix whose columns consist of selected interferent vectors.


 The optimum SNR in this case is given by
                        max
                            =(A'PA,1/2
                               —  —'
If the noise is uniform and uncorrelated, eq.  (B-13) reduces to


                                  -i                                        (B-1G)
                     P=I-Q(Q'Q)  Q' .




This form has the simple geometric interpretation of dropping a perpendicular from


the  signal vector down to the subspace spanned by the m interferents.






      On the other hand, if there are no orthogonality constraints,  Q = (),  and eqs.


(B-12) and (B-13) reduce to eq. (B-8) as expected.
                                     B-7

-------
      An alternative method of imposing orthogonality constraints is to assign an
 equal amplitude variance n to the m interferents and to include them in the covariance
 matrix using eq. (B-10) it can be shown that as /z becomes large, the optimum weight
 calculated by eq. (B-8) will converge to a vector that is orthogonal to the m selected
 interferents.  An alternative method of computation is therefore available. The choice
 of methods will depend on the particular problem at hand.  For example, if the noise
 is uniform and uncorrelated,  then eq.  (B-16) applies which only involves the inversion
 of an m x m matrix as opposed to the n x n Inversion required in eq. (B-8).  On the other
 hand, for correlated noise, the  alternative method may be preferable.

    Multiple Weights

      In  some applications, several linearly independent targets can be present
 simultaneously.  If it is desired to measure or detect each target independently,
 then the  linear weight for each target is required to be orthogonal to the other
 targets,  i.e. ,
      In matrix notation, eq. (B-17) becomes
                W'A = I                                                   (B-ls)
where W = (W , W ..... W  )  and A = (A , A  ..... A  ) are n x m matrices whose
             L    £.        m     ~   ~ L   £       m
whose columns are the W. and A. vectors respectively.
      The optimum constrained weight matrix is given by
and the SNR for each target is given by
                 d      -1/2
                                                                          (B-20)
                                     B-8

-------
where the r..'s are diagonal elements of the matrix
           u
It is noted that R is the cross response matrix in the absence of orthogonality
constraints.

                                                         r  -1*    u
      For m = 1, eq.(B-19) reduces to the usual form W^ = at)_    A^ where a \s a
scalar constant.  On the other hand, if the number of targets is equal to the dimension-
ality of the space, i.e., m = n, then
                                                                        (B-22)
              W' = A
      For the special case when the noise is uniform and uncorrelated,  i.e. ,
       2
  £ =cr  I, eq. (B-19) reduces to
                         -1                                              (B-2.1)
              W - A(A'A)

 This expression is the well-known "generalized inverse" of the matrix A and W'Y
 is the "least squares"  solution to the over deter mined system of equations AX^Y.

     Application

      For the present problem, the number of targets is m  = 3.   Since neutral
 attenuation is a dominant  interference  and is not very statistically well-behaved
 or modeled, the  weights will be orthorgonally constrained to reject this interfered,
 i.e.,
                W  + W  + W  + W  = 0
                  J_     Lt    O     *
                                                                          (B-24)
 for each target.  This will be indirectly accomplished by considering neutral
 attenuation as a 4th "target" in the formulation of equations (B-17) through (B-21).
 All other interferents will (by necessity in this case, since we only have 4 wavelengths)
 be considered to be "well behaved" and will be described by the noise  covariance
 matrix.  At least one such interferent, HO vapor will be included in this set.
                                        Lt
                                         B-9

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                                APPENDIX C
   WAVELENGTH SELECTION

   Introduction

     A large number of spectral lines are typically available using the CO^ laser.
However, practical  considerations limit the number of lines used to about 4 to 8.
A selection of the best subset of available lines is based on maximizing the signal to-
noise-ratio (SNR) for a specified set of targets and interferents.
                                   •lo  1C
     For the present 4 wavelength C  O    laser system, there are about 74 possible
                                      £4
lines from which to select.  A direct combinatorial approach to selecting the best 4
                                               74
wavelengths out  of the available 74 would require (4 )  = 1, 150,626 combinations; an
exceedingly large number of computations.  Each SNR computation involves an express-
ion of the form of (B-21).  This eolation Involves the construction  and inversion of a 4 X
4 matrix, 20  multiplications, and 20 adds to determine the SNR for ozone alone - the
target  we are optimizing.  Consequently, even if each computation  were  on the order
of one  cent,  the  required total cost would be prohibitive.

      Fortunately, a viable and expedient alternative exists that  can at least narrow
down the number of wavelengths to be considered to a manageable number.  As a bonus,
the method can also determine the increase in performance that  could be attained if
                                        C-l

-------
more than 4 wavelengths were used.  This technique was developed (Reference 1)


as an outgrowth of Reference Sand is referred to as the "squeeze method" of wave-


length selection.




    Squeeze Method
      For a scanning system, the noise  O" . associated with a measurement at each


wavelength \  . is indirectly proportional to the time T. spent at that wavelength:




                     O       O /                                          /f~>  1 \
                  rr  \   - v   /rr                                         (^-l)
                  Ol   - K.   1.
                           l    L



where K. is a constant determined by the system noise sources.  For a fixed scan


rate,  the sum  of the time intervals is fixed, i.e. ,




                       T  + T  + ... +  T = T.                               "^
                        1   2         n



      Assuming uncorrelated noise, the  variance of a weighted sum of measurements


is given by


                             n


                    0-  2=   Vffi 2 |W 1 2                                (C-3)
                            /         i


                            i  = 1

where W. is the weight attached to the measurement at  A  ..


By using a  variational argument, (Reference 3,  Appendix E) it can be shown that the


time intervals that minimize (C-3) subject to the constraint (C-2) are given by

                                         n

                                      /«
                       T  - TK
                        i     i
                                       i

                                       j =  1
                                    C-2

-------
i.e.,  the optimum time intervals are proportional to the product of the noise

constant and the absolute value of the weight.  Substituting (C-4) into (C-l)

                                  n
                   _  2      K     TII
glves              CT<   =    i     \K.  |W|,                           (C_rj)
TJW. | L_ ]
and determines the system noise component of the noise covariance matrix used

in computing the optimum linear weights.



      In Appendix  B, procedures were developed for selecting optimum weights.

These procedures were dependent on the noise covariance matrix.  If the optimum
time intervals are selected according to Eq. (35) , then the covariance matrix is

of the form
where D is a diagonal matrix, representing system noise,  whose elements are given

by (C-5) and is a function of W,  and .A. represents the noise due to other interferents.   Since D

and hence T. are themselves functions of W, the solution of W is in implicit form.  An

iteration procedure is therefore indicated.  An initial guess of the solution, say WQ' =

(1, 1 ..... 1) , is substituted into Eq. (C-6) and the optimum weighting vector W1 is

calculated by one of the techniques given in Appendix B.  For the next iteration, J^

is substituted into eq.  (C-6) and W  is calculated.  In this  manner, a sequence of weights
                                 u
will be determined which will converge to the desired optimum weight.
                                          C-3

-------
       A consequence of this procedure is that weights corresponding to wavelengths
  of low information will  converge to zero and the required wavelength seleetion process
  is thereby attained.  In general, m + p wavelengths will be retained in the limit,
  where p is the number of independent agents to be detected and m is the number of
  intcrferents (assuming  n > m <- p).

       If several  targets are to be simultaneously optimized, a suitable averaged
  weight can be  used in the feedback loop.

       A computer program (LWSP) was developed for implementing the above
 procedure (Reference 1) and is described in Appendix D.  It assumes a detector-
 noise-limited  system so that K. = NEP/P. where NEP is the noise-eqmvalent-power  '
 of the detector and P. is the received power at A   ..  The program is restricted to
 computing weights by (B-ll) and (B-12) with a diagonal  covarlance  matrix, i.e.,  it
 assumes that enough wavelengths are available so that all interferents can be com-
 pletely rejected and that all system noise is uncorrelated.

 Application

       In order to use the LWSP program for the present application,  ozone was
 considered as a single target and all other gases were considered as interferents.
 In addition, the present application was expected to be optical-noise-limited rather
 than detector-noise-limited and so, the P.'s were all set equal except for those
 that are so low as to preclude reliable operation.  In this manner, the 74 available
 lines were  reduced to a  set of 10 from which a final selection was based.
       The final selection uses another program (CMFIL) in order to compute the
performance of all ( 4 ) = 210 combinations of wavelengths using equations (B-20)
and (B-21).  This program was adapted from another existing program (MFIL).
                                   C-4

-------
LWSP
         A description of the LWSP program which implements the "Squeeze Method"
as previously noted is given in Appendix D.  This program essentially eliminates
wavelengths of low information by an iteration process of adjusting the power allocation
according to an optimization algorithm.  In this manner, the power allocated  to un-
important wavelength coverages to zero thus accomplishing the selection process.
         The present configuration of the LWSP program operates in the orthogonal
mode, i. e.,  the linear weights are constrained to completely reject all of the gasses
in the prescribed interferent set.  In this mode of operation, the number of significant
wavelengths will converge to the sum of the number of linearly independent targets and
the number of linearly independent interferents.
       For the present application, the detection of one target, O ,  was considered
                                                              «J
in the presence of 5 interferents:  CO  , HO, C H  , NH , and neutral attenuation.
                                   Z   Lt    Z 4    o
With this target and interferent set,  the number of  significant wavelengths will then
converge to 6.
       A 25 iteration LWSP run with the above target and interferent set resulted in
the line selection illustrated  in Figure 14.  The solid lines in this figure represent
the linear weights  applied to each wavelength and their length is indicative of  the
relative importance of each line.  The X's designate normalized ozone absorption
coefficients and the +'s designate the average interferent noise level.  As can be seen,
the number of significant wavelengths converged to 6 as advertised.
CMFIL
       A four-wavelength system was selected on the basis of compromising per-
formance and complexity.  This choice  is later justified as explained in the introduction
and illustrated by Figure 16.  In this  case, the number of wavelengths used is not
                                        C-5

-------
 sufficient to null out all of the interferents.  Therefore, the strength (variance) of '
 each inh'rfoivnt must be estimated and :i linear weight is computed Hint gives llu-
 best performance on  UK- average.  The di-tails of this nu-Uuxl ;nv di-si-rUn-d in
 Appendix B. A program (MFIL) that computes the  linear weights and
 SNR's for a given set of wavelengths using this algorithm is described in Reference
 17.  This program was modified (CMFIL) in order to evaluate all combinations of
 N wavelengths  taken M at a time and to order the combination according to SNR.
        Table V shows the input data that was used for the CMFIL program.  The
 wavelength  set was obtained from the top 9 wavelengths of "the LWSP output combined
 with the ethylene line.  The interferent CL variances listed in Table I were estimated
 from the best guesses available of the environment.  The CMFIL output listing that
 was obtained with the input data of Table V and the  spectral data  in Tables I and II
 is shown in  Figure 15.  As expected, the P12 and P14 (5 and 6) which correspond
 to the peak  ozone absorption, appear in all of the highest rankings.  The RIG, R14,
 and  P24 (3,  4,  8) lines also predominately appear in all of the highest rankings and
 are therefore indicated as good  reference lines.  The combination 4,  (5,  8,  10 (R14,
 P14,  P24, P14) was selected as the  combination that gave the highest SNR while
 retaining the ethylene line.
       By examining the linear weights associated with the output listing, the
performance of 2 and 3 wavelength systems was estimated and is shown in
Figure 16.  As can be seen, a three-wavelength system (which we essentially
have at the present due to the retention of the 10. 5321 micron  ethylene line)
provides near optimum performance with a minimum  of complexity. A  two-
wavelength ozone system results in about 1/2 the sensitivity.
                                     C-6

-------
             WAVELENGTH SET
O
i
001-020








001-100
TARGETS (RECORD
R30
R18
R16
R14
P12
P14
P20
P24
P30
P14
NO.)
9.219690 microns
9.282444
9.293786
9.305386
9.488354
9.503937
9.552428
9.586227
9.639166
10.532080

    Ozone 03 (244)




INTERFERENTS (RECORD NO.)




    Neutral (201)




    Carbon Dioxide CO2 (243)




    Ethylene C2H4 (245)




    Ammonia  NHg (246)




    Water Vapor HjO (244)




DETECTOR NOISE VARIANCE
                   10
                     -5
 VARIANCE (CL)   COMMENTS




 1.0             If T log-normal, 4:1 variation 50% of time




10cO             10% x 320 ppm x 1 km




 25 x 10'6        50 ppb x 1 km




 25 x 10"6        50 ppb x 1 km




 )06             -^58 - 100% RH at 73 degrees F x 1 km
                                                   Table C-l.  CMFIL Input Data

-------
                               APPENDIX D


         LWSP - LASER WAVELENGTH SELECTION PROGRAM
PURPOSE
      To select those laser lines from the CO laser bands which arc best for
                                          £

etection of agents in the presence of noise.
GIVEN
      a.  Spectra of-C12O l6 laser,  including relative power at each wavelength
                        Lt

      b.  Spectra of agents and interferents.


      c.  Relative importance of each agent.
COMPUTE
      The weight which should be applied to each line for optimum S/N and the time


fraction (power) to be allocated to each line.
 DATA FORMAT
      Same as MFIL (Reference 17).  Laser data can be input by either cards or

tape.  Individual and combined spectra are in the library.
                                      D-l

-------
 PROGRAM OPERATION





      Deck setup and operation are almost identical to that for MFIL.  Fewer


cards are required and a laser must be specified, along with the usual targot


and interferent list.




      There are two modes of operation.  One  uses independent wavelengths  for


each target and optimizes the weights for each individually.  The second me!,h">d


uses a common set of wavelengths and involves the use of an average weight  in the:


iteration loop which causes the weights for each target to move  move nearly  together.


If this option is chosen, the relative importance of each target is specifier! by use


of the "AVG" card.





      Five iterations will be made unless otherwise  specified on the "G" card. If


cards are used for laser data, they  must contain wavelength and power,  in th;it or.hr,


in (7X2F8.4) format.  A blank card  (wavelength = 0) terminates reading of the laser


data.  These cards must immediately follow the "LASER/CARD" command.



                   COMMAND LIST FOR LWSP
 COMMAND  TYPE    XI      X2     X:3      X4
                                         X5
 LASER


 LASE R


 TRGTS


 IFNTS


 NEVT


 AVG


 RESET


 G0


 END
          Li b. Scan No


CARD     (Follow by  A, pin (7X2F8.4) format, term,  with blank t-irclj
       '   Same as MFIL  (Reference 17)
w      w
  -L      £
                                w.
(ZER0)   K-plot  K-A/N K-iter  NDP
W
                                     D-2

-------
MATHEMATICAL METHOD
 1.  Construct Interferent Matrix
                   QMIj,  I2 ..... 1tt)            (n x m)                 (D-])




where the columns are n- dimensional interferent absorption coefficient vectors, n


is the number of wavelengths available, and m < n is the number of interferents.




2. Initialize Average Weight and Weight for Each Target




               (0)     (0) =
              W    =W.

                              lt P2 ..... Pn)'  , i = l, 2 ..... p           (D-2)
                                                                      .1.
where p is the number of targets and P. is the relative power at wavelength j




3.  Compute the Diagonal Matrix, Scale Factors,  and Time Intervals




for each iteration k=0, 1, 2,..., Kas follows:




      a.  Independent Wavelengths


Compute the diagonal matrix
                                 v..           (n x m)
                  1      J     j •   0    •



and scale factor
                                     D-3

-------
                        0


                     -  Y  |W

                        L    i

                      J   1
for each target i = 1, 2	p where W. (k) = (W , (k),  W „  (kl	W    (k))'
                                    ~ i        il       i2             in


       th
is the k   iteration weight vector for target i.  Also,  compute the time fraction


(power) allocated to  wavelength j




                  T    I  /P  F  "<>
                    U       '   U.  •   '    j  >.
for each target i = 1, 2,  ... , p.
      b.  Common Wavelengths
      Compute the diagonal  matrix
D(k) - dia   P. W. (k)
                     diag (P. W.   )
      and scale factor

                                n
                               y
                               f—
     Fx
                      .1        3
     where W    = (W ,  W	W )' is the kl iteration average weight.
            —         i    £         n                                •
                                     D-4

-------
      In this case,  it is only necessary to perform the computation once for each


 iteration.  The common time fraction allocated to wavelength j is computed as





                 T (k)  =  w  (k)   /P F .                               (D-S)

                   J         J         J  j




 4.  Compute Next Weight Vecto-r
                 W.      . D.
 for each target absorption coefficient vector A. , i -  1, 2 ..... p.  (In the common


 mode, D. is replaced by D in the above).





 5.  Compute Relative Signal -To -Noise Ratios





                SNR  =(W'(ktl)A /F) 1/2                             <
                   i   ~i        -i    i




for each target i.  (Again, in the common mode, F. is replaced by F in the above)





C.  Normalize Each Weight to an Absolute Peak of ].





7.  F>rint Weights. SNR's. and Time Fractions for each Target
                                    D-5

-------
 -~- Cotviputo Average Weight

                                    P
                     w(k '  n  -     r-        K.|W. (k '  1}|                 (

                                  i  ---- 1


 where the K.'s are weighting factors corresponding to the relative importance of
 each target.


 i>.  Print _Sum ma ry_and_ Comp u te_Next__Ite_rati_on


 Go to Step 3 and repeat until k - K.


 10.  Compute Target Cross-Response Matrix R (p x p)


 with elements
                  R  - GW (K)A    L i  -  1  2
                  lx^j    [-J   - i'   »J    i> Z
where


                  Gr SNRi ("7V"V  "I-2	f

JLL-_C^mjgjjte Interfercnt Cross-Response Matrix U (p^ xjlll_

with elements


                                     j = 1, 2, ... , m

12.  Compute Next Iteration (Go to Step 3)

A flow chart describing these operations is shown in Figure D-l.

                                     D-G

-------
Step
Loop
                        Input Data

                            *
                            (i)
                   Read Wavelengths, Powers,
                      Targets, Interferents
                            (2)
                      Initialize Weights
                           (3)
                 Compute Diagonal Matrix,
                Scale Factors,  Time Intervals
                                     Mode
                                     Switch
         (4)
Compute Next Weight
                                             Common
         (5)
    Compute SNR
                           (6)
                     Normalize Weights
                           i
                          (7)
            Print Weights, SNR's, Time Fractions
                          (8)
                 Compute Average Weight
                         (9)
                     Print Summary
                       (10, II)
                 Compute Cross-Responses
               Print Absorption Coefficients,
                     Cross-Responses
                      Stop;  End
                                                              Independent
Target
Loop
                                                              Plots
    Figure D-l.   FLOW CHART OF  LWSP PROGRAM
                                D-7

-------
                                      TECHNICAL REPORT DATA
                              (Please read fnuruftions on the reverse before completing)
 I. REPORT NO.
  EPA-650/2-74-046-a
 A. Tl VLE AND SUBTITLE
  Development of a Gas Laser System to Measure Trace Gases
  by Long  Path Absorption Techniques, Vol.  I:  Gas Laser
  System Modifications for Ozone Monitoring	
  . AljT
      HOR(S)
                                                                8. PERFORMING ORGANIZATION REPORT NO.
  S.E. Craig,  D.R. Morgan, D. L. Roberts,  L.R. Snowman
 9. PERFORMING ORGANIZATION NAME AND ADDRESS
  General Electric Company, Ordnance Systems,
  Electronic Systems Division, 100 Plastics Avenue, Pittsfield,
  Mass.. 01201	
 12. SPONSORING AGENCY NAME AND ADDRESS

  U.S. Environmental Protection Agency
  National  Environmental  Research Center
  Research Triangle Park,  North Carolina, 27711
              3. RECIPIENT'S ACCESSION-NO.
               5. REPORT DATE
                    June  1974
              6. PERFORMING ORGANIZATION CODE
                    OS 74-13
                                                                10. PROGRAM ELEMENT NO.
                                                                     1A1010 (26ACX)
               11. CONTRACT/GRANT NO.
                   68-02-0757
               13. TYPE OF REPORT AND PEHIOD COVLRtO
                   Final
               14. SPONSORING AGENCY CODE
 15. SUPPLEMENTARY NOTES
  Volume II of the set is being published as  EPA-650/2-74-046-b
 16. ABSTRACT            '•                            ~~~~	
                 Modifications of a gas laser system for long path monitoring of trace atmospheric
     constituents by infrared absorption are described.   Modifications were made in preparation for
     an ozone field measurement program reported in Volume II wherein path monitor data were
     compared with those from a  point monitor moved along the optical path.  System modifications
     included incorporating a digital signal processor in the system  and a spatial filter in the laser
     beam.  Spectral studies of ozone,  carbon dioxide, water vapor, ethylene and ammonia are
     presented in connection with the selection of laser wavelengths used in the system to discrimi-
     nate ozone effects from interferences.  Design considerations and a proposed configuration
     for an isotopic C©2  laser are presented.
 7.
                                  KEY WORDS AND DOCUMENT ANALYSIS
                   DESCRIPTORS
  Lasers
  Atmospheric Absorption
  Ozone
  Air Pollution Monitoring
 3. DISTRIBUTION STATEMENT
  Release Unlimited - Copies Available from
  NTIS; APTIC (EPA)
                                                 1). IDENTIFIERS/OPEN ENDED TERMS  K.  COSATi i-'icld/din
   I LAMS
   Methodology for Point
   Monitor,  Path Monitor
   Comparisons
                                                 VJ. SECURITY CLASS (This Krptirl>
                                                       Unclassified
       1705
20. SECURITY CLASS (This page)
      Unclassified
I 21. NO. Oi- f'AGES
	123	
 22*. PRICE
EPA Form 2220-1 (9-73)
                                               D-8

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