EPA-650/2-74-034
June 1974
                           Environmental  Protection Technology Series

                                                               • » • • • • • «

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                                  EPA-650/2-74-034
   OPTICAL MEASUREMENTS
   OF  SMOKE PARTICLE  SIZE
GENERATED  BY  ELECTRIC ARCS
                   by
                P. W. Chan
           Colorado State University
           Fort Collins, Colorado 80521
             Grant No. R-800150
             ROAP No. 21ADL-21
          Program Element No. 1AB012
        EPA Project Officer: D. C. Drehmel
           Control Systems Laboratory
       National Environmental Research Center
        Research Triangle Park, N. C. 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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                                ABSTRACT





     Light extinction and photometric scattering measurements employing



laser sources have been used for sizing polydispersed metallic particulate



systems of unknown index of refraction.  Two time-averaged intensity ratio



measurements including (i) intensity ratio at two angles and (ii) polari-



zation ratio at one angle, were carried out at several small forward-



scattering angles so that the measured values are essentially independent



of the index of refraction.  Results were presented for smoke generated



by electric arc discharges between carbon, copper, aluminum and tungsten



electrodes.  In the two-angle ratio method, the average size is obtained



by using the theory of Hodkinson.  In the polarization method which is



more suitable for sub-micron particles, the experimental curve of polar-



ization ratio at several scattering angles is fitted by a theoretical



best fit using a logarithmic normal size distribution similar to that



used by Kerker et al., from which the modal value of the radius and the



logarithmic deviations are obtained.  The optical system was calibrated



with standard latex spheres.  The fit was found to be rather good for the



arc smokes (polydisperse systems) and good for latex (monodisperse)



spheres.  The light scattering results agree with those obtained by light



extinction method.  Combination of the two schemes in one instrument may



provide a device for sizing polydisperse particulate systems from .Olyia



to lOym in diameter, independent of refractive index.  The possibility



of measuring size distribution in real-time using instantaneous measure-



ments based on the above schemes, similar to that used by Gravatt, are



considered.  With some improvements, the device will be able to size


                            7                                  3
particulate systems up to 10 /cc or higher at a flow rate of 10  cm/sec



using commercially available electronics.  The same device will also



count the number density to determine the particle concentration.




                                  iii

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                            ACKNOWLEDGEMENTS








     The technical assistance of Mr. Opas Apichatanon in the laboratory




throughout the course of investigation is greatly appreciated.  Discus-




sions with Dr. C. Y. She of the Physics Department, Colorado State




University and with Drs. D. C. Drehmel, J. Abbott and W. Kuykendal of




the National Environmental Research Laboratory, Research Triangle Park




are most helpful.




     This work is supported by a grant sponsored by the U. S. Environ-




mental Protection Agency.
                                   IV

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                                  CONTENTS

                                                             Page
  Abstract .......................... iii

  Acknowledgements  ....................  iv

  List of Figures  ...................... vi

  List of Tables   ...................... vi

  Sections


   I   Conclusions ......................  1

  II   Recommendations ....................  2

 III   Introduction  .....................  3

  IV   Theoretical Background  - .Mie  Scattering Theory
       and Applications ....................  5

   V   Optical Instrumentations  for  Particle
       Size Measurements ................... 14
  VI   Experimental Methods,  Results  and Analysis   ...... 19

 VII   Instantaneous Forward  Scattering Methods   ....... 32

VIII   Discussion  ...................... 39

  IX   References  ...................... 41

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                                 FIGURES


No.                                                            Page

1.     Light  Scattering  Geometry 	   6

2.     Essentials  of  Extinction (Transmission)
       Measurements   	  15

3.     Optical  System for  Scattering Measurements	17

4.     Experimental Set-up for  Observation of
       Scattered and  Transmitted Light  	  18

5.     Theoretical Curve of E(m,a)  for DOP Smoke (m = 1.486)  .  21

6.     Experimental Results of  Three-wavelength
       Transmission Measurements 	  22

7.     Variation of Intensity Ratios versus Size Parameter
       a According to Fraunhofer Diffraction 	  26

8.     Viewing  Particles in a Flowing System 	  37

9.     A Proposed  Real-time Device  for  the Determination
       of Particle Size  Distribution	38
                                  TABLES


 No.                                                          Page

 I.    Theoretical Scattering Intensity - ratios 	 13

 II a. Three Wavelength Transmission Measurements
       of DOP Smokes	20

    b. Analysis of Three Wavelength Transmission
       Measurements of DOP Smokes	23

III    Average Particle Size of Smokes Particles as Measured
       by the Two-Angle Ratio Method 	 27

 IV    Summary of Experimental Results of Parameters of Arc
       Smokers as Measured by the Two-Angle Ratio Method and
       by the Polarization Method	31
                                    Vl

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I.  Conclusions



     Two main conclusions can be drawn as a result of Che present inves-



tigation dealing with optical methods for measuring sub-micron polydispersed



smoke systems of unknown refractive indices:



(i)  The two-angle ratio forward scattering technique has been found to



be a reliable and accurate method for obtaining average sizes of several



smoke systems generated by an electric arc between carbon, copper, aluminum



and tungsten electrodes.  The results can almost be obtained in real-time



by comparing experimental results with available universal graphs of



Hodkinson.  However, in order to obtain particle size distribution (i.e.



mean radius as well as standard deviation) for sub-micron particulate




systems, the inversion procedure is rather lengthy and inaccurate since



the two-angle intensity ratio is insensitive to particle size smaller



than 0.2 ym.



(ii)  The polarization ratio method appears to be a simpler amd more



practical method for obtaining size distribution of sub-micron polydisperse



smoke systems.  The tecnique involves in measuring the polarization ratio



of the scattered light at several scattering angles and fitting the



experimental data with the best theoretical fit.  For monodisperse latex



particles, the fit is extremely good.  However for polydispersed systems



the fit is only fair.  Performing the measurements of polarization ratio



in small forward scattering angles also renders the technique to be



applicable to particulate systems with unknown refractive indices.



(iii)  In addition, theoretical calculations indicate that these techniques



have great potentials in real-time applications for sizing sub-micron poly-


                                                    7                    3
dispersed particulate systems with concentrations 10 /cc and flow rate 10



cm/sec with megahertz electronics, the number concentration that can be handled



increases with the bandpass of electronics and decreases with flow rate.

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II.  Recommendations



     The results of this investigation establish the feasibility of a



practical technique for measurement of size distributions of polydis-



persed, absorptive particulate systems of unknown index of refraction



throughout the range of particle size ranging from O.Olym to several



microns.



     The next phase of this investigation will be to extend the present



time-average measurements to instantaneous intensity-ratio and polari-



zation measurements.



     Theoretical estimates (Section VII) show that with commercially



available fast electronics, these techniques can be used to monitor



smoke size in real-time for particulate systems with concentrations up


     7                                 3
to 10  particles/cc at flow rates of 10  cm/sec, typical for many smoke



stack and effluents from power plants.  Thus it is strongly recommended



that a self-contained unit suitable for field operation be built for



measuring particulate size distribution of fine particles.

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III.  Introduction




     Many optical methods exist for measuring particle size (average),




size distribution, concentration and shape.  Broadly speaking they




can be classified as light transmission (extinction) measurements,




photometric (multi-particle) scattering measurements and single part-




icle scattering (counting) measurements.  Except under special laboratory




controlled conditions where particles under study are sufficiently mono-



dispersed and the flow is non-turbulent, very few satisfactory methods



have been found to size particles in the size range of .Olum to several




microns.  Since particles of this size range are of utmost concern to




air pollution control and public health, development of accurate, real-




time methods to monitor particulate size and concentration in this size




range are of urgent importance for legislating environmental standards




for air pollution control.  Indeed, accurate characterization of particle




size, distribution and concentration is important for developing tech-




niques for conglomeration of fine particles.  This report describes sev-




eral optical particle sizing techniques suitable for in situ measurements




and remote sensing for micron and sub-micron particles generated by an




electric arc, which are highly dispersive systems similar to those en-




countered in smoke stacks and power plants.  The advantages and limita-




tions of each of the methods will be discussed.  It should be noted that




since the goal of the investigation is to result in a real-time particle




in situ instrument for particulate monitoring, the emphasis of the in-




vestigations are on the reliability of the Instrumentation and in the




simplicity of extracting information from experimental data.




      Reliable and rugged lasers  such as the He-Ne or Argon ion lasers




 are used  for the light source which, because of the monochromaticity, also

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greatly increases the signal to ambient noise if narrow -interference filter




is used in the detector system.  In Section IV, the Mie scattering theory




which forms the theoretical background of the experimental methods used




in this investigation is discussed.  Section V describes the optical and




electronic instrumentation for both transmission and scattering measure-




ments.  Section VI describes experiments on transmission methods from




which particle concentration and average size is obtained as well as two




scattering methods:  one based on measuring the scattered ratio of inten-




sities measured at two forward scattering angles, and the other based on




measuring the polariziatlon artio at a particular angle, (measured at




several scattering angles) from which the average size as well as the




size distribution are obtained.  The possibilities and capabilities of




real-time devices based on these optical techniques are analyzed in detail




in Section VII.  A summary of the present investigation as well as some



suggestions for future work in developing the techniques to a real-time




system for air pollution is presented in the discussion in Section VIII.




Detailed literature references are given in Section IX.

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IV.  Theoretical Background - Mie Scattering Theory and Applications

     The Mie equations provide a general description of light scattered

by uniform spherical particles illuminated by a plane wavefront.  The

results can be expressed in terms of the following parameters:

m = relative index of refraction of particles to the background medium,

    can be a complex quantity if the particle is absorptive:  m - m1 - im"

A = wavelength of incident radiation

r = radius of spherical particles

a = 2irr/A = ird/A = size parameter
                                          o
I  = irradiance of incident light (Watts/m )

6 = scattering angle (defined with respect to forward direction)

Plane of observation - plane containing the direction of propagation

     of incident wave (k ) and the direction of observation  (k. ) .

Plane of Polarization - plane containing the direction of propagation

     of incident wave (k ) and the direction of its electric field  in

     linearly polarized incident beam  (E).

 = angle between the plane of observation and polarization  (see Fig. 1)

     For a linearly polarized incident beam, a scattered irradiance I
                                                                     s
        2                                                           1
(Watts/m ) at a distance  R  from the  scattering center is given by

                    A2I
     I  {a,m,6,<|>} = - —  (i-{a,m,0}  sin 2 + i, {a,m,6}  cos2)     (1)
      S             4ir2R2    i                  2
and for an unpolarized incident beam,

                     \2I
     I  {a,m,9,<|>} = - —   (i..{a,m,e} + i   {a,m,9»   =   I, + I-       (2)
      S             8ir2R2    *           2                X     2

The scattered intensity function i, is proportional  to  the scattered

light perpendicular to the  plane of observation and  i~  is proportional

to the scattered light parallel to the plane of observation.   The functions

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                                                             Plane  of  Polarization
            Plane of
            Observation
Fig. 1.    Scattering geometry shewing the incident wave vector  k  ,  scattered  wa_ve vector kj,
           electric field vector E of a linearly polarized  incident  wave,  (k , E)  is the plane
           of polarization and (lc  k^) is the plane of observation.   $  is  the*  angle between the
           planes of polarization and observation,     (fl =  90° is  a  common scattering geometry).
           6 is the scattering angle between k^  and kj  , 9  =0 define the forward direction
           of the beam.

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i..(a,m,0) and i~(a,m,9) each have the form of an infinite series of half


                                                2

order Bessel functions and Legendre polynomials.   In addition, express-



ions for light scattering for non-spherical particles have been worked



out in simple cases such as cylinder, disks and ellipsoids.  Light scat-



tering from irregular shape particles such as fragments of coal and


                                    3 4
quartz has been studied by Hodkinson '  experimentally and the same gross



light scattering characteristics similar to those of spherical particles



are found, except for some fine structures.  Thus, Mie scattering can be



applied to non-spherical particles for obtaining information on size



distribution and concentration or number density.



     Simplified theoretical solutions exist for very small particles,



particles with relative index close to one, and for large particles.


                                                          2 i  2

For example, for small particles (a«l,ma«l), i. = a6 ( T~O )  and
                                                L        m —/


i. = i. cos29.  For large particles (a»l), all but the finest details



can be described by an incoherent superposition of expressions for



diffraction, refraction, reflection and absorption.   This is particular-



ly useful for o»50 since in this case the series contained in the Mie



equations converge slowly and Involve small differences of large terms,



requiring relatively lengthy computer calculations for precision.



     For the size range from O.Olym - lOym employing visible light source



(0.4 - 0.7ym) no simplified solutions exist for the Mie equations although



computer calculations are fairly readily available.



     In real situations where the particles are highly polydispersed and



in some cases where the index of refraction is complex and not known, special



methods aiming at both simplicity and elegance and real-time practical



application are desirable.  Several techniques aiming at these goals are

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                             -8-
investigated, the theory of the methods, one based on transmission


or extinction measurement, and the other on two-angle forward scattering


ratio and polarization ratio measurements will now  be discussed.


A.  Light Transmission Method


     The method of light extinction or transmission measurement is useful


for obtaining average size.  It is based on the Bouguer or Lambert-Beer


law which relates the transmitted flux  f  and the incident flux  f


to the thickness  t of the suspension


         f = f exp ( -naEt)                                   (3)
              o

where  n  is the number density,  a  is the projected area of the


particle (against the beam), and E(ct,m) is the particle extinction


coefficient. For spherical particles of a diameter  d  and of known


refractive  index m  (relative to the  suspending medium), illuminated


in monochromatic light of wavelength X  in that medium, the variation


of  E  against the particle-size parameter  a = ird/X can be calculated


from the Mie theory.  For diotyl phthalate (DOP) n = 1.486, the  E


versus  a  curve has been calculated by R. B. Penndorf  and shows



the usual oscillatory features.  To make use of the theoreticel curve


for deriving the average particle size, the transmittances of a partic-


ulate suspension at three wavelengths Xp A , Ag  are measured and are


equal to (f/f0)lt (f/fo)2» and  (f/fo)3 respectively.  From Bouger's


Law  E   : E2  : E3 = ln(f/fQ)   : ln(f/fQ)2  : ln(f/fQ)3 and the ratios


existing between the corresponding particle-size parameters are



      cij^c^a-j =  Xj^   :^2~  :^3  .


To derive an estimate of particle-size, the theoretical curve of  E


versus  a   is plotted on a  log-log graph paper.  On a second, identical

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                            -9-





 sheet of  graph paper  are plotted  the points




       [ln(f/fo)1/ln(f/fo)l = 1, 1r/X1]




       [In(f/f0)2/ln(f/fo)1    § */X2]




       [In(f/f0)3/ln(f/f0)1    f Ti/X3].



 The second sheet is then slid over the  first,  keeping the corresponding




 axes on both sheets parallel, until the plotted points best  fit the




 theoretical curve.   The correspondence  of the  logarithmic abscissae



 nd/X  and ir/X gives the value of   d; the value of   E  for any wavelength




 may be read also, and the particle number density  (n) can be derived




 from Bouguer Law.




   The results could be checked by a direct measurement of the mass




 concentration  c.  If p is the bulk density  of the particles, and  n




 the number density, then — irr3pn  = c and from Bouguer's Law




 D - log,Qf/f  = naEt/2.303  where a = irr2 for spherical particles.




 Hence c = 4prD(2.303)/3 tE and r  and n  may be  calculated.  It should be



 noted the mass concentration of smoke particles is difficult to be




 measured  accurately  for  particulate systems in real  situations.
B.  Light Scattering Methods




     In particle size analysis it is usually assumed that light is scat-




tered incoherently by the particles so that the scattered intensity is



proportional to the number density.  It is also assumed that the system




is so dilute that no neutral polarization effect or multiple scattering




occurs.  While mutual polarization effect occurs only when particles




are very close together (distance smaller than several particle diameters),



multiple scattering occurs quite commonly.  As a rule of thumb, trans-




mission should not be less than 90% to reduce the error due to multiple




scattering.

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                                   10
     The basic theory of forward light scattering is based on the fact,

                         g

first noted by Hodkinson,  that the angular distribution of the scattered



light within the forward lobe is primarily due to Fraunhoffer diffraction,



and as such, is independent of the index of refraction.  Since the forward



scattering arises from the light passing near the particle rather than



from rays undergoing reflection and refraction (which depends on the re-



fractive index), the scattering intensity function is given by





i (8, a) = i|(0,a) + ii, (9, a) = 2a  [J^ (a  sin 8) / sin26]
                    - 2a2 (J±2 (a 9) /02)                              (4)
The scatter flux (per unit angle per unit area) for small 6 is





          1(9, a) = — — 2a2  (J 2  (a 9)/92)

                               X
          = a2(J 2 (a 8)/92) where a E  -^  , a = a particle radius  (5)
                JL                         A




For a polydisperse system of spheres





          1(9) =  /  a2^2 ( / O2]




is a function of any set of small angles, 0, and 6_.  A set of
                                    Q

graphs is thus obtained by Hodkinson  from which a or  the  radius  of  the



particles can be calculated.  In order to obtain the size  distribution,



one can assume a size distribution  in Eq.  (6), or the  integral  can be

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                                   11
                                       9 10
inverted as done by Shifrin and Perlman *   to give the size distribution
as
                      OB
     p(o) = -(2/a2)  /  06.^(0 9) N^a 8) *(9) d6                    (8)
                     o
where
     *(e) =~         {I 2ym)
particles and narrow size distributions.  One of the limitations of the
two-angle ratio method is that it becomes rather insensitive for particles
with o < 1 (d<0.2ym).
     The polarization ratio method first proposed by Kerker et al.   is
more sensitive for submicron particles.  Based on Hie theory, for  a
monochromatically illuminated sphere which scatters incoherently,  the
two polarization components of scattered light are given by

                             p(a) da                                 (10)

          I||(8) =  c/ i|j(6) p(a) da                                (11)

The polarization ratio for each of the angles 6  is defined by

          p  (6)  4  Ijj  (6)  I ^(8)                               (12)

and is a function of the refractive index m (relative to the surrounding
medium),  a = 2ira/X, with  X=X /m where X  is the wavelength in vacuum.
                              o          o
The procedure here is to assume a size distribution.  A zero-order log-
arithmic distribution (ZOLD) is used and is defined by
                 (log a - log a^2          .
     p(a) = exp  	5^2	     (2ir)   OQ a^
where a  = log standard deviation
      «  = modal value of the radius.

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                                   12
                                                            12
For narrow distributions, the standard deviation a = a«  a .   The
                                                      M   o


theoretical curve is then fitted to experimental data.  Excellent agree-



ment has been obtained by E. Matijevic et al.    Note that the index of



refraction must be known and the method fails if a  > 0.3. (broad size
                                                  o —


distribution).  In order to apply the polarization method for submicron



particles, without knowing the index of refraction, a natural thing to



do is to perform the polarization ratio measurements at forward scat-


                                                             14
tering angles.  Using the values of Mie scattering functions,   Table 1



shows some value of ii(6) / i.i  (6).  One sees that this ratio does not



depend on the index of refraction especially for small angles.  Thus,



by combining the features of the forward scattering and the polarization



ratio method, a system could result to provide a practical method of



measuring size distribution of particles from .Olpm to lOum or larger.

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                              13
Table I.  Calculated Scattering Intensity-ratios for Different
          Size Parameter  a  and Refractive Index m.
*

CM
0
II
0

1)
2)
3)
4)
5)
6)

0
•
f-H
II
a


:D
:2>
:3)
:4)
:s)
[6)


0
•
CM
II
a

(i)
:2)
[3)
:4)
:s)
(6)


o
•
U1
II
a

CD
(2)
(3)
(4)
(5)
(6)

m = 1.05
1.0076
1.1324
1.0001
1.0234
1.0116
1.0468

1.0075
1.1312
1.0046
1.0277
1.0160
1.0649

1.0073
1.1267
1.0187
1.0415
1.0299
1.1247

1.0066
1.1115
1.1271
1.1496
1.1382
1.7083

m = 1.15
1.0076
1.1323
1.0001
1.0234
1.0116
1.0468

1.0074
1.1286
1.0046
1.0273
1.0158
1.0647

1.0063
1.1134
1.0196
1.0401
1.0297
1.1237

1.0046
1.0720
1.1379
1.1535
1.1456
1.7601

m = 1.30
1.0076
1.1321
1.0002
1.0233
1.0116
1.0467

1.0072
1.1234
1.0047
1.0267
1.0156
1.0634

1.0053
1.0895
1.0210
1.0374
1.0291
1.1213

1.0011
0.9996
1.1605
1.1635
1.1624
1.8746

Intensity-ratios :
(1)  1 (5-)/i|, (5°)
(2)
(3)
(4)
(5)
(6)
                                          iM(200)]

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                                  -14-
V.   Optical Instrumentations for Particle Size Measurements




         Optical  instrumentations  for both transmission and angular  scattering




     are  basically simple.   With  the  advent of  lasers  as well-collimated  light




     sources,  the  usual  condenser-pinhole-collimator combination  for  producing




     a  collimated  light  beam can  be eliminated   especially  if only  urn or  sub-




     micron  particles  are of interest.




     (A)  Consider  first  the  optical requirements for transmission measurements.




     It is clear that  from the definition  of transmission or extinction that




     its  requirement demands all  of the  undeviated  light, and virtually none




     of the  scattered  light, to reach the  measuring device.  This is  accom-




     plished in the simple apparatus  as  shown in Fig.  2.  Consider the case,




     if the  first  pin-hole can be assumed  as a  point aperture then  the only




     light reaching the  photocell,  besides the  transmitted  beam,  would be




     light scattered through angles less than the exact angle subtended at



     the  pole  of the collector lens by the radius of pin-hole  (2).  The




     scattered light is  concentrated  closer to  the  forward  direction, the




     greater the particle size, and with visible light (  X- 0.5 ym) a pin-



     hole is needed only for particles with  d>10pm.   It  is sufficient in




     practice  if the angle subtended  by  each pin-hole  at  its lens is  not




     more than one-tenth of  the angle of the first  angular  minimum  in the




     Fraunhofer diffraction  pattern of a disc equal to the  particle's pro-




     jected  area,  i.e.,  not  more  than 1/10 of 3.84/a radians.  For  example,




     if the  largest particle is 5 ym, the  pin-hole  angle  should be  limited




     to 0.7° and for a lens  of 10 cm, 1.2  mm pin-hole  would be small  enough.




     If the  largest particles are d = 1  urn, the angle  is  3.5° and the pin-




     hole would be 5 mm  in diameter.  Thus  for a He-Ne  laser of 1-2  mm diameter,



     apertures of  1mm  placed fin the beam  and in  front of the photodetector




     are  sufficient for  the  present experimental conditions where only

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                   Pin-hole I
                                                         Pin-hole 2
Light
Source
                                     Particles
Condenser
  Lens
Collimator
 Lens
Collector
  Lens
Photocell
                                                                                                       Ln
                                                                                                        I
      Fig.  2.   Essentials of Extinction (Transmission) Measurements

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                           -16-
partides of 0.01-2vim are of interest provided the detector is far away


(more than 10 cm) from the scattering centers.  For spectral rejection,


a narrow band interference filter (A       = 6328 A° = A,    ), should
                                    center              laser"

also be placed in front of the detector to reduce room light noise level.


(B)  Next consider light scattering requirements.  An idealized optical


system is shown in Fig. 3.  With reference to Fig. 3, the illuminated

           3
volume is W /sin6, the solid angle within which light is received is


wh/J,2 ster. and if there are n particles per unit volume of projected

        2
area irda /4, and 1(6) is the scattered intensity dejrined as _flux_scattered

                                                   nird 2           19
per unit solid angle per particle, then  fs(6)  -  —r-2-W3(sin 6 ) x whi  1(8).


Since all values in the formula are derived from measurements, the projected

                            2
area concentration C_ = nird  /4 is found if 1(6) is known from theory.
                    **      Si

In most light scattering sizing methods, only relative intensity measure-


ments are important.  From the above formula we see that, for angular


scattering measurements,   f (8)/ f (62) = (sin62/sin 8^ ' (I^O)/^^))


and f2(8)/f..(6) = I_(9)/I (9) = p(8) so that all but the obliquity factor


drops out when measurements involve only the reading of the photodetector.


The experimental set-up for both extinction and scattering measurements


for the present investigation is summarized as shown in Fig. 4.  The light


source is a low-power  (l-2mw) He-Ne laser.  The scattering cell is of


cylindrical geometry to permit angular scattering observation.  The


angular observation is carried out by rotating a rigid optical bench


located at the center of the scattering cell.  A polarizer at the collection

                                              -*•
optical arm selects either the perpendicular (E i plane of observation)


or the horizontal Intensity.  Aqueous solutions of latex spheres of known


size distribution and DOP smokes are used for checking the accuracy of


the experimental results.

-------
            Slit  h

          (_L to Paper)
Light
Source
                            Scattering
                            Chamber
Aperture =hxW
                                                                                   Photomultipiier
         Fig.  3.   Optical  System  for  Scattering Measurements.

-------
          •Interference   Filter

          •Slit   Aperture
                     'Rotatoble  Optical  Bench

                                •Cylindrical   Lens
        Pin-hole
        Aperture^*,
	L
Photomultiplier
Pin-hole
Aperture
                   He-Ne  Laser
                    (X0=6328 A)
                                                                                                      oo
                                                                                                      i
             Interference
             Filter
             (X0=6328 A)
                                                         Cylindrical   Smoke
                                                         Chamber  (Plexiglas)
  Fig.  4.   Experimental Set-up for Observation of Scattered and Transmitted Light
            from Smoke Particles Generated by an Electric Arc.

-------
                                   19
VI.  Experimental Methods, Results and Analysis

     This Section describes the experimental methods of transmission

measurement and angular scattering measurements for various kinds of

smoke particulate systems.  Results are presented for smokes generated

by carbon, copper, aluminum and tungsten arcs.  Standard latex spheres

and DOP smokes are used as calibration standards.


A.  Transmission Measurements of DOP Smoke Particulates

     DOP smoke is used as a calibration standard since the index of re-

fraction is well known, and the extinction coefficients E(a,m) are

available in the literature,  and is reproduced here in Fig. 5.  The

apparatus was essentially the same as that given in Fig. 3 and Fig. 4 of

Section V.  Two schemes were used, one employing the measurement of the
                                                    o             o
transmission at three different wavelengths at 6328 A (red), 5460 A (green)
         o
and 4358 A (blue), and the other by measuring transmission at one wave-
             o
length (6328 A) as well as weighing the smoke.  In the transmission method,

the light sources used were a He-Ne laser which provides the red line at
          o
A  = 6328 A and a mercury arc lamp with a green (Corning 4-74) filter
                                                                 o
and blue (Corning 5-56) filter, providing the green line at 5460 A and
                      e
the blue line at 4258 A respectively.  In the case of the mercury arc

light source, the light was first passed through a pinhole, then con-

densed and collimated by a lens system.  Dioctyl phthalate (DOP) smoke

was dispersed in a clean smoke Plexiglas chamber for 15 seconds with the

fan on to ensure smoke homogeneity.  The initial (without smoke) and the

final (with smoke) readings of the photomultiplier tube (RCA 1 P22) were

taken for each of the three light sources used.

-------
                                   20
     Experimental Results and Analysis



     The experimental results are tabulated as follows:





Table Ha.—Three-Wavelength Transmission Measurements of OOP Smoke
Wavelength
Flux
(yA meter reading)
f
o
f

XL = 0.6328 y
500 yA
165 yA

X2 - 0.546 y
80 yA
30 yA •

*3 = 0.438 y
200 yA
80 yA
     The theoretical curve of E versus a for dioctyl phthalate smoke




(m = 1.486) is shown in Fig. 5.  On a second identical sheet of paper




were plotted the three points located at




                                         = 1,  4.9646]
                     / ln(f/fo)1 , ir
          [In(f/f0)2 /
                                            [0.8846,  5.7531]
          [ln(f/fo)3 / ln(f/fQ)1 , ir/X3] =  [0.827,  7.21]





as shown in Fig. 6.  A second sheet is then slid over the first with the




axes parallel until the plotted points best fit the theoretical curve.




From the best fit the extinction coefficient E can be found, d is then




read off from the graph and n can be calculated from Bonguer law.  The




results are summarized in Table lib.

-------
                                      21
      10
                            1	1   I  I I I  I	1	1	1   I  I  I  I  I
UJ
 
-------
 1.0
                                 22
 10
                                            I     I
O.I
                                  10
too
  Fig. 6.    Experimental Results of Three-Wavelength Transmission
            Measurements.

-------
                                   23
          Table lib.—Analysis of Three Wavelength Transmission
Wavelength
\x = .6328 u
X2 = .546 u
\3 = .438 p
o = ttd/X
3.8
4.4
5.4
d (ym)
.76 ± .06
.76 ± .06
.75 ± .06
E n = D(2.303 / aEt
4.0 3.3x10 particles/cc
3.4 3.5x10 particles/cc
3.2 3.6x10 particles/cc
     The accuracy of the measurements was about 10%.  Hence, the average


diameter of the particles is .76 ± .06  m, and the average number den-


sity is 3.47 ± 0.4 x 10  particles/cc; the values are quite consistent


for all the three wavelengths.  To check the accuracy of these figures,


we repeated the extinction measurement using the He-Ne laser light source,


and weighed the smoke by the usual practice of passing the smoke and


weighing the asbestos before and after.  Since the volume of the smoke

                                        3
chamber is known (18.35 x 25.4 x 33.4 cm ), the mass concentration C can


be calculated; it has already been shown that C - 47rrD(2.303) / 3tE where


p = 0.8692 gm/cc is the bulk density of the OOP smoke, where D is the


optical density, and t = 18.35 cm in our experiment.  From the value E


for the three wavelength extinction measurements, a mass concentration


C was obtained 9.33 mg/cc which agrees well with the direct measured


value.


     Although this transmission method is quite accurate, a knowledge of


the index of refraction is necessary.  The theoretical curve of E(m,a)


versus a is also needed for obtaining particle size.  It appears that


the technique has very limited potential for sizing highly polydispersed


arc smoke particles with absorptive and often unknown refractive index.

-------
                                   24
Thus, forward scattering methods which do not require a knowledge of




the refractive indices were carried out.  However the transmission tech-




nique gives a convenient method of checking the particle size against




values obtained by light scattering methods.  As a general rule, at




least in laboratory work, light transmission measurements should be




carried out in addition to light scattering measurements.  Transmission




data also can be used for monitoring the reproducibility of the smoke




system, and to ensure that smoke density is not too high as to create




multiple scattering, which could render light scattering measurements



inaccurate.




     Theoretically, one could obtain the size distribution n(r) from the




transmission measurement by Mellin's transformation.    However, except




in special cases where the particles are very large or very small or




have narrow size distributions, the inversion has been found to be highly



inaccurate especially for sub-micron particles.  Hence the inversion pro-



cedure of transmission method will not be pursued here.






B.  Angular Scattering Measurements




     The two-angle ratio and the polarization ration method, both meas-




ured at small scattering angles are used.  These methods are both inde-




pendent of the refractive indices because scattering is primarily due to




Fraunhofer Diffraction.




     1.  Two-Angle Intensity Ratio Method



     In this method the ratios of the scattered intensities at selected




pairs of angles are measured.  The intensity ratios vary with the par-




ticle size parameter a according to the Fraunhofer diffraction- formula




Eq.  (4).  The two main types of scattering geometries are the goniometer




set-up, and the axially symmetric anular set-up.   In the goniometer

-------
                                   25
set-up, a telescope is rotated around the scattering cell whereas in the




axially symmetric anular set-up, light is collected by an anulus ring




(lens with the center blocked) or fiber optics.  Because of the simplicity




of the goniometer set-up, this is employed in the present study.  The




photomultiplier is mounted on a rigid bar rotable around the center of




the scattering volume.  Accurate and reproducible angular scattering




geometry is achieved in this way.  The reproducibility of the smoke sys-




tem generated each time is checked by monotoring the transmitted light.




Although there are slight deviations, the reproducibility is good to 10%




provided the arc spacing and electrode surfaces are reset and repolished




each time.  DOP smoke is also used as a reference as its properties have




been measured by the transmission technique.




     Experimental Results and Analysis




     All the smokes (except those of DOP) are generated in an electric




arc for a specific time period and subsequently dispersed with a fan in




the smoke chamber for a specified period.  The experiment was run at




least two times to check the reliability of the method.  The results are




summarized in Table II for each smoke particulate system and the particle




size parameter is read from the theoretical curve as shown in Fig. 7 as




calculated by Hodkinson.




     The results of the DOP smokes with d = (.66 ± .06)  m agrees quite




well with the results obtained by the transmission method (d = 0.76 ±




.06) ym.  The results of the arc smokes are the average of two separate




runs and the agreements between runs are good.

-------
                              26
0)
x
   1.0


   0.9


   0.8


   0.7


   0.6
•o

-------
                                   27
     Table III—Two-Angle Forward Scattering Measurements of Latex, DOP,
                Carbon, Tungsten, Copper and Aluminum Arc Particles
Type of Smokes
or Particles
Latex
DOP
Carbon
Tungsten
Copper
Aluminum
2. Polarization
Average Particle Size Diameter of Particle
Parameter (a) (micron)
2.0
3.3
2.97
3.81
2.52
5.2
Ratio Method
0.34 ±
0.66 ±
0.60 ±
0.77 ±
0.51 ±
1.05 ±

.05
.06
.10
.16
.13
.10

     Essentially the same experimental arrangement as in the two-angle

forward scattering experiment was used with an additional polarizer

placed in front of the photomultiplier to select either the vertically

(Ij_(6)) or horizontally (I/;(9)) polarized components of the scattered

light.  The experiment was performed with standard latex spheres in

dilute aqueous solution for scattering angles from 10° to 40° at 2.5°

intervals.  Background light for each polarization is measured at each

angle and is subtracted from the total scattered light to obtain I//(9)

(horizontal polarization) and 1^(9) (vertical polarization).  The

polarization ratio p(8) defined as the ratio of the intensitied of the

horizontally polarized (I//(6)) to the vertically polarized components

of the light scattered at each angle was measured at several scattering

angles.  He-Ne laser (X  = .6328y) light source was used in the experi-

ment.  All particles investigated were assumed to follow a Zeroth Order

Logarithmic Distribution (ZOLD) function characterized by a modal value

-------
                                   28
of size parameter, CL. or cL., and a logarithmic standard deviation, o .



The computer program,   which compared the experimental values of p(6)



with theoretical values of p(9) X for m = 1.332 (index of refraction of


                                                                         12
latex relative to water) at X = 0.6328 ym or A      = .63/1.333 - .474 urn .
The values of OL. and a  will be the solutions which fit the data.  The



experiments and calculations were repeated with other smoke systems.



     We note, in applying this method, the index of refraction must be



known; and therefore, the method may not be suitable for complicated



polluted smoke particles.  However, polarization ratio measurements



limited to small scattering angles (6 < 40°) do not depend on the index



of refraction  (Fraunhofer approximation) and can thus be used under



conditions where the refractive index is not accurately known.  In



particular since p(6) is sensitive for small a (small particles), it



therefore complements the two-angle forward scattering scheme in extend-



ing the lower limit of particle size to the sub-micron range down to



0.01  ym.  The polarization ratios were measured at 2.5° intervals from



scattering angles of 10°-40° for the smoke particulates.  The computer



program was used to fit the experimental data.  The average particle



size and standard deviation are obtained from the best fit.




     Experimental Results and Analysis




      (i)  Latex Spheres



     The theoretical polarization ratio values  p(6) were computed by the



computer CDC 6400 for an extensive array of combinations of CL,, o , m



and 6; viz



          OL. = 0.50 to 2.400 in step of ActM = 0.10



          a  = 0.100 to 0.145 in step of Aa  = 0.005
           o                               o

-------
                                   29
                  9 - 10° to 40° in step of A8 - 2.5°



                  m = 1.322 = index., of refraction of latex relative to

                              water



The acceptable results are the best theoretical polarization which fit



with the experimental value at different scattering angles.



     The best ten fits for CL. and o  are values for which agreement was



obtained between the experimental and theoretical values of p(6) at 10



angles.  The final best solution of a  and  a  was selected from o  - o



values at different scattering angles for which the mean square deviation



between the experimental and theoretical p(0) values was a minimum [11].



The final best solution of modal a  in log-normal distribution is found



to be o^ = 2.400, and a  = .115.  The diameter is 0.36  ± .06 y and the



standard deviation .04 y.



     (ii)  Carbon Smokes



     The parameters were used in computation



                 CL^ = 4.000 to 5.900 in step of ACL^ = 0.10



                 o  =0.16 to 0.25 in step of Ao  = 0.01
                  o                             o


                  9 - 10° to 40° in step of A9 = 2.5°



                  m » 2.000 - 0.6600 i17



The best ten fits for OL^ and o  values are for which agreement was ob-



tained between the experimental and theoretical values of p(9) at ten



angles.  The final best solution is CL. = 4.00, o  = 0.16, diameter -



0.80 ± .10 y and the standard deviation 0.08 u.



     (iii)  Tungsten Arc Smokes



     The parameters were used in computation



                 OL^ - 4.000 to 5.900 in step of Aa  = 0.10



                 o  = 0.160 to 0.250 in step of Ao  = 0.01
                  o                               o

-------
                                   30
                 6 = 10° to 40° in step of A9 = 2.5°
                 m - 3.4000 - 2.7000 i at 6330 A 18
The best ten fits for a  and a  are values for which agreement was ob-
tained between the experimental and theoretical values of p(e) at ten
angles.  The final best solution is o^ = 4.00, a  = 0.169, diameter =
0.80 ± .08 u and the standard deviation 0.13 u.
     (iv)  Copper Arc Smokes
     The parameters were used in computation
                 o^ = 4.000 to 5.900 in step of Ao^ = 0.10
                 o  = 0.160 to 0.250 in step of Ac  = 0.01
                  o                               o
                  6 = 10° to 40° in step of  A9 = 2.5°
                  m = 0.5600 - 3.0100 i at 6330 A1
The best ten fits for OL. and o  are values for which agreement was ob-
tained between the experimental and theoretical values of p(0) at ten
angles.  The final best solution is oLj = 3.9, o  =  .250, diameter =
0.78  ±  .15 u and the standard deviation 0.19 p.
     (v)  Aluminum Arc Smokes
     The parameters were used in computation
                 c^ = 4.000 to 5.900 in step of A
-------
                                   31
Su/nmo'ur o

     The experimental results of the polarization ratio measurement are

summarized in Table IV together with those measured by the two-angle

ratio method for the five particulate systems investigated in this work.

     Table IV.—Summary of Experimental Results of Parameter of
                    Particles Generated by Electric Arcs
Smokes or
Particles
Latex
Carbon
Tungsten
Copper
Aluminum
Two- Angle Ratio
Methods (d) pm
0.34 ± 0.06
0.60 ± 0.10
0.77 ± 0.16
0.51 ± 0.13
1.05 ± 0.10
Polarization Ratio Method
d (ym)
0.36 ± .06
0.80 ± .10
0.80 ± .08
0.78 ± .15
1.18 ± .10
o
o
0.11
0.16
0.16
0.25
0.25
     It should be noted that the size of latex as measured by the two-

angle ratio method and by the polarization method agree well with each

other.  The theoretical fit of the experimental data (polarization

method) was very good in the case of latex but not as good for all other

arc smokes.  It is believed that the poor fit is due to the broad size

distribution of the arc smokes as explained in Section IV.  Thus these

forward scattering techniques are only partially successful in solving

the problem of sizing sub-micron polydisperse particles with unknown

refractive indices.  Instantaneous intensity ratio methods are suggested

in the next chapter on a possible solution to this problem.

-------
                                   32
VII Instantaneous Intensity-Ratio Measurements



     The fact that the intensity-ratio measurements In the forward scat-



tering lobe yield results insensitive to refractive index, makes the



size measurement of highly dispersive systems (with unknown index m)



similar to those encountered in smoke stacks and power plants possible.



Besides its limitation in handling complex and broad size distributions,



the methods of average intensity-ratio measurements described above are



time consuming; they cannot be considered as real-time methods to monitor



particulate size distribution in the size range of urgent importance



(O.Olym to lOvnu).  The difficulties encountered in determining the



particle distribution from angular-dependent average intensity-measure-



ments can be avoided if the particles are viewed one at a time.  If the



instantaneous two-angle intensity ratios, 1(0 )/i(8_) and the polariza-



tion ratio, i|i(6)/i|(9) can be measured with sufficient resolution, not



only can theoretical analysis be much simplified, a real-time determina-


                                                               19
tion of complex size distributions should be possible.  Gravatt   was



the first to devise a system to measure size distribution in real-time


                                       20
with two-angle scattering.  Chan et al.   have considered the possibil-



ities of real-time measurements in more details.



     If there is at most one particle scattering light at any instant,



the measured intensity-ratio is a function of time,




          1(6,, a)


                  = P[e9'al = p[a(t)1 = p(t)
When there is no particle scattering light at a particular instant,



p[a(t)] gives no signal  (only noisy fluctuations). Whenever a particle



passes through the scattering volume, light will be scattered to yield



an  intensity-ratio current pulse corresponding to a particular particle



size.  The pulse width depends on  the response of the photomultlplier

-------
                                   33
and amplifiers used.  Processing of the measured signal, p(t), by means




of either a probability analyzer or a pulse-height analyzer would give




the frequency of occurrence of the intensity-ratio current pulses as a




function of pulse height (thus particle size).  When the pulse height is




transformed to the size parameter by Mie scattering theory, a direct




determination of size distribtuion  f(a)  can be made.  The discussion




here holds for either the instantaneous two-angle intensity-ratio or




the instantaneous polarization-ratio measurements.  The technique can




handle nearly any type of particle distributions, and gives real-time



measurements.




     The technique of detecting the individual particles is achieved by




focusing the viewing laser radiation onto a small scattering volume V;




the particulate matter under study is flowing across this scattering




volume with speed  v  as shown in Fig. 8(a).  For clarity, the scatter-




ing volume is assumed to be orthorhombic with volume V ° abfc.  The total




number of particles in the scattering volume at any time would on the




average be N - nV where  n  is particle concentration.  The scattered




radiation is detected by a photomultiplier-amplifier system whose




response time or resolution time it  T_.
                                      K


     One way'to view individual particles is to allow one particle at a




time into the scattering volume, i.e., N = 1.  This would put an upper




limit on the detectable concentration, i.e., n <^V   = (ab£)  .  Since




there is only one particle traversing the scattering volume at any



time, the photomultiplier-amplifier system records non-overlapping cur-




rent pulses whose width equals particle transit time  T .  For the



arrangement considered  T  = b/v.  Fig. 8(b) shows current pulses de-




tected for a modest flow speed  v; the magnitude of an individual

-------
                                   34
pulse depends on the particle size under viewing at the instant.  As



flow speed increases, T  decreases and the current pulses come closer



together in time as shown in Fig. 8(c).  Because It takes a finite time



for the electronics in the detection system to respond, the transit



time  T   must be larger than the resolution time  T_ if the current
       C                                            R


pulses are to maintain their individual identities.  This limits the



flow speed to be less than b/T , i.e., v = b/T  < b/T .  For example,
                              K               t      J\

                                                    _3
if we choose a scattering volume with a = b = 2 x 10   cm (20ym) and


           _3
I = 25 x 10   cm (250ym), which is typical and practical, the maximum



concentration which can be handled would be  n = (ab£)   - 10 /c.c.  for


       —(\                                                     —"\   —6
TD = 10   sec, the maximum flow speed manageable is v = 2 x 10  /10   =
 K


2 x 10  cm/sec.  Although not commonly recognized, it is quite clear



that by committing oneself to this case of  N = 1, the electronic system



is not efficiently used for slower flows.  One should be able to increase



the manageable concentration by improving the detection efficiency.



This can be done by allowing the total number of scatterers to be greater



than unity.



     When there are several particles in the scattering volume at a



time, the detecting system will record several overlapping pulses in a



transit time  T .  The number of ripples during a transit time  T



shown in Fig. 8(d) corresponds to the number of particles  N  in the



scattering volume.  Due to the fact that individual particles are



still seen individually as long as the ripples in Fig. 8(d) are distinc-



tive.  As flow speed increases, or  T   decreases, the ripples come



closer together as shown in Fig. 8(e).  Because the time between two



successive ripples, T  , called particle arrival interval, is much less
                     A

-------
                                   35
than the transit time  T  (T  = — T  for N = 3 as shown in Figs. 8 (a)
                        t   *\   J  t


and 8(e), one must make sure that individual particles arrive at an



interval  T.  longer than the electronic response time of the system  T



if the particles are to be individually identified.  Since on the average



there are  N  particles arrived for viewing in a transit time, T. = T /N.



The only criterion for "single" particle detection is then,
                          b ___ b_ _  1      T_                   (15)

               N  "  N    vN   vnabA ~ vna£  -
Or, equivalently ,
          n < (valT"                                              (16)
                                        -3                -3
Using the same example of a = b = 2 x 10   cm, I = 25 x 10   cm,


          3                   -6
v = 2 x 10  cm/sec and T  = 10   sec, one obtains again the maximum
                        K


detectable particle concentration of  n = 10 /c.c.  However, when the



flow speed is made slower by two orders of magnitude, the maximum


                                        g

detectable concentration can go up to 10 /c.c. for the same scattering


             — 7   ^                             —ft
volume V = 10   cm  and resolution time  T  = 10~  sec.  The detectable



concentration can be made even higher if faster electronics are used.



In short, the capability of the detection system is fully utilized when



the total number of scatterers in the scattering volume is allowed to



be larger than one.  The flow speed  v  and the size of scattering volume



(more precisely the cross-sectional area, ai) together determine the



detectable concentration.  For readily available electronic and optical



set up, instantaneous intensity-ratio measurements can be easily carried



out for particle concentrations of 10 /c.c. under a typical flow con-



dition with speed around 10  cm/sec.

                                         o

     Continuous-Wave He-Ne laser (X= 6328A) and argon-ion laser

         o         o

(A = 4880A and 5140A) may be used for the experiments.  Different

-------
                                   36
wavelengths not only provide a check for the size distribution measure-



ment but allow an extension of the range of particle size measurable by



the proposed techniques.  For a given measurable parameter  a =  ird/A,



the particle diameter measured depends on the incident wavelength.



     A self-contained real-time device for determination of particle



size distribution is shown in Fig. 9.  The set up is schematically


                                19
similar to that used by Gravatt,   except the conversion function



p[6 ,6.,a] resulted from Mie theory is included in the present scheme.



The Inclusion of this conversion function should not only broaden the



range of detectable size parameter  a, but increase the accuracy of



particle sizing.  Because the particles are viewed "one at a time In



the set up, the system of Fig. 9 permits automatic determination of



particle concentration as well.

-------
                                          37
                       Sample
                       Volume
                           Lens     Aperture
            Laser
I(t)4

PMT




AMP

1(1)

                                         Light/
                                         Block
                                        (a)
                                                                     Large
                                                                     Particle
                                                                          Small
                                                                         Particle
                                        J	I
                                                                     j	I
                   (b)
                                                    (0
             H   h-TA
                   (d)
                                                    (e)
       a.
       b.
       c.
       d.
       e.
       Fig.  8  Viewing Particles in a Flowing System
Experimental arrangement.
Current pulses for a modest flow speed.
Current pulses for an increased flow speed.
Viewing several flowing particles in the scattering volume.
Viewing several flowing particles in the scattering volume
at increased speed.

-------
Optical
Chamber
Electronic  Unit
              PMT
           Movable on
             Track
   Intake
                                                                        Probability
                                                                            or
                                                                       Pulse-Height
                                                                         Analyzer
                               -[AMP j-
                                         I2(0
x= Pin-hole
    Fig. 9.  A Proposed  Real Time Device for  the Determination of Particle Size Distribution

-------
                                   39
VIII Discussion




     In this chapter we summarize the research results obtained so far,




the investigations which are being continued but could not be reported




at this time and suggest some extended work for real-time application




which should be done in the future.




A.  Summary of Results and Critique of the Experimental Methods



     The transmission method investigated in this work gives both the




number density and the average size particles.  However, the method




involves more than one light source or one set of optical set-up and




only gives average size information.  The application of the method




also depends on a knowledge of the refractive index and an available




E (a,m) theoretical curve.  In air pollution monitoring, this does




not seem to be promising as having great potentials for developing




into real-time techniques.




     Light scattering measurements, in spite of its complications, offer




many more variations and possibilities and in special circumstances,




they can be greatly simplified.  Two special scattering methods have




been investigated.  The two-angle forward scattering ratio method has




been found to give reliable and accurate results of size measurement




and most important, the method does not require a knowledge of the




refractive index and it would seem to have a practical and real-time




potential application.  The polarization ration method is found to




give both average size and size distribution.  Although in general the




method depends on the refractive index, measurements limited to the




forward direction could make its dependence on refractive index




unimportant.

-------
                                   40
B.  Future Work




     The ultimate goal of this work is to develop, at least in principle,




a rugged, practical, outdoor and real-time air-pollution monitoring




system for the enforcement of pollution standards by the EPA.  Hence,




the future work will involve in refining, extending and combining the




two-angle forward scattering ratio method as well as the polarization




method so that they will yield size distribution measurement in real-




time or almost real-time conditions.  Although the 'average* scattered




light measurements described in this investigation does rely on the




computer to obtain particle size, preliminary investigations suggest




with the fast electronics now commercially available, 'instantaneous1




scattered signal can be analyzed and a real-time device based on this



approach is indeed possible.  The details of this investigation as well




as design specifications of the device are described in a forthcoming



proposal to the EPA.

-------
IX.   References;

     1.  H. C. Van de Hulst, Light Scattering by Small Particles, (Wiley
         & Sons,  Inc., New York, 1957).

     2.  S. Ramo, J. R. Whinnery and T. Van Duzer, Fields and Waves in
         Communication in Electronics, (John Wiley, New York, 1967).

     3.  J. R. Hoskinson, Proceedings of the First National Conference
         on Aerosols, edited by K. Spuony (Gordon & Reach Science
         Publishers, New York, 1965).

     4.  J. R. Hodkinson, I.C.E.S., Electromagnetic Scattering, edited
         by Milton Kerker (Pergammon Press, London, 1963).

     5.  J. R. Hodkinson and I. Greensleaves, J. Opt. Soc. Am.^3, 577
         (1963).

     6.  R. B. Porndorf, J.  Opt. Soc. Am. 47, 1010 (1957).

     7.  J. R. Hodkinson, The Optical Measurement of Aerosols in Aerosol
         Science, edited by C. N. Davies (Academic Press, N. Y., 1966).

     8.  J. R. Hodkinson, Appl. Optics .5, 839 (1966).

     9.  K. S. Shifrin and A. Y. Perlman, Tellus 1£, 566 (1966).

    10.  K. S. Shifrin and A. Y. Perlman, Optical Spect. (Eng. Trans.)
         20, 385  (1966).

    11.  M. Kerker, E. Matijevic, W. F. Espenscheid, W. A. Farone and
         S. Kitani, J. Coll. Sci., 19_, 213 (1964).

    12.  M. Kerker, The Scattering of Light, (Academic Press, New York,
         1919).

    13.  E. Matijeori, S. Kitani, and M. Kerker, "Aerosol Studies by
         Light Scattering II.  Preparation of Octanoic Acid Aerosols of
         Narrow and Reproducible Size Distributions," Jour. Coll. Sci.
         19, 233  (1964).

    14.  H. H. Denman, W. Heller, and W. J. Pangonis, Angular Scattering
         Functions for Spheres, Wayne State Univ. Press, Detroit (1966).

    15.  K. S. Shifrin and A. Y. Perlman, Electromagnetic Scattering,
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    16.  0. Apichatanon, "Measuring Aersol Distributions," M.S. Thesis,
         Colorado State University (1974).

    17.  J. E. Me Donald, "Visibility Reduction Due to Jet-Exhaust Carbon
         Particles," J. Appl. Met., ],, 391 (1962).

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18.   G.  Hass and L.  Hadley in American Institute of Physics Handbook,
     edited by Daniel N. Fischel, Harold B.  Crawford, Don A. Douglas,
     and Winifred C. Eisler (McGraw-Hill Book Company, New York, Third
     Edition, 1972).

19.   C.  C. Gravatt,  Jr., "Real Time Measurement of the Size Distribution
     of Farticulate Matter in Air by a Light Scattering Method," presented
     at Annual Meeting of the Air Pollution Control Association at Miami
     Beach, Florida, June 18-22, 1972.

20.   P.  W. Chan, 0.  Apichatanon, and C. Y. She, "Particle Size Measure-
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     Presented at the Annual Meeting of Air Pollution Control Association
     at Denver, Colorado, June 10-13, 197A.

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                                      43
                                TECHNICAL REPORT DATA
                          (Please read luanii tuna on llir rerene before completing)
 I REPORT NO.
  EPA-650/2-74-034
 J TITLE AND SUBTITLE
                           2.
Optical Measurements of Smoke Particle Size
   Generated by Electric Arcs
                                5. REPORT DATE
                                  June 1974
                                6. PERFORMING ORGANIZATION CODE
                                                      3. RECIPIENT'S ACCESSION-NO.
7 AUTHOR(S)

P.W.  Chan
                                                      8 PERFORMING ORGANIZATION REPORT NO.
9 PERFORMING ORGANIZATION NAME AND ADDRESS
Colorado State University
Fort Collins , Colorado  80521
                                                      10 PROGRAM ELEMENT NO.
                                  1AB012; ROAP 21ADL-21
                                 11 CONTRACT/GRANT NO.

                                  Grant R-800150
12 SPONSORING AGENCY NAME AND ADDRESS
EPA, Office of Research and Development
NERC-RTP, Control Systems Laboratory
Research Triangle Park, NC  27711
                                 13 TYPE OF REPORT AND PERIOD COVERED
                                 • Final
                                 14 SPONSORING AGENCY CODE
15 SUPPLEMENTARY NOTES
16 ABSTRACT ft\e report gives results of a study of the use of lipt transmission ana
photometric scattering measurements  using    lasers for sizing polydispersed metal-
lic  particulate systems (often with unknown index of refraction) produced by  a dc elec-
tric arc smoke generator. The study emphasized the reliability and accuracy of these
techniques, the  information obtainable,  and potentials  for developing these methods
into real-time techniques. Transmission (extinction) methods are simple to  apply and
give average particle size and number density if the refractive index is known: accu-
racy is good but the size distribution cannot be obtained.  The two-angle forward scat-
tering intensity  ratio method gives by far the most accurate results- most important,
it does not depend on a knowledge of the refractive index. Average size measurements
have been obtained with this technique on several metallic and non-metallic particulate
systems; the size distribution  can also be obtained by computer calculation.  The
polarization ratio method gives better sensitivity for smaller sub-micron particles
(though dependent on refractive index unless forward scattering is used) and has been
used successfully to measure size distribution of sub-micron latex spheres.  Also
discussed is combining the intensity ratio method (at two forward scattering angles)
and the polarization ratio method (at one forward angle) for sizing polydispersed
particulate systems. and developing it into real-time devices.
17.
                             KEY WORDS AND DOCUMENT ANALYSIS
                DESCRIPTORS
                                          b IDENTIFIERS/OPEN ENDED TERMS
                                             C. COSATI 1 Icld/Group
Air Pollution
Optical Measurement
Smoke
Particle Size
   Distribution
Electric Arcs
Lasers
Light Transmission
Smoke Generators
Reliability
Accuracy
Forward Scattering
Rexractivity
Extinction     	
Air Pollution Control
Photometric Scattering
Particulates
Polarization Ratio
Two-Angle Forward
 Scattering Intensity
 Ratio
13B,  20F,
14B , 15B
21B , 14D
20N
      20H
20C
20E
 '1 OlSmiBUTION STATEMENT

Unlimited
                    19 SECURITY CLASS (Hut Report)
                    Unclassified
                         21 NO. OF PAGES
                             49
                                          20 SECURITY CLASS (Tinspage)
                                          Unclassified
                                                                   22 PRICE
CPA Form 2220-1 (9-73)

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