United States
Environmental Protection
Agency
Health Effects Research
Laboratory
Research Triangle Park NC 27711
EPA-600/4-79-002
January 1979
Research and Development
Analysis of
Ensemble Averaged
Concentrations and
Fluxes in a Tracer
Puff

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                                              EPA-600/4-79-002
                                              January  1979
ANALYSIS OF ENSEMBLE AVERAGED CONCENTRATIONS
         AND FLUXES IN A TRACER PUFF
                     by
              Main R. Hutcheson
            School of Meteorology
           University of Oklahoma
           Norman, Oklahoma  73019
              Grant No. 804507
               Project Officer

            Kenneth L. Demerjian
     Meteorology and Assessment Division
 Environmental Sciences Research Laboratory
     Research Triangle Park, N.C.  27711
ENVIRONMENTAL SCIENCES RESEARCH LABORATORY
     OFFICE OF RESEARCH AND DEVELOPMENT
    U.S. ENVIRONMENTAL PROTECTION AGENCY
     RESEARCH TRIANGLE PARK, N.C.  27711

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                          DISCLAIMER
      This report has been reviewed by the Environmental Sciences
Research Laboratory, U.S. Environmental Protection Agency, and
approved for publication.  Approval does not signify that the con-
tents necessarily reflect the views and policies of the U.S. En-
vironmental Protection Agency, nor does mention of trade names or
commercial products constitute endorsement or recommendation for
use.
                                11

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                           ABSTRACT
      This research was initiated to analyze tracer concentra-
tions and fluxes in a diffusing puff released from an instan-
taneous ground level point source.  The concentration data used
was made available by the Battelle Memorial Institute.  Three
basic steps are performed.  First, an estimate of the ensemble
averaged tracer fluxes is developed.  Secondly, an estimate of
the ensemble averaged tracer concentration is obtained.  Then
the estimates are used to determine concentrations and fluxes
which satisfy the diffusion equation and are as close to the
estimates as possible.

      The tracer fluxes are estimated as the negative of the pro-
ducts of the appropriate diffusivities and concentration gradi-
ents.  The diffusivities are derived using the fact that they
are proportional to a characteristic length and velocity scale.
This approach yields diffusivities which are the diffusion rates
for a Gaussian puff.  The flux estimates are shown to satisfy
the diffusion equation for all puff diffusion rates when com-
bined with a Gaussian concentration model.

      Since the available observations are too sparse to use
alone in obtaining a concentration analysis in space and time,
a concentration model is developed to provide data at grid
points where there are no observations.  This model is a modi-
fication of the Gaussian one, taking into account surface scav-
enging and wind shear.  A variational technique then incorpor-
ates the observations and model data into concentration analyses.
A variable observational weight forces the analyses towards the
observations, and time filtering in a Lagrangian coordinate sys-
tem allows the effect of an observation to be felt over several
analysis times.  Spatial filtering spreads the effect of the
observations and helps eliminate short waves.  The resulting
analyses conform to the observations and provide reasonable con-
centration distributions in both space and time.

      A model to estimate the ensemble averaged concentration is
developed based upon the above analyses.  Due to the random na-
ture of turbulence, concentrations averaged over many trials
should be more nearly normally distributed in the horizontal
than the analyses are.  Therefore, the model estimates are nor-
mally distributed in the horizontal, but the centroid of the
horizontal distribution at a given level is displaced downwind
relative to the centroid at the adjacent lower level.  This type

                               iii

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of distribution is in general agreement with the concentration
analyses described above.  The ensemble averaged concentration
estimates are then made to conform to the analyses as closely as
possible using a least squares technique.  Concentration gradi-
ents are obtained from these estimates for use in computing the
estimated fluxes.

      The concentration and flux estimates are combined with the
diffusion equation in a variational functional.  The Euler equa-
tions resulting from taking the first variation of the functional
may be solved so that concentrations and fluxes obtained satisfy
the diffusion equation and are as close to the estimates as the
observational weights allow.  It is assumed that these quantities
are the ensemble averaged concentrations and fluxes.

      The ensemble averaged concentrations are close to the anal-
yses obtained from the first variational technique in magnitude,
but the ensemble averaged horizontal distributions are more Gaus-
sian.  Furthermore the ensemble averaged concentrations are in
very close agreement with the observed-concentrations.  Since
they also satisfy the diffusion equation, the ensemble averaged
concentrations obtained are very reasonable.

      The ensemble averaged concentrations and horizontal fluxes
are very close to their estimates, but the vertical flux differs
significantly from its estimate.  Due to the manner in which the
observational weights were chosen, this indicates that the con-
centration and horizontal fluxes may be modeled in the manner in
which the estimates are obtained, but some modification must be
made to correctly model the vertical flux.  Since the horizontal
fluxes are close to their estimates, they are nearly proportional
to the concentration gradients.  Therefore, in this case, the
diffusivity concept has a physical significance.  Since the dif-
fusivities are the diffusion rates of the puff, they can be mea-
sured in the atmospheric surface layer.
                               IV

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                           CONTENTS

Abstract	iii
Figures	    vi
Tables	vizi
Abbreviations and Symbols	    ix
Acknowledgment 	  xiii
    1.  introduction 	     1
    2.  Review of Pertinent Diffusion Theories and Assumed
        Puff Distribution	     3
             The Gaussian model	     3
             Diffusivity and the diffusion equation	     4
             The gradient transfer hypothesis	     5
             The statistical theory of dispersion	     6
    3.  Determination of the Turbulent Flux Estimates.  ...    10
             Diffusivity and the diffusion rate	    10
             Satisfaction of the diffusion equation	    11
             Boundary conditions 	    11
             A relationship with the statistical theory
             of turbulence	    12
             Expressions for the fluxes	    15
    4.  Data utilized in This Research	    16
             Krypton-85 as an atmospheric tracer 	    16
             Puff dimensions	    20
    5.  Determination of the Ensemble Averaged Concentra-
        tion Estimate	    25
             The initial concentration model 	    25
             Combining the model data and observations  ...    36
             Filtering characteristics 	    39
             Boundaries	    45
             Analyzed concentrations 	    45
             Concentration estimates 	    61
    6.  Combining Flux and Concentration Estimates 	    64
             The variational formalism 	    64
             Analysis of a Gaussian puff	    66
             Analysis of puffs P5 and P7	    70
             Ensemble average concentrations 	    76
    7.  Conclusions	    81
Bibliography 	    84
Appendices

    A.  Derivation of the expression for diffusivity ....    87
    B.  Centered finite difference algorithms	    90
    C.  Numerical solution of the analysis functional.  ...    92
    D.  Numerical solution of the functional combining
        flux and concentration estimates 	    94
                               v

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                     FIGURES
Numbe]
1.
2.
3.
4.
5.
6.
7.

8.
9.

10.

11.
12.
13.

14.

15.

16.

17.
r
Tentative profiles of vertical diffusivity 	
Motion of a tracer particle in a turbulent flow . . .
Motion of two particles in a puff 	
•A.
Schematic representation of the field grid 	
Concentrations at the 1.5 m level for test P5 . . . .
Concentration profiles on the 114° azimuth for
test P5 	
Concentrations at the 1.5 m level for test P7 . . . .
Concentration profiles on the 114° azimuth for
test P7 	
Relationship between observation and model
coordinates 	
Time cross section at grid point 13,8,3 for test P5 .
Time cross section at grid point 16,7,5 for test P5 .
Response function using a9/a-, = 20, do/a-, =2.5 and
a4/ai - 50 	 \ ! . . . .J. t 	
Response function using a0/an = 1, ao/Oh = .125 and
~ //>, — •? c: ^ J. J J-
a4/al ~^*-> 	
Analyzed concentrations at the 1.5 m level for
puff P5 	
Analyzed concentrations at the 6.1 m level for
puff P5 	
Analyzed concentrations at the 1.5 m level for
Page
7
7
13
13
17
30

31
32

33

34
34
37

41

43

48

52

puff P7 .......................   55
                        vi

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 18.   Analyzed concentrations at the 6.1 m level for
       puff P7	58

 19.   Ensemble averaged concentration for Case 1, test P5,
       at the 1.5 m level	67

 20.   Ensemble averaged downwind flux for Case 1, test P5,
       at the 1.5 m level	67

 21.   Ensemble averaged crosswind flux for Case 1,
       test P5, at the 1.5 m level	68

 22.   Ensemble averaged vertical flux for Case 1,
       test P5, at the 1.5 m level	68

 23.   Ensemble averaged concentration profile for Case 1,
       test P5	69

 24.   Ensemble averaged concentration for Case 2,
       test P5, at the 1.5 m level	69

 25.   Ensemble averaged downwind flux for Case 2,
       test P5, at the 1.5 m level	73

 26.   Ensemble averaged crosswind flux for Case 2,
       test P5, at the 1.5 m level	73

 27.   Ensemble averaged vertical flux for Case 2,
       test P5, at the 1.5 m level	75

 28.   Ensemble averaged concentration for Case 2,
       test P7, at the 1.5 m level	75

 29.   Ensemble averaged downwind flux for Case 2,
       test P7, at the 1.5 m level	77

 30.   Ensemble averaged crosswind flux for Case 2,
       test P7, at the 1.5 m level	77

 31.   Ensemble averaged vertical flux for Case 2,
       test P7, at the 1.5 m level	78

 32.   Ensemble averaged concentration profile for Case 2,
       test P5	78

33.    Ensemble averaged concentration profile for Case 2,
       test P7	    79
                              Vll

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                            TABLES


Number                                                      Page

  1.   Meteorological Data for the Two Tests	18

  2.   Measurements of Puff Dimensions	21

  3.   Puff Diffusion Rates	,  .  .  23

  4.   Available Data for Test P5 When the Puff Centroid  is
       Near the 200 m Measuring Arc	26

  5.   Available Data for Test P7 When the Puff Centroid  is
       Near the 200 m Measuring Arc	27

  6.   Parameters Optimized to Fit the Model to
       Observations	29

  7.   Analyzed Concentrations for Test P5 When the Puff
       Centroid is Near the 200 m Measuring Arc	46

  8.   Analyzed Concentrations for Test P7 When the Puff
       Centroid is Near the 200 m Measuring Arc	47

  9.   Parameters Optimized to Fit an Ensemble Averaged
       Estimate to the Analysis	62

 10.   Diffusivities and Their variances 	  71

 11.   Correlation Between Fluxes	72
                              Vlll

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                  ABBREVIATIONS  AND SYMBOLS


   A   scavenging factor

   A   amplitude  of  filtered analysis

   A   amplitude  of  observations

  a,   constant of proportionality  for downwind standard devia-
       tion relation

  a~   constant of proportionality  for crosswind standard devi-
       ation relation

  a.,   constant of proportionality  for vertical standard devia-
       tion relation

   B   the value of \ on the ordinate

  b,   time power for downwind standard deviation relation

  b_   time power for crosswind standard deviation relation

  b3   time power for vertical standard deviation relation

C(T)   correlation between u'(tf -  T) and u'(tf)

C(t)   dimensionless time dependent parameter

  C,   time dependent proportionality parameter

  C9   correlation between a  and u1
   £                        ^C
  C3   ratio of C, to C2

   F   over relaxation factor

  F    flux in the x direction
   5C

  F    flux in the y direction

  F    flux in the z direction
   &

  F    estimated flux in the x direction
                             ix

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   F    estimated flux in the y direction



   F    estimated flux in the z direction
    z



    G   constant determined by interval-halving



   K    diffusivity in the x direction
    j£


   K    diffusivity in the y direction



   K_   diffusivity in the z direction
    Z


    k   wave number




   L    wavelength,  downwind direction
    JS.




y or z   transverse wavelength



   t,    characteristic length scale

        distance that a tracer particle is displaced from the

        puff centroid in the x direction



    Q   Actual source strength



   Q '    virtual source strength



    R   response function



   Rv   residual of the Euler equation at the v-th iteration



    r   detector count rate



    T   Lagrangian integral scale



   T    period of the wave
    o   c


    t   travel time from the source



   t.    lower limit of the time integration



   tf   observation time



   At   time interval



    u   mean wind velocity



   u1   turbulent wind fluctuation in the x direction



   u    effective transport wind speed

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    v1   turbulent wind fluctuation in the y direction

    VR   variance of the residual of the diffusion equation

    w'   turbulent wind fluctuation in the z direction

     x   distance of the puff centroid from the source

    x1   distance that a tracer particle is carried in the
         x direction by turbulent wind fluctuations

     y   crosswind distance from the puff centroid

    y1   distance that a tracer particle is carried in the
         y direction by turbulent wind fluctuations

    AX   downwind grid interval

    Ay   crosswind grid interval

     z   vertical distance from the puff centroid

    z'   distance that a tracer particle is carried in the
         z direction by turbulent wind fluctuations

    AZ   vertical grid interval

    z    height at which u  is determined
     o                    o

    ct-i   observational weight

o,2» 0,3*
0,4/0,5    filtering weights

     P   -dlnA/dt

Yi'Y2'
Y-5'YA    observational weights

    \    spectral scale of the vertical component of motion

     e   rate of dissipation of turbulent kinetic energy per unit
         mass of air

    a    concentration standard deviation in the x direction
     2t

    a    concentration standard deviation in the y direction

    a_   concentration standard deviation in the z direction
     Z

     T   tf - t
                               XI

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cp   azimuthal angle to puff centroid

X   ensemble averaged puff concentration

X   krypton-85 concentration

X   analyzed concentration

X   model concentration or, if available,  krypton-85
    concentration

    ensemble averaged concentration estimates
                         xii

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                       ACKNOWLEDGEMENTS
      I wish to express my sincere gratitude to Dr. Rex L. Inman,
who was my scientific counselor.  His encouragement, understand-
ing of meteorology and knowledge of the research process helped
me immeasurably during this research.

      I am grateful for suggestions made by other members of my
Doctoral Committee, Drs. E. M. Wilkins, Y. K. Sasaki, R. A. Mill,
R. L. Coleman and E. D. King.

      I wish to also thank my lovely wife, without whom comple-
tion of this research would have been impossible.  She not only
gave me needed moral support, she also helped me check the math.

      This research was supported by the Environmental Sciences
Research Laboratory, United states Environmental Protection
Agency, under Research Grant 804507.
                             Xlll

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                           SECTION 1

                         INTRODUCTION
      This paper describes an analysis technique which has been
developed to analyze ensemble averaged concentrations and fluxes
for tracer puffs diffusing in the surface layer.  It is not pos-
sible to achieve this goal using available observations directly,
because it is impossible to measure the ensemble averaged pro-
perties of the puffs.  The ensemble average is an average taken
over a large number of individual events which occur under iden-
tical ambient conditions.

      It is sometimes possible to estimate ensemble averages from
time averages.  As shown by Wyngaard  (1973), the turbulent pro-
perties of a stationary flow may be derived from time averages,
if the averaging period is sufficiently long.  However, a tracer
puff residing in stationary flow is continuously changing, due
to the diffusion process.  The puff, unlike a tracer plume, can
never achieve a steady state.  Therefore, long time averages are
not representative of the ensemble averaged properties of the
puff and other means of obtaining the concentrations and fluxes
must be developed.

      Fluxes are derived which satisfy the diffusion equation for
a Gaussian puff spreading out at an arbitrary rate.  These fluxes
are then used as estimates of the ensemble averaged fluxes for a
puff diffusing in the surface layer.

      Concentration estimates may be based upon observed data;
however, this information is usually too sparce to use alone in
analyzing concentrations.  Therefore, analyses are obtained by
combining the data with a concentration model using a variational
technique.  The model is a modification of the Gaussian distri-
bution which accounts for wind shear and surface scavenging.  The
ensemble averaged concentration is more nearly normally distri-
buted than is the concentration in an individual puff, so the
ensemble averaged concentration estimates are produced by the
model such that they are normally distributed in the horizontal
and as close to the analyses as possible.

      In the next step the flux and concentration estimates are
combined to produce ensemble averages which satisfy the diffusion
equation.  This is accomplished through the use of a variational
formalism, which forces satisfaction of the diffusion equation

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while keeping the analyzed fluxes and concentrations close to the
estimates.  These quantities are assumed to be the true ensemble
averaged concentrations and fluxes.

      The analysis technique has been tested on two data sets
collected by the Battelle Memorial Institute.  The data sets con-
sist of radiation measurements obtained from Geiger Miiller tubes
when 85 Kr was released as instantaneous point sources.  The
Geiger Miiller tubes were arranged on arcs at 200 and 800 m from
the source.  The radiation measurements are converted to concen-
trations and may be compared with the concentration analysis.

      Horizontal and vertical cross sections of observed and
analyzed concentrations are constructed.  The analyzed concen-
trations agree closely with those observed.

      Two research tools are developed which deserve special men-
tion because of their applicability to other diffusion studies.
In Section 3 a method of estimating diffusivities is explained.
It is later shown that this method is valid for puffs which are
reasonably Gaussian in shape.  In Section 6 a variational for-
malism is developed which produces superior analyses of concen-
trations and fluxes, since the results are forced to satisfy the
diffusion equation.  While these techniques are developed for
diffusing puffs, they can be adapted for use with plumes.

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                           SECTION 2

          REVIEW OF PERTINENT DIFFUSION THEORIES AND

                   ASSUMED PUFF DISTRIBUTION
      In order to perform this research, it is necessary to ob-
tain estimates of the ensemble averaged fluxes and concentrations
in a diffusing tracer puff.  To this end theories which attempt
to explain the mechanism by which tracer fluxes diffuse the puff
and describe the shape which the puff will subsequently assume
will be examined below.

THE GAUSSIAN MODEL

      The tracer puff concentration distribution upon which this
research is based is the ubiquitous Gaussian diffusion model
(Roberts, e_t al^ , 1970), which maybe represented as


     X = -   - expC-t^-)2 + -   + -]} .         (1)
The mean wind, u, is in the x direction where x is the distance
of the puff centroid from the source, and y and z are perpen-
dicular horizontal and vertical, respectively, from the puff
centroid.  The ax, ay and az are the time dependent standard
deviations of the puff concentration, y^, in the respective co-
ordinate directions and Q ' is the virtual source strength.
This is the source strength which, at a given travel time, t,
would be required to produce the concentration observed at x, y,
z  (Van der Hoven, 1968) .  It is assumed, therefore, that the
scavenging of the tracer is uniform throughout the puff, and Q'
will decrease with increasing travel time, in the absence of
sources other than the initial one.  A scavenging factor A may
be defined such that

                            Q1 = AQ ,                         (2)

where Q is the actual source strength.

      The Gaussian model is applicable only under homogeneous,
stationary conditions in which the tracer concentration exhibits
a normal distribution.  While this model is not universally ap-
plicable, it will be used here to represent an ensemble averaged

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puff concentration in the absence of external boundaries, be-
cause, due to the random nature of turbulence, the concentration
averaged over many experiments within the same turbulent flow is
more nearly normally distributed than is that of a single puff.
The model will be modified to provide an estimate of the ensem-
ble averaged concentration of a tracer puff diffusing in the
atmospheric surface layer.

      The concentration standard deviations are assumed to have
a power dependence upon time which may be expressed as

              bl              b2                 b3
      ax = a-^t   ,    a  = a2t   , and   az = a3t   .        (3)


Since the a's and b's are arbitrary and the standard deviations
increase from zero at the source, little restriction is placed
upon them or their derivatives by this assumption.  Substitution
of (3) into (1) yields
                                     t     2a2 t     2a3 t

                                                              (4)

DIFFUSIVITY AND THE DIFFUSION EQUATION

      In order to develop reasonable extimates of tracer fluxes,
the mechanism by which a puff diffuses must be examined.  The
diffusion equation and the diffusivity concept will be intro-
duced in order to aid in this examination.  It can be shown that,
under the proper circumstances,  (4) is a solution to the Fickian
diffusion equation, modified to  accomodate a sink term, p^.  This
will be done in order to examine the restrictions which must be
placed on the concentration standard deviations and the sink term
in order for (4) to satisfy the  diffusion equation.  This dif-
fusion equation may be expressed as
      The diffusivities, K  , Ky and K  , may be expressed in  terms
of the standard deviationsX(Pasquill,  1974) such  that

        Kx = ax/2t  ,     Ky = o^/2t  and   KZ = az/2t  .       (6)


These relationships  are  obtained by equating the  solution  of the
Fickian diffusion equation  to Eq.  (1).  The analytical solution
to the Fickian equation  using the appropriate boundary conditions
was  first obtained by Roberts  (1923).

      The temporal  and spatial derivatives in  (5)  are  evaluated
                               4

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using (2) and  (4) as follows:
                            °X              °Y
                 2
                   - 1]} + X       ,                           (7)
                                     - 1]  ,                   (8)
                             2
                           rY. __ n
                    222
and                          2
                               - 1]  -                        do)
                             z
Substitution of (6) -(10) into  (5) yields
                        °z
                      2
             (b  - -)[   - 1]} + X(L +  p)  =  0  .            (11)
Thus, the Gaussian model may be a  solution  to  the  Fickian  dif-
fusion equation when b^ = b2 = b3  =  1/2.  That this  is  the ex-
pected result may easily be demonstrated by combining  (3)  and
(6) to obtain
               2bx              2b2                  2b3
           a, t             a7                    a?
      Kx = —^ - .   Ky = — ^ -  ,   and   KZ = -^ -  .   (12)


When b^ = b2 = b3 = 1/2, Kx, Ky and  Kz  are  constant.   In  addi-
tion to the diffusivities being constant,  (3 must be  equal  to
- SlnA/Bt to satisfy  (11).

THE GRADIENT TRANSFER HYPOTHESIS

      The gradient transfer hypothesis  assumes that  turbulence
causes a net movement of tracer down the gradient  of material
concentration at a rate proportional to the magnitude  of  the
gradient  (Pasquill, 1974) .  Therefore,

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              x    •   Fy s - K

For b-i = b2 = b3 = 1/2 the fluxes may be obtained since Kx, KV/
Kz and •£ are known.  However, when the puff is spreading such
that t>i ^ b2 7^ b3 ^ 1/2, the fluxes are not known since the dif
fusivities are no longer constant.
      In general b^, ^2 an<^ ^3 are ^ar from equal, and are us-
ually not close to 1/2.  In the data utilized in this study b^
and b2 are always much larger than 1/2.  As Pasquill (1974)
points out, the use of a constant diffusivity when dealing with
atmospheric turbulence is obviously erroneous.  Therefore, flux-
es cannot be determined using (13) unless an expression for the
diffusivities is found which is applicable to puff spreading out
at an arbitrary rate.  The diffusivities represented by (6) will
therefore be a special case of this general formulation, valid
when b^ = b2 = b3 = 1/2.  Since the diffusivities represented by
(6) are not applicable to a puff diffusing in the surface layer,
other formulations must be utilized.

      Little is known about the nature of the diffusivity of an
inert material.  The gradient transfer hypothesis has proven use-
ful, but there is no consistent means of accurately predicting
eddy diffusivity variations under untested conditions (Lewellen,'
et. al_. , 1972).  Pasquill (1970) states that since no a priori
specification of the eddy diffusivity is available, the K-theory
approach is physically plausible and equivalent to other approach-
es only for the case of vertical spread from a source at ground
level.  The practical equivalence of the above approach and simi-
larity theory may be demonstrated for short range vertical dif-
fusion in neutral conditions.  A form for Kz may be obtained
(Pasquill, 1974) such that
where e is the rate of dissipation of  turbulent kinetic energy
per unit mass of  air  and  \m is the spectral  scale of the verti-
cal component of  motion.  Xm = u/nm, where nm  is the frequency
at which the normalized spectral density  function is a maximum.
Using (14) it is  possible to specify a K  profile over a consid-
erable height range and in any stability, since turbulence data
on e and Xm is becoming increasingly available,  profiles ob-
tained using  (14)  for unstable, neutral and  stable cases, re-
spectively, are displayed in Fig. 1.   Note that all profiles
begin with a near-linear  increase with height  but then depart
from this significantly.

THE STATISTICAL THEORY OF DISPERSION

      In order to gain a better understanding  of the diffusion

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             Fig. 1.  Tentative profiles  of
             vertical diffusivity.  (From
             Pasquill, 1974)
   X7
x'(t
                       •f
 a.   The path of a tracer
 particle displaced a dis-
 tance x1 (tf) at time tf.
                              u'=o
                                         t-
                    t,
b.  The distance x' (tf)
is the shaded area  under
the curve .
 Fig. 2.  Motion of a tracer particle in a turbulent  flow.

                            7

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mechanism, so that reasonable flux estimates may be obtained, the
statistical theory of dispersion will be examined.  Some of the
concepts developed here will be used in the determination of dif-
fusivities which yield reasonable flux estimates.  Furthermore,
it will be shown that at long travel times the diffusion rate
obtained from the statistical theory is the diffusivity required
to satisfy the diffusion equation.  The above theory attempts to
explain the mechanism by which tracer is spread in a puff.  Tay-
lor (1921) derived a fundamental diffusion theorem which applies
to diffusion in one space dimension or to three-dimensional dif-
fusion in-a stationary, homogeneous turbulent flow.  He postu-
lated that the distance, x1, that a tracer particle is carried
away from an origin by turbulent wind fluctuations, u1, at the
observation time, tf, is
                               r
                     x'(t ) = /  u'(t) dt .                  (15)
                         r    -o

This relationship between distance and velocity perturbation is
shown in Fig. 2.  Since u'(tf) and the ensemble averaging process
are independent of time,       ^
                x'(tf)u'(tf) =J  u'(t)u'(tf) dt  .            (16)


Taylor demonstrated that the usual laws of differentiation may
be applied to the mean values of fluctuating variables and their
products.  Therefore,     	

                        ^f^-1 = 2 ^T ,                    (17)

where
                               = u.
                                 U   *

Substitution into  (16) yields

                      	     tf
                        ,2    (
                  \ ^dt }  % u'(t>u'(tf) dt  •              <18)

      In the stationary flow  that is considered  here, the origin
of time is irrelevant, so  that the correlation between u'(t)  and
u'(tf) will depend only upon  the time difference T  = tf  - t.
Since u'(tf - r)u'(tf) is  the covariance  of u1,  a correlation
coefficient, C(T) may be defined:

                              U'(t   - T)u'(t  )
                       C(T) =	— ,             (19)
         2
where u1   is  the  variance  of the  downwind  component  of the wind

                                8

-------
velocity perturbation.  The correlation coefficient decreases as
the time interval T increases, and at large values of T the velo
cities are uncorrelated.  Substitution of  (19) into (18) and use
of the definition of T yields
                         _         tf
                           2    _  • f
                     ±djl_l = u,2    C(T) dr ^            (2Q)
      A Lagrangian integral scale, T, may be defined  (Tennekes
and Lumley, 1972) such that
                       T =   C(T) dt .                       (21)
                           'o

It is assumed that C(T) decreases rapidly enough that at large T
the Lagrangian integral scale is finite.

      Therefore, far from the source (where tf is sufficiently
large)                   _
                       2  dt          '

so that the diffusion rate of the puff is constant in this re-
gion.  There are several ways to demonstrate that the puff should
in fact diffuse at a constant rate far from the source  (Gifford,
1968) .  It will be shown in the next section that at long travel
times the diffusivity required for satisfaction of the diffusion
                                     2
equation at all diffusion rates is u1  T.  Using  (13), the de-
sired fluxes may therefore be obtained far from the source using
the statistical theory of turbulence.

      A basis for the required ensemble averaged flux and concen-
tration estimates has been developed using established theories.
The Gaussian model will be modified to provide reasonable con-
centration estimates in the atmospheric surface layer.  Fluxes
will be estimated with the air of the diffusivity concept.  The
validity of the dif fusivities derived in the next section will
be tested to show that the resulting fluxes satisfy the diffu-
sion equation.  Furthermore, it will be shown that far from the
source the dif fusivities are the diffusion rates obtained using
the statistical theory of turbulence.

-------
                           SECTION 3

         DETERMINATION OF THE TURBULENT FLUX ESTIMATES
      In the preceding section it was shown that fluxes obtained
from the gradient transfer hypothesis, using the conventional
expressions for diffusivity, do not satisfy the diffusion equa-
tion for a Gaussian puff except when the diffusion rate is con-
stant.  Since the diffusion rate observed for puffs in the atmos-
pheric surface layer is not constant except far from the source,
it is desirable to use other expressions for the diffusivities.
In this section it will be shown that, if the diffusivity is ex-
pressed as the diffusion rate, the diffusion equation for a Gaus-
sian puff is satisfied for all diffusion rates.  Fluxes obtained
using these diffusivities will be employed later as estimates of
the fluxes in a puff diffusing in the surface layer.

DIFFUSIVITY AND THE DIFFUSION RATE

      Pasquill (1974) expressed the diffusivity as the diffusion
rate at large travel times.  His formulation, which may be writ-
ten as                           	

                          K  = I d*'2                        /23)
                          Kx   2  dt  '                      (   '

employs the diffusion rate derived from Taylor's fundamental dif-
fusion theorem.  It was shown in Section 2 that the diffusion
rate in (23) is valid for a diffusing puff only at distances far
from the source.  Therefore, a limiting value, which the diffu-
sivity must approach at long travel times, may be obtained by
combining  (23) and  (22) to obtain

                          KX = u'2 T  .                       (24)


      Hildebrand  (1977) defined an apparent eddy diffusivity as

                                    2

                                                             (25)


Similar expressions may be defined for the y and z directions.
In order to illustrate the nature of  this diffusivity a deriva-
tion is shown  in Appendix A.
                               10

-------
SATISFACTION OF THE DIFFUSION EQUATION

      Using the procedure employed  in Section 2,  it may be shown
that the dif fusivities defined by  (25)  satisfy the diffusion
equation for all puff diffusion rates.   Since the dif fusivities
are functions of time only,  the diffusion  equation may be ex-
pressed as
if the sink term used  in Section  2  is  included.   Substituting
(7) -(10) and  (25)  into (26) one may obtain
                                   (b2
                                             °y
         (b3 - b3)c   -  1]} + X  (T   -     T)  = 0 .       (27)
This equation, as opposed to  (11) ,  is  identically zero.   There-
fore, (4) is a solution to the diffusion  equation for the values
of the a ' s and b ' s  one expects to find in the atmospheric sur-
face layer.

BOUNDARY CONDITIONS

      A restriction  is placed upon these  quantities by the bound
ary conditions.  The conditions  specifying a point source are
(Button, 1953) :

               •X ->  0 as t -» oo                                (28)

               •% -»  0 as t -» 0   (except at the source)        (29)
  ,               o°
and              r
                    xdV = Q1 .                                (30)
                ••' — oo
      In order for  (4) to satisfy the  first boundary condition,
b]_,  b2 and b3 must be positive.   For the  second boundary condi-
tion to hold,  a.]_, a.2 and a^ must be positive.  Remembering the
definition of  the density function of  a normal distribution and
its special properties  (Mood  and Graybill,  1963) , it is  easy to
show that under these circumstances the third boundary condition
is also satisfied by the Gaussian model.   Using (1) Eq.  (30)
becomes
Q'
          _ro (2TT,

-------
Since the concentration distribution is jointly as well as sep-
arately normal,  (31) may be written as
                oo  oo  oo
                f.
            Q1 .   ,      n(x) n(y) n(z) dxdydz =Q' ,          (32)
               ™"*OO ""• CO ^C
where n(x), n(y) and n(z) represent the density  functions of  the
normal distributions in the respective coordinate directions.
Since
         00            00            00

          n(x) dx s    n(y) dy s    n(z) dz = 1  ,            (33)
       • A-flO          •-' —00           — 00

the third boundary condition is indeed satisfied.

      Even though the  three boundary conditions  discussed above
are adequate  for Fiekian diffusion, a more stringent boundary
condition is  needed when the diffusivity is time dependent.   It
can be shown  that an inverse relationship between diffusivity
and travel time is unreasonable for a Gaussian puff.  As seen in
Appendix A, the diffusivity is proportional to the product  of a
characteristic eddy velocity scale, which must be constant  in a
stationary flow, and a characteristic length scale.  Therefore,
the length scale must  decrease with travel time  if Kx does.   This
cannot occur  under the conditions  necessary for  the tracer  con-
centration to obtain a normal distribution.  Under these condi-
tions the eddy size most effective in transporting tracer par-
ticles, hence the characteristic  length scale, will increase  as
the puff grows, until  the largest  eddies are dominant.

      Since the diffusivity, hence diffusion rate, must  increase
with travel time or remain constant for a Gaussian puff, a  new
boundary condition may be formulated.  Using  (3) ,


       1 dax     2   ^l""1    1 day    2   2b2"1
       2 ~dt  = al blt      '  2 dt = a2 b2fc       and


                       1 d°z     2   2b3~l
                       I -ST = 33 V       •                  <34>

In order  for  the diffusion rates  to increase or  remain constant
with travel time, b^,  b2 and b3 must be equal  to or greater than
1/2.  This  is a more  stringent requirement than  (28), which re-
quired that the b ' s be positive.

A RELATIONSHIP WITH THE STATISTICAL THEORY OF  TURBULENCE

      It  is important  to understand the relationship between the
diffusion  rates used  in this  section  and  those derived  from the
statistical theory of  turbulence.   Then  it will  be possible to

                              12

-------
  x'(t
                          +tp
Fig. 3.  Motion of two particles  in  a
puff.  The puff centroid is at p  at  time

V
    u'=o
       o  t,
                MOLECULE TRAJECTORIES
 Fig. 4.
Relationships between^,  and u'.
                       3C
 The shaded areas equal
                         x'
and
                      t'-[ and
 are the lower integration limits  required
                   13

-------
compare these diffusivities with those obtained by Pasquill.
Proceeding in a manner similar to that used in Section 2,  (A.9)
may be integrated to obtain

                            tf
                     £  =    u1 dt ,                         (35)
                      X    ti

where £x is the distance that a tracer particle is displaced from
the puff centroid in the downwind direction.  The above expres-
sion is similar to Taylor's diffusion theorem, Eq.  (14), except
that the integration is from a time ti rather than the initial
time, as seen in a comparison of Figs. 2, 3 and 4.  The tj_ ^ 0
unless x'(tf) = &x.  Multiplying both sides of  (35) by u'(tf)
and taking an ensemble average, we obtain
               £
                x
u'u1 (tf) dt .                  (36)
      Changing the viewpoint from which Taylor observed  the  dif-
fusion process, a series  of puffs released  from  a point  source
under identical conditions are considered here.  The particle
which arrives at x' (tf) after each release  is studied.   As de-
picted in Fig. 3, the position of the puff  centroid with respect
to the abscissa is variable.  Therefore, the position  at travel
time tf will change  for each release.  The  length £  ,  for par-
ticles which arrive  at x'(tf) will be different, due to  the
change in centroid position.  Furthermore,  the path which the
particles took to arrive  at x'(tf) changes  due to the  randomness
of the turbulence.   While the total  area under the curve in
Fig. 4 is always x'(tf),  the area under any segment  of the curve
varies.  For these reasons the time  ti must be different for
each release.

      Since t  is variable,  in general
                  u'u'(tf)  dt   ^       u'u'(tf)  dt .         (37)


 However,  under the proper circumstances,  the variation of ti is
 not important.  For stationary turbulence Eq. (36) may be written
 as                         6t
                *xu'(tf)  =    u'(tf - T)  u'(tf)  dT ,          (38)
                           o

 where 6t = tf - ti and T was defined in the preceding section.
 Where tf is very large in comparison with tj_, 6t is essentially
 constant and the ensemble average may now be taken inside the
 integral.  In this case  (38) may be written as
                               14

-------
                 £ u1 (t-) = u1     C(T) dT ,                 (39)
                  x    r        0


where C(T) was defined in  (19).  The consequence of a large  6t
is the same as described for a large tf in Section 2.  When
tf - ti is large the integral becomes constant, regardless of
§t.  In this case  (39) may be written as
                         da?.
                                                             (40)
using  (A. 10) and the definition of the Lagrangian  integral scale.
Since  §t can only be large at long travel times,  (40)  is valid
far from the source.

      A comparison of  (40) and  (22) shows that the diffusion rate
employed in this section  is identical to that obtained using Tay-
lor's  classical diffusion theorem at distances far from the
source.  Therefore, the dif fusivities reach the  limiting value
obtained by Pasquill (1974) at  large distances.

EXPRESSIONS FOR THE FLUXES

       Since the diffusivities in  (25) satisfy the diffusion equa-
tion under the specified restrictions, exact expressions for the
fluxes under these conditions may be obtained.   Using  (25) and
(13),
where Fx, Fv and Fz are the fluxes in the respective coordinate
directions.  Therefore, the fluxes are known  as a  function of
space and time for a puff diffusing in a stationary, homogeneous
non-isotropic flow in which the scavenging of the  tracer  is uni-
form.  It has not been shown how well the true fluxes are repre-
sented by  (41) for a puff diffusing in the atmospheric  surface
layer.  in this case the flow is neither stationary nor homo-
geneous.  Furthermore the contact of the puff with the  surface
ensures that the scavenging is not uniform throughout the puff.

      Because the fluxes represented by  (41)  have  been  shown to
be valid for a Gaussian puff diffusing at an  arbitrary  rate,
they will be used as estimates of the ensemble averaged fluxes
in the puffs selected for analysis.  The validity  of the  esti-
mates will be examined further in a later section.
                               15

-------
                          SECTION 4

                DATA UTILIZED IN THIS RESEARCH
      In order to develop an estimate of the ensemble averaged
puff concentrations as a function of space and time, analyses of
puffs of tracer material released from an instantaneous point
source must be obtained.  Details for the ensemble averaged con-
centration estimates are then deduced from these analyses.

KRYPTON-85 AS AN ATMOSPHERIC TRACER

      Since the small puffs rapidly pass the concentration mea-
suring devices, instruments with fast response times must be
used.  The best concentration measurements available for analy-
sis were obtained from the release of the radioactive gas
krypton-85 as an atmospheric tracer.  Since the gas is radio-
active, measuring devices with very high response times may be
used to sample it.  Krypton-85 is inert, so the tracer has mini-
mum interaction with structures or vegetation, and it does not
react with other atmospheric constituents (Nickola et al.,
1970a).

      Nickola et al. (1970b) published the concentration mea-
surements as a volume of atmospheric diffusion data, due to their
high quality.  Measurements were made simultaneously at 64 field
locations.  The sampling array, on arcs at distances of 200 and
800 m from the source, consisted of 40 Geiger-Miiller tubes at 2°
intervals and an elevation of 1.5 m above the surface with 24
more tubes on 6 towers  (see Fig. 5).  The 200 m arc towers were
instrumented at .8, 1.5, 3.0, 6.1 and 10.7 m.  The 800 m arc
towers were instrumented at .8, 1.5, 4.6, 10.7 and 21.3 m.

      The dispersing krypton-85 gas emitted  .69 Mev  (max) beta
particles which were detected by the halogen-quenched Gerger-
Miiller tubes.  Information from these detectors was relayed to
a 4096 address memory, programed to accept data simultaneously
from the 64 detectors for 64 time increments.  Time intervals
permitted were 1.2, 2.4, 4.8 and 38.4 sec.

      Ambient wind  and  stability data are available from two
meteorological towers located near  the  source.  The wind speed
sensors were three-cup  anemometers, and the wind direction trans-
ducers were Beckman and Whitley Model 1565 vanes.  Since the
wind vanes were poorly  oriented, no mean wind directions were
published.
                               16

-------
           Source
              122 - m-A
           Meteorology Tower
- m Meteorology
    Tower
Fig.  5.  Schematic representation of the field grid.
(From Nickola et al.,  1970a)
                           17

-------




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      There were thirteen releases of the noble gas tracer.
Eight of these were in the form of instantaneous puffs, while
the remaining five took the form of plume releases of 10 to 20
minutes duration.  The puffs were generated by crushing quartz
ampules containing the tracer in a quillotine-like device at
ground level.  The gas in each ampule was sealed at mean atmos-
pheric pressure to minimize the initial volume of the instan-
taneous point source.

      The data from two of the eight puff releases are available
for analysis here.  in experiments P5 and P7 the puff centroids
passed close enough to one of the instrumented towers so that a
reliable vertical profile of the puff is available for the 200 m
arc.  Puff P5 was released during a period of high wind speeds.
It was therefore considered practical to start the automatic
data storage increments well before tracer arrival and concen-
tration measurements taken every 2.4 sec sampled the entire puff
within the 64 time increment limit.  The meteorological data for
test P5 is given in Table 1.  While the highest wind speed was
observed in this experiment, the speed and direction standard
deviations are not larger than in some other cases.  The Rich-
ardson number computed by Nickola (1971) for this case is -.02/
indicating an essentially neutral atmosphere.

      Puff P7 was released on the day following the release of
P5 when the wind speeds were lower.  In this case some tracer
arrived at the 200 m measuring arc prior to switching the moni-
toring system from accumulate to automatic.  Therefore, the con-
centrations were not observed at specified times until the puff
was well into the monitoring system.  As is the case with test
P5, the tracer is completely embraced within the horizontal ex-
tent of the grid, and tracer concentration at all detectors re-
turned to the background level prior to the completion of the
data storage period.  Due to the slower wind speed, which kept
the puff in the field grid for a longer period of time than in
the previous experiment, a time increment of 4.8 seconds was
used.  The meteorological data for test P7 is given in Table 1.
The Richardson number for this test was -.16, indicating an un-
stable situation.

      The concentrations used in this study were deduced from
the detector count rates.  A total of 1.9 counts/sec was sub-
tracted by Nickola et al. (1970a).  This subtracted value con-
sists of a background mean of about 1.2 counts/sec plus approxi-
mately three standard deviations from that mean.  The relative
concentrations listed in the volume of atmospheric diffusion
data are in counts per 10 sec.  Meaningful atmospheric concen-
trations may be obtained from these count rates by using the
relationship

                          X = .103r ,                       (42)

where •% is the krypton-85 concentration in |j C./m  and r is

                               19

-------
detector count rate in counts/sec.

PUFF DIMENSIONS

      Nickola  (1971) computed the puff dimensions at the 200 and
800 m arcs.  The array of samplers is relatively dense in terms
of atmospheric sampling grids, but is inadequate for completely
defining concentration distribution in a small puff.  Spacing
between sampling arcs is 600 m, and between towers is 56 m and
224 m, on the 200 and 800 m arcs, respectively.  Since none of
the puffs intersect more than two towers at a given distance
from the source, we have little knowledge of the distribution of
concentration with time on a horizontal plane other than z=1.5m.
The puffs generally extended above the top of the sampling array,
so the puff distribution could not be completely determined on
any vertical plane.

      Since the distribution of concentration with time is well
defined for the 1.5 m height, Nickola computed the crosswind and
downwind standard deviations of the distribution at this height.
He assumed that the mean transport wind is applicable during an
entire puff passage at a given distance and at the 1.5 m eleva-
tion, so the observed distribution with respect to time may be
converted to a distribution with respect to downwind distance.
The standard deviation of the crosswind summed concentration dis-
tribution of 8^Kr, a -  may therefore be computed.

      The downwind integration of concentration with time may be
performed using Ax = u At, where Ax is the downwind grid inter-
val and At is the time increment over which the ^'s were suc-
cessively measured.  The exposure, Y^At/Q, was computed by
Nickola, and the standard deviation of the downwind summed con-
centration distribution, axj, obtained from the exposure dis-
tribution.

      The vertical concentration profiles obtained did not, in
general, resemble those obtained from the Gaussian model, which
predicts that, for perfect surface reflection of the tracer, a
half-bell shape is obtained from a surface release.  Because of
this, Nickola  computed the azi values by two different methods.
Where possible, the data was used directly and total perfect re-
flection was assumed.  This technique was used only in cases
where the vertical profile approached the half-bell shape, such
as for puff P7 on the 200 m arc.  In an attempt to eliminate the
interferring effects of the surface, ozj values were usually gen-
erated using a second technique.  The observed exposures were
redistributed  into  a virtual distribution extending below ground
level, assuming that the tracer was partially rather than totally
reflected.  The exposures were then subtracted from a given level
above the surface and added to a level below the surface on a
trial and error basis until a  curve with a reasonably smooth,
bell  like shape was obtained.  Computation of azj was then

                               20

-------





























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performed.  Because the puffs were not, in general, normally
distributed in the vertical, azj does not define the puff as
uniquely as aT or a, T do.
             x j.     y •*-
      The values that Nickola obtained for the puff dimensions
are displayed in Table 2.  Note that for puff P5 no az-r value
was given at the 800 m arc.  Examination of the data shows that
the vertical concentration profiles bears no resemblance to a
normal distribution at the observation tower.  However, a value
for ozj is needed in order to determine the rate at which the
puff is spreading in the vicinity of the 200 m arc.  Since the
puff diffuses very slowly iri the vertical under all conditions,
an average azj was computed from the azj's determined for the
other puffs.  This value was used for puff P5 on the 800 m arc.

      Since it takes a finite time for a puff to pass an arc,
the instantaneous width of the puff will be less than the width
of arc intercepted by the puff, due to the effect of meander of
the wind.  However, Nickola (1971) points out that, for a puff
released under the unstable or neutral conditions considered
here, there is essentially no difference in these two widths,
due to the relatively high wind speeds and resulting short peri-
od of puff passage at an arc.  Therefore, it is assumed that the
instantaneous and integrated standard deviations are identical.

      Since most of the data was collected at the 1.5 m level,
it is at this level that ax and av are valid.  However, useful
standard deviations are in the plane passing through the puff
centroid, which may be at a different level.  Since the puffs
were released at the surface, it is assumed that their centroids
remain at this level, but that the standard deviations are those
measured at the 1.5 m level.

      The a's and b's used to define the standard deviations in
(3) may now be determined using the axi» CTyi and ozj computed by
Nickola at 200 and 800 m from the source.  A system of two equa-
tions in two unknowns may be set up for each coordinate direc-
tion.  In the downwind direction,

                In o     = In a, + b. In t2QQ
                    X200

                ln a     = ln al + bl ln ^00 '              <43>

Similar equations may be derived in the other directions.

      The a^, etc., obtained yield the measured standard devia-
tions at 200 and 800 m from the source, but ax, Gy and az deter-
mined when the puff centroid is not on a measuring arc are valid
only if the time rate of change of puff size is correct.

      The puff's diffusion rates are determined using  (34).  The

                               22

-------
Table 3.  Puff diffusion rates.

time
37.6
40.0
66.4
71.2
experiment
P5
P7
experime
P5
P5
P7
P7
al
2.034
1.247

-»t
mt 2 dt
32.6
33.9
11.7
12.2
a2 33
.02452 .2704
.01544 1.573
1 dav
~2 dt
3.09
3.54
2.21
2.55
bl b2
.8131 1.612
.7718 1.537
!^2
2 dt
.547
.568
.232
.227
b3
.8070
.3446
                               23

-------
results are displayed in Table 3 for the travel times on either
side of the time the puff centroid crossed the 200 m arc.  The
diffusion rates all increase with time except for vertical dif-
fusion in experiment P7.  In this case the diffusion rate de-
creases,  since ~b% is less than 1/2.  This cannot occur under the
assumptions stated in Section 2.  It is shown in Section 3 that
the diffusion rate for a Gaussian puff increases with travel
time until the puff is far from the source.  However, the assump-
tions used in the previous sections are not applicable in the
atmospheric surface layer.

      It was shown in Section 2 that the nature of the function-
al dependence of the puff growth rate upon time changed as the
travel time increased.  It must be assumed that this is true for
the growth rate of the analyzed puffs also.  Since the puff's
dimensions were measured on only two arcs, only one set of a's
and b's are obtained for each experiment.  Therefore, only one
functional dependence is computed using  (43), so the puff dif-
fusion rates obtained cannot be valid over the entire travel
time of the puff.  The diffusion rates obtained are therefore
a reasonable estimate of the true diffusion rates for some time
interval within the time required for the puff centroid to reach
the 800 m arc.  It is assumed that this time interval includes
those observation times when the puff centroid is near the 200 m
arc.
                               24

-------
                           SECTION 5

            DETERMINATION OF THE ENSEMBLE AVERAGED

                    CONCENTRATION ESTIMATE
      Since the array of samplers is inadequate to completely
define the concentration distribution in a tracer puff, conven-
tional analysis techniques cannot be used here.  The data used
at the six times closest to the time the puff passed the 200 m
arc are given in Tables 4 and 5.  The analyses are most likely
to be correct at times when the puff centroid is near the mea-
suring arc.  However, analyses are produced at fourteen times
in test P5, and ten times in test P7, so that the temporal bound-
aries will be far from the analyses of interest.

      A modified analysis, based upon Sasaki's (1970a, b and c)
variational method is performed.  First, a concentration model
is fitted as closely as possible to the available data.  The
model values are replaced by Nickola's observations at the appro-
priate grid points.  The results are then filtered in space and
time using the variational technique.  The concentration model
is modified and refitted to the resulting analysis in order to
obtain an estimate of the ensemble averaged concentration.

THE INITIAL CONCENTRATION MODEL

      The basic concentration model utilized is defined by (4).
However, the Gaussian model does not account for two processes
which occur in the atmospheric surface layer.  Wind speed shear
is present in any boundary layer.  Also, since the SS^r tracer
is inert, scavenging occurs only at the surface.  These proces-
ses tend to deform the puff from a normal distribution.

      In order to account for these processes, the Gaussian model
is modified by making u a function of height such that

                         u - UQ + G(z - ZQ) ,               (44)


where uo is the effective transport wind speed, computed by
Nickola  (1971) at the observation level zo = 1.5 m.  A linear
wind profile is assumed because both surface scavenging and wind
shear are accounted for by this method.  This produces a dis-
tinctly different concentration distribution than would be

                              25

-------
Table 4.  Available data for test P5 when the puff centroid is near
the 200 m measuring arc.  (From Nickola et al.  (1970b))

a. Concentrations
Time 104 106
32.8 1.5 4.7
35.2 .9 5.6
37.6 .7 2.7
40.0 1. 12.5
42.4 .4 2.0
44.8 .3 1.8
b. Concentrations








(nCi/m ) at the 1.5 m level
Azimuth (degrees)
108 110 112 114 116
63.8 120.
62.3 162.
37.2 191.
55.0 166.
11.5 93.
9.7 77.
(nCi/m3)

Time
32.8
35.2
37.6
40.0
42.4
44.8
0 167.9
1 210.9
5 176.7
7 157.4
3 100.1
7 114.4
at the

.8
214.4
161.6
130.0
121.4
110.0
78.0
203.4 64.6
132.5 48.7
127.4 26.8
117.2 14.6
87.3 24.6
58.8 50.7
114 azimuth
Level (m)
3. 6
208.5 191
96.1 54
71.8 29
84.8 26
76.1 34
34.4 16
118 120
9.2 4.5
5.7 3.4
4.1 1.0
2.0 .3
1.1 .7
6.2 1.3


.1
.7
.5
.3
.5
.3
.9
122 124
2.5 .2
2.1 .3
1.1 .1
1.5 0.
.4 0.
.6 .1









                               26

-------
Table 5.  Available data for test P7 when the puff centroid is near
the 200 m measuring arc.  (From Nickola et al. (1970b))

a. Concentrations (^Ci/m ) at the 1.5 m level
Azimuth (degrees)
Time 104 106 108 110 112 114 116 118 120 122
56
61
66
71
76
80
b.








.8 .2 0. 2.2
.6 .2 .1 4.
.4 .3 12.3 22.2
.2 2.1 12.7 25.9
.0 1.2 5.8 25.2
.8 0. 1.1 6.7
34.1
15.
49.9
53.4
63.2
32.3
Concentrations (|jCi/m ) at

Time
56.8
61.6
66.4
71.2
76.0
80.8

.8
237.3
240.4
181.2
132.6
90.2
46.8
134.7 212
85.4 213
90.7 160
111.6 107
70.2 71
30.5 44
the 114*
Level
3
221.2
214.0
158.4
75.9
43.1
37.3
.5 126.9 24.8 15. 6.
.6 100.6 58.7 27.6 10.4
.9 68.7 50.9 20.2 5.2
.5 32.2 36.7 21.2 3.2
.5 32.5 22.1 4.8 .8
.9 19.3 10.6 5.1 1.5
azimuth

6.1
234.0
78.2
61.0
24.3
17.8
6.8
124
.3
.9
.2
.3
.1
.8









                             27

-------
obtained using a traditional power law vertical profile, such
as the one employed by Yeh and Huang  (1975) .  Since the centroids
of the horizontal concentration distributions are displaced down-
wind with height, the maximum concentration in the forward part
of the puff is aloft, while the maximum concentration in the
rearward portion is on the surface.  This is in agreement with
the observations.  The G is then chosen such that the model con-
centrations are as close to those observed as possible.  it is
implicitly assumed here that while tracer is scavenged only at
the surface, small turbulent eddies with time scales smaller
than the incremental averaging time tend to smooth our discon-
tinuities produced by the surface scavenging and the effect of
wind shear.  Tl>e concentration model therefore has a normal dis-
tribution in the horizontal, but the vertical concentration dis-
tribution is not Gaussian.

      The variables which must be determined such that the model
fits the observed data as closely as possible are;  A(t), aj_, a2/
33, bi, b2/ b3, u(z), x(t) and y(t) .  The alf a2, aj, blf b2 and
b3 are obtained by the method described in the previous section
and A(t) is defined in (2).

      The x(t) and y(t) may be computed when the azimuth, cp(t) ,
of the puff centroid is known.  The azimuth must be determined
at each observation time to ensure optimal fit to the data, so
an interval-halving technique is utilized for this purpose.  An
azimuth interval is chosen which contains the optimalAaximuth.
The interval is then halved until the quantity
                                                      .
mized, where ^ is the measured concentration  and -^  is obtained
from  (4) .  When the quantity  is a minimum the optimal azimuth is
obtained.

      Since, data useful in determining the  optimal  azimuth  is
contained only in the measuring arc  at 1.5  m  elevation,  other
data may be ignored in this interval-halving  technique.  Nichola
computed the transport wind speed at the arc  level,  so u(1.5 m)
is known.  Since the interval-halving technique minimizes the
difference between the model  value and the  data,  it is not  nec-
essary to optimize A(t) at this point.  Therefore,  A (t)  is  taken
to be 1 without loss of accuracy in  determining the optimal azi-
muthal angle.

      The optimal azimuth displays some variability,  as  seen  in
Table 6, for two reasons.  As the puffs move  with the flow, wind
fluctuations cause the puff centroids to meander.   Furthermore,
the actual puffs are somewhat non-Gaussian, as seen in Fig. 6
to 9.  As the model adjusts to the tracer observations on the
200 m arc, shifts in the optimal azimuth will occur.  Therefore,
the variability of the azimuth is not due solely  to changes in
the centroid ' s azimuthal position, it is partly due to irregu-
larities in the puff's concentration distribution.   This intro-
duces an error in the estimate of the puff's  azimuth.


                               28

-------
Table 6.  Parameters optimized to fit the model to observations
Travel time

23.2
25.6
28.0
30.4
32.8
35.2
37.6
40.0
42.4
44.8
47.2
49.6
52.0
54.4

52.0
56.8
61.6
66.4
71.2
76.0
80.8
85.6
90.4
95.2
B(t)
a.
.7708
.4261
2.260
6.854
4.271
1.639
-2.151
-1.922
- .4363
-1.142
.04
- .2584
- .4419
- .577
b.
5.586
2.669
-1.827
.5847
.0433
- .5869
- .4587
- .7582
- .2361
.01481
A(t)
Test P5
1.207
1.008
.8978
.7309
.6701
.5632
.5420
.5794
.4675
.5036
.4494
.5275
.4654
.4514
Test P7
.9881
.8061
.5983
.5047
.4790
.5051
.4292
.4267
.3247
.1775
CD(t)

115.8
112.6
112.6
113.3
112.8
111.8
111.6
111.4
112.1
112.3
111.5
110.9
112.2
113.6

113.7
113.9
114.3
113.8
112.8
112.4
113.0
113.5
113.7
113.4
tp(t) = optimal azimuthal angle
A(t) = coefficient obtained from least squares fit
B(t) = constant obtained from least squares fit
Optimal G for release P5 = .1875
Optimal G for release P7 = .1016
                               29

-------
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                             31

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-------
SOURCE
                                    OBSERVATION SITE
                                      	—  PUFF CENTROID
                                    X-Dt   I
Fig.  10.  Relationship between observation and  model
coordinates.   The cp represents the  aximuthal angle to
the  puff centroid, while  cp1  is the  azimuthal angle to
the  observation site and  ro  is the  radial distance to
the  observation site.
     	 MODEL
     	ANALYSIS
  3000

  2000
  1000
   922
   600
   700
   600
   500
 f  400
•P 300

 ^ 200
 O
 a.

 * '
   60
   50
   40

   30

   20
                               0 OBSERVATION
    10
    20.B
       23.2 25.6 280 30.4 32.8 352 37.6 400 424  44.8 47.2 496  52.0 34.4
                        t (sec.)—
 Fig. 11.
 8,  3.
Concentration profile at grid  point 13,
                           34

-------
      Once the azimuth is evaluated, the position of the obser-
vation sites with respect to the model coordinates may be com-
puted.  Therefore, the x and y distances needed in  (4) may be
obtained.  As shown in Fig. 10, the optimal azimuth is the direc-
tion from the source to the puff centroid.  Since the azimuth and
range of the observation site is known, x and y may be determined
from the geometry depicted.

      The data on the_vertical tower is utilized to obtain the
mean transport wind, u, as a function of height.  G is determined
by the interval-halving technique using data from all the avail-
able times.  Not only is it undesirable to obtain G at each time,
it is impossible.  Since A(t) has not been optimized, when data
at only one time is used, the quantity I(x' ~ X)^ ^s minimized
by forcing G to be either very small or very large, depending
upon whether the puff centroid has reached the measuring arc or
not.

      A(t) is the final parameter to be determined.  It may be
found using a least squares fit at each observation time.  The
regression equation used to obtain A(t) is

                      X = B(t) + A(t) x' ,                   (45)

where x' is given by (4) with Q1 = Q and B(t) is the value of x
on the ordinate.  A comparison of Table 6 with Tables 4 and 5
shows that B(t) is very small in comparison with the observed
concentrations in the vicinity of the puff centroid, and may
therefore be ignored.  As seen in Table 6, A(t) generally de-
creases with travel time.  Due to the nature of A(t)  (see Eq.
(2)), the decrease is most likely a result of the puff losing
mass as it proceeds downwind.  However, if the puff were Gaus-
sian, residing on the surface, and totally scavenged upon en-
countering the ground, A(t) could not be less than one.  When
the centroid of a Gaussian puff is on the surface, the mass flux
must be away from the surface, towards lower concentrations.
Only the concentration in the lower half of the theoretical puff
is considered scavenged.  If no absorption occurs, then the
tracer is reflected from the surface and A(t) = 2.

      Since the optimal A(t) is generally less than one, the
Gaussian model with the puff centroid on the surface cannot fit
the data very effectively because there must be some mass flux
towards the surface.  As seen in Figs. 6 and 8, the tracer puff
is reasonably Gaussian in the horizontal.  However, in the verti-
cal, the puff is somewhat non-Gaussian.  The data shows that in
the forward portion of the puff there is a concentration gradient
towards the surface.  This is reflected in the model, and is one
of the reasons it was decided to depart from the Gaussian verti-
cal profile.

      The optimal A(t) in Table 6 decreases in a somewhat

                               35

-------
irregular manner and at times actually increases.  Due to irreg-
ularities in the tracer puff, A(t) is forced to behave errat-
ically in order to fit the data as closely as possible at each
observation time using the least squares procedure.

      Figs. 6 to 9 show that the model does a good job of fitting
the data in the horizontal;  an acceptable fit in the vertical is
also obtained.  Since the puff is not normally distributed in the
vertical, it is more difficult to model the vertical concentra-
tion profile.  For example, in experiment P5, the data shows that
until t = 32.8 sec, when the forward portion of the puff resided
over the 200 m measuring arc, concentrations aloft consistently
exceed those at the .8 m level.  However at t = 35.2 sec, the
concentration at the .8 m level greatly exceeds those aloft  (see
Table 4).  The model is not capable of changing the vertical pro-
file in such a rapid manner.  However, at t = 40 sec in Fig. 7,
the .8 m model concentration has become larger than those at
higher levels.  At longer travel times the concentration at the
.8 m level is always the greatest.  Therefore, the concentration
in the central and rearward portions of the puff is largest near
the surface while in the forward portions of the puff the concen-
tration is largest aloft.

COMBINING MODEL DATA AND OBSERVATIONS

      In order to reduce some of the irregularities in the model,
an analysis combining both model and measured data is performed.
The resulting concentrations are to be utilized in the determi-
nation  of ensemble averaged  concentration estimates.  These  esti-
mates, along with estimates  of the tracer fluxes will be forced
to conform to the diffusion equation, Eq. (5), in which the  local
time rate of change of concentration is one of the most important
terms.  It is therefore imperative that the grid point concentra-
tions change smoothly in time, if reasonable  fluxes are to be
obtained.  Since the puff centroid's position fluctuates, and
A(t) changes in an erratic manner, the model  concentrations  at
a grid point exhibit a high  amplitude, short  period fluctuation,
as shown in Figs. 11 and 12.  Therefore, it is necessary to  im-
pose a  low pass filter in time on the data in order to damp  out
the short period fluctuations.

      As seen in Table 6, there are times when A(t) actually in-
creases rather than decreases.  This  suggests that some source
has added to the tracer mass in the puff at that time.  This,
however, is unreasonable, since the only source of tracer is  at
the initial time.  Smoothing in time eliminates the bogus
sources.

      Figs.  6-9 show that the model does not  conform  to the  ob-
servations exactly.  Therefore, it is desirable to design the
filter  such  that there is a  tendency  to force the  analysis  to-
wards the collected data.  This may be accomplished by using a

                               36

-------
        	MODEL
        	ANALYSIS
   300
   200
 t 100
 ST 90
 E 80

 5 ro
 ^ 60
 X 5°
   40

   30
   20
    10
                         © OBSERVATION
     20.8 23.7 256 280 30.4 328 35.2  376 400 42.4 44.8 47.2 496 52.0 54.4
                           t(sec.)-*
Fig.  12.   Concentration  profile at grid point 16,
7,  5.
                                37

-------
higher observational weight at grid points where data is avail-
able.  However, it is more important that the resulting analysis
be smooth, rather than conform to the data.  Therefore, filter-
ing weights are chosen such that the analyses do not always con-
form .to the data exactly.  However, Figs. 6-9 show that in gen-
eral the analyses are closer to the data than the model is.

      The concentration model cannot account for many of the
mechanisms by which a puff disperses.  For example, a backing or
veering wind will tilt the puff.  This produces a disparity be-
tween the model and the tracer puff, which can exist for a sig-
nificant length of time.  Since the amount of data available is
minuscule, it is desirable to equip the analysis with a "memory",
so that model-data differences in a certain region of the puff
are "remembered" for a short time before and after the observa-
tion time.  This may be accomplished using a quasi-Lagrangian
coordinate system, moving with a mean wind speed.  The time fil-
tering alters the analysis at a grid point, which maintains its
relative position in the puff, at times other than the observa-
tion time.  This is particularly evident in Fig. 12, where the
dotted line represents the analysis with a larger weight attach-
ed to the observational constraint when data is available.  The
effect is also present, although not so noticeable, in Fig. 11.
This effect cannot be produced in an Eulerian coordinate system,
because the puff moves through the grid points, so that a speci-
fic grid point does not retain its relative position within the
puff.

      Since transport wind speed shear is accounted for in the
model, the puff remains stationary within the Lagrangian coor-
dinate system only at the 1.5 m level.  However, because the
shear is small and the time span over which the "memory" acts is
generally short, the effect of the speed shear upon the analysis
is negligible.  Furthermore, the puff is free to move laterally
within the grid system.  This will also shift the puff centroid
with respect to the grid points.  However, the large time filter-
ing does not allow the puff centroid to shift very rapidly.
Therefore, the time filtering has the additional effect of forc-
ing the Lagrangian coordinate system to maintain its relative
position with respect to the puff centroid, and the inclusion of
observations into the analysis tend to distort the analyzed puff
from its Gaussian shape as well as dictate the position of the
puff centroid.  It is important that the puff centroid remain
reasonably stationary with respect to the coordinate system,
otherwise it will be impossible to separate the effects of dif-
fusion on the puff concentration from the effects of advection.

      Since measuring devices are located on vertical towers on
arcs of 200 and 800 m radii from the source, a cylindrical coor-
dinate system seems appropriate, because observation sites may
then be placed on grid points in an Eulerian system.  In a La-
grangian  system, however, the observations can be placed closer

                               38

-------
to grid points using a rectangular coordinate system, except
near the time the puff centroid is at an observation site.  As
the origin of the cylindrical coordinate system moves, the range
and azimuth to an observation site changes.  Therefore, distances
between grid points in the vicinity of a stationary measuring arc
are continuously changing.  At the end of the grid farthest from
the origin, the grid spacing is much larger than the distance be-
tween observation sites, while at the near end the distance is
much less than that between the sites.

      The narrow tracer puffs may be confined to 11 observation
sites on the 200 m arc.  The analysis is shown observations only
from these sites.  Since the arc from which observations are
utilized is so short, it can be approximated by a straight line.
Using a properly oriented Lagrangian cartesian coordinate system
with a grid row always located at 199 m from the source, the dis-
tance between the nearest grid point and an observation site are
much less than a meter in the y direction, and between .3 and
1.7 m in the x direction.  Therefore, observations may be assign-
ed to the nearest grid point with little loss of validity.

      In order to spread the effects of the observations and mesh
them with the concentration model, smooth spatial gradients are
required.  Therefore, spatial as well as temporal filtering must
be accomplished.  The analysis system is incorporated in the
variational functional:


             J = / Wx- X)2 + a
                 V 't
                         ,-        - 2
                    + a4(ff) + a-5(W 1 dv dt .             (46)

The functional is minimized and appropriate boundary conditions
are applied to obtain the second order linear partial differen-
tial equation
  -2 7   + -3     + ««     + «5     - «1   + "1 X -    •
     dx       dy       dz       dt

Since this Euler equation is elliptic, it may be finite-differ-
enced and solved numerically using an over-relaxation  technique.
Because the measuring devices are not equally spaced on the tow-
ers, the finite-difference scheme must take into account the non-
equal grid spacing.  The finite-differencing schemes used in this
research are reviewed in Appendix B, and the derivation and solu-
tion of the finite-difference form of (47) is discussed in Appen-
dix C.

FILTERING CHARACTERISTICS

      The filtering characteristics of (47) may be examined by

                               39

-------
defining a response function, R, where

                          R = A/A  .                          (48)

A is the amplitude of the filtered analysis, and X is the ampli-
tude of the observations.
Using
              -   -  i(kx + % + *
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-------
smaller than the large scale distribution.  This allows the anal-
ysis to conform to the observations more closely.  A comparison
of Figs. 14a-d show that as the transverse wavelength decreases
the filtered amplitude also diminishes.  This is desirable, since
the observed data shows short wave fluctuations which should be
damped to a certain extent in order to produce a smoother anal-
ysis.

BOUNDARIES

      The concentration boundaries utilized in this analysis
technique are composed of generated data.  The top and side
boundaries cause no problem, because the puff is completely con-
tained within these boundaries.  However, the temporal and bottom
boundaries have a noticeable effect upon the analysis.  The ef-
fect of the initial time boundary, computed at a travel time of
20.8 seconds, may be seen in Figs. 11 and 12.  The heavy temporal
filtering forces the analysis away from the model value, towards
the boundary value.  This is one of the reasons that further
analyses are performed at times as far from the temporal bound-
aries as possible.  The high amplitude, short period fluctuations
observed in Fig. 11 near the initial time indicates that the op-
timal azimuth obtained when the puff centroid is far from the
measuring arc may not be a good estimate of the centroids true
position.  A considerable amount of puff meander would be re-
quired to produce this effect.  This is another reason for not
using the analyses close to the boundaries.

ANALYZED CONCENTRATIONS

      The analyzed concentrations are reasonably close to those
observed during the time period of interest.  This may be seen
by a comparison of Tables 7 and 8 with 4 and 5, respectively.
However, the  azimuth of maximum concentration changes more rap-
idly in the data than in the analysis in test P5, a result of
the temporal filtering.  The analyzed concentrations are closer
to those observed in test P7.  One reason is the aximuth of max-
imum concentration changes more slowly in this case.

      The analyzed concentrations differ from the model values
in several respects.  The shape of the distributions in both the
horizontal and the vertical are very similar, but differences due
to the inclusion of observations are evident.  Fig. 15 shows the
analyzed concentration on the 1.5 m level, where most of the ob-
servations were taken, for the six central time periods in test
P5.  In each of these analyses, observations were available on
one entire grid row.  At t = 32.8 sec, the data is on the third
grid row downwind of the puff center.  At t = 44.8 sec, the data
is on the third grid row upwind of the puff center.  The grid
length is chosen such that data is assigned to consecutive grid
rows at each new time.  Since the weight assigned to data obser-
vations is much larger than that assigned to model observations,

                               45

-------
Table 7.  Analyzed concentrations for test P5 when the puff centroid
is near the 200 m measuring arc.

a. Concentrations (nCi/
'm3)at
m ; at
the 1.
, 5 m level
Azimuth (degrees)
Time
32.8
35.2
37.6
40.0
42.4
44.8
104
1
1
1
2
2
2
106
5
6
6
13
7
6
108
48
51
40
51
23
20
110
115
151
171
150
95
75
112
184
220
194
167
114
106
114
190
144
134
121
93
63
116
63
56
41
30
33
45
118
9
8
7
6
6
9
120
3
3
1
1
2
3
122
2
1
1
1
1
1
124
0
0
0
0
0
0
b.  Concentrations
                  Time
                          ) at the 114° azimuth
                                Level  (m)
                           .8     3      6.1
32.8
35.2
37.6
40.0
42.4
44.8
193
159
137
123
105
76
191
111
89
91
77
40
164
61
37
31
34
18
                              46

-------
Table 8.  Analyzed concentration for test P7 when  the  puff centroid
is near the 200 m measuring arc.

a. Concentrations (yCi/m ) at the 1.5 m level
Azimuth (degrees)
Time 104 106 108 110 112 114 116 118 120 122
56
61
66
71
76
80
b.








.8 0 0 3 35
.6 0 1 6 24
.4 1 11 22 52
.2 2 12 26 55
.0 2 7 25 59
.8 1 3 9 32
Concentrations (^Ci/m ) at

T ime . 8m
56.8 216
61.6 223
66.4 174
71.2 126
76.0 86
80.8 47
134 212 123 26 13 5
101 216 109 55 23 8
101 165 80 49 18 4
109 110 43 36 18 3
70 72 36 22 6 1
33 44 22 12 6 2
the 114° azimuth
Level
3m 6 . 1m
223 231
214 89
158 65
79 22
45 18
36 7
124
0
1
0
0
0
1









                             47

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there is a tendency to induce short waves in the analysis.  How-
ever, inspection of Figs. 15a-f shows that with the weighting
system used this effect is not very noticeable.

      Fig. 16 contains the analyses for the six central times at
the 6.1 m level.  A comparison with Fig. 15 shows the effect of
wind speed shear.  In Fig. 16 the maximum concentration is dis-
placed considerably windward.  A comparison of the two figures
further shows that the maximum concentration at the 6.1 m level
is displaced towards the right with respect to the maximum con-
centration at the 1.5 m level.  This is due to the extremely high
concentration observed at the 6.1m height on the 114° tower at
t = 32.8 sec.  Fig. 12 shows that this observation forces the
analyzed concentration to be much larger than the model concen-
tration at times later than 32.8 sec at this quasi-Lagrangian
grid point.  However, Table 4 shows that at later times the con-
centration is much lower at this observation site.  Therefore,
at positions nearer to and upwind from the puff centroid, the
concentration is much smaller, so the combined observations pro-
duce a distinct bulge in the right front quadrant of the puff.

      These analyses are consistent with the concept under which
the analysis scheme was devised:  namely, that the abrupt changes
in concentration distribution are due to a combination of meander
of the puff centroid and irregularities in the puff distribution.
Fig. 16 indicates that the analysis exhibits a distinct departure
from the Gaussian distribution, especially at the shorter travel
times.  Furthermore, the puff centroid is still allowed to mean-
der, as shown in Table 9a.  Comparison with Table 6a shows that
the meander is considerably damped by the analysis scheme, how-
ever.

      Figs. 17 and 18 show that the analyses for the six observa-
tion times closest to the time that the puff P7 centroid passes
the measuring arc, at the 1.5 and 6.1 m levels, respectively.
Note that the tracer is more nearly normally distributed in this
case.  As with puff P5, the concentration aloft is greatest for-
ward of the puff centroid.  This is demonstrated again in Ta-
ble 5.  The observed concentration at the 6.1 m level is much
larger at t = 56.8 sec than at the following times.  The combined
effect of wind shear and surface scavenging has again distorted
the puff so that its distribution is no longer Gaussian in the
vertical.

      Even though puff P7 traveled for a much longer time to
reach the 200 m measuring arc, its concentration is comparable
to that of puff P5, because the puff is diffusing more slowly in
the former case.  The puff appears to be losing mass due to more
rapid scavenging in test P7, but this is partly due to the fact
that the time interval between observations is twice as large as
in the other case.
                               51

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      The parameters optimized to fit the initial concentration
model to the analysis are shown in Table 9.  The optimal cp(t)
and A(t) in Table 9 are obtained in the same manner as those in
Table 6, except the analyzed concentrations have been utilized.
The scavenging coefficient, p, is on the same order for both
tests, but is more variable in test P7.  Since B(t) is very
small, it may be ignored.

      The analysis presented here using the indicated weights
has many desirable features.  Filtering in time produces smooth
temporal changes in concentration and tends to allow model-data
differences to be preserved for short periods of time.  The use
of larger observational weights when measured concentrations are
available forces the analysis toward the observed puff and away
from the model.  The spatial filtering reduces the amplitude of
short waves and therefore helps blend the model and data together.

      The analysis scheme is designed to yield concentration pat-
terns with the high frequency waves filtered out.  This is con-
sistent with the observations used, which were averaged over the
collection interval.  However, the analysis cannot be used di-
rectly as an estimate of the ensemble averaged concentration.

CONCENTRATION ESTIMATES

      The ensemble average concentration estimate is based on
the concentration model developed at the beginning of the sec-
tion.  The assumption that the ensemble average concentration is
approximately normal in the horizontal is reasonable since puff
irregularities are eliminated when puffs diffusing under identi-
cal conditions are averaged, due to the random nature of turbu-
lence.  In the vertical, the ensemble average concentration pro-
file will still be affected by the combined effects of wind shear
and scavenging occurring only at the surface.  As seen in Figs.
16 and 18, the positions of the concentration maxima at the 6.1 m
level change very slowly with time.  Therefore, for the six cen-
tral times in each test, the average position for the concentra-
tion maximum at each height is computed with respect to the posi-
tion of the maximum at the 1.5 m level, using  (44) with uo = 0
for the effective transport speed.  This allows for the genera-
tion of the ensemble average estimates in a true Lagrangian coor-
dinate system, since the azimuthal variation of the puff centroid
may also be eliminated using an ensemble average model.

      The quantity A(t) has already been computed using the anal-
yses and is shown in Table 9.  This represents an improved esti-
mate for use in an ensemble average over estimates given in
Table 6, since A(t) decreases with time in a reasonably smooth
manner.  However, the scavenging coefficient, p(t), which is
computed using A(t), displays a somewhat erratic nature.  There-
fore, for an ensemble average, further smoothing of A(t) may be
desirable.  Because so little is known about the nature of the

                               61

-------
Table 9.  Parameters optimized to fit an ensemble  averaged  esti-
mate to the analysis.

Travel time














cp(t)
A(t)
B(t)
P(t)

32.8
35.2
37.6
40.0
42.4
44.8

56.8
61.6
66.4
71.2
76.0
80.8
B(t)
a.
1.072
.5611
.2351
.0338
.0354
.0516
b.
.1309
.1854
.2930
.2965
.1952
.1095
A(t)
Test P5
.6168
.5855
.5608
.5438
.5163
.5017
Test P7
.7479
.6156
.5234
.4769
.4574
.4153
cp(t)

112.5
112.3
112.1
111.9
112.0
112.1

113.9
114.0
113.8
113.2
112.9
113.0
f3(t)


.0198
.0154
.0172
.0168



.0372
.0266
.0140
.0144

= optimal azimuthal angle
= coefficient obtained from least squares fit
= constant obtained from least squares fit
= scavenging coefficient
                                62

-------
scavenging in the diffusion puffs or the effect of wind shear,
further smoothing is forgone.

      In spite of a lack of knowledge concerning the precise man-
ner in which wind shear and scavenging affect an ensemble aver-
aged puff, reasonable estimates of the ensemble averaged concen-
tration may be obtained using the model described above.  The
effect of wind shear and scavenging was examined for the data
available;  Figs. 7 and 9 show that the modeling used to describe
these effects, though crude, is reasonably effective.  The assump-
tion that the ensemble averaged concentration is nearly normally
distributed in the horizontal is a good one, because of the ran-
dom nature of turbulent flows.  Puff P5 shows some displacement
in the transverse direction with height, possibly due to wind
direction shear.  However, this effect is not included in the
ensemble averaged estimate, because, on the average, wind direc-
tion shear is negligible in the atmospheric surface layer.  Con-
centration estimates obtained above will be used in the varia-
tional formalism developed in the next section.
                               63

-------
                           SECTION 6

          COMBINING FLUX AND CONCENTRATION ESTIMATES
      A variational technique has been developed to combine the
ensemble average concentration estimates and the analytical flux-
es such that the diffusion equation is satisfied.  This is not
the first variational technique to use the diffusion equation.
Wilkins (1971, 1972) developed a technique for the purpose of
optimizing objectively contoured patterns of air pollution con-
centrations.  He used the diffusion equation as a dynamical con-
straint in a numerical objective analysis technique to remove
pattern inconsistencies between successive isopleth pattern pre-
sentations.

THE VARIATIONAL FORMALISM

      The diffusion equation is used here as a strong constraint,
so it is satisfied as closely as the numerical methods allow, by
adjusting both the concentration and flux estimates.  This ap-
proach is similar to that employed by McFarland  (1975) when he
used the continuity equation to obtain dynamically consistent
wind fields.  As shown by Sasaki et al.  (1977), the proper fi-
nite-difference scheme must be used in order to satisfy the
strong constraint.

      In a Lagrangian coordinate system  the diffusion equation
may be written as
                     dF    dF    dF
                   + ^ + ^ + ;r-^+Bx = 0  •               (51)
                at
                        3y
where Fx = x'u'» Fy  - X'v'» Fz = x'w'  an<^  P  i-s defined  in  Section
2.  The fluxes and concentrations  all  represent ensemble averaged
quantities .

      The variational functional which incorporates the concen-
tration, fluxes  and  diffusion equation is
J =
      / >  (
                                    3F
V3(Fy- V2
dF
                                            0X)IdVdt .
                                                              (52)
                               64

-------
The 
                                              0  .             (57)


The derivation of the finite-difference form of  these equations,
a discussion of boundary conditions and the solution of the equa-
tions are included in Appendix D.

      The above equations may be combined to obtain a second
order elliptic partial differential equation in  X, the Lagrange
multiplier.  Once X is determined •£, Fx, Fy and  Fz may be obtain-
ed by substitution into (53)-(56).  These ^uan^ities satisfy  the
diffusion equation and are as close to •%, Fx, Fy and Fz, respec-
tively, as the weight ratios Y2/Yi» Y3/Y1 an<^ Y4/Yi allow, except
at grid points adjacent to or on the boundaries.  Therefore,  the
outermost three grid points in each spatial dimension are not
available for the final concentration analysis,  since the con-
sistent finite difference scheme for second order partial differ-
entials involves two rows of boundary values.  in Appendix D,
second order differentials of the concentration  estimate appear
in the equation for X.  Because it is desirable  to obtain good
results at the 1.5 m level, where most of the data is located,
the first three levels of the ensemble averaged  concentration
estimate are generated below the surface.  The levels at which
concentration estimates are computed are -8.1 m, -4.9 m, -1.7 m,
1.5 m, 4.7 m, 7.9 m, 11.1 m, 14.3 m, 17.5 and 20.7 m.  The grid
spacing was chosen to permit convenient computer output.  In
order to reduce the truncation error in the finite-difference
scheme, the grid intervals used here are smaller than those used
in the preceding section.  In the downwind and crosswind direc-
tions the grid intervals used are 8 and 4.8 m, respectively.

                               65

-------
ANALYSIS OF A GAUSSIAN PUFF

      To analyse the results obtained from the variational tech-
nique, two different cases are considered for test P5.  in Case 1,
•)( is generated such that it is as close to the ensemble averaged
concentration estimate as possible, except that no wind shear or
non-uniform scavenging is allowed so that the concentration dis-
tribution is Gaussian.  It was shown in Section 3 that the esti-
mated fluxes and concentrations satisfy the diffusion equation
exactly in this case.  Therefore, errors in the final analysis
will be numerical, such as truncation errors in the finite-
difference schemes.  These numerical errors are not small, al-
though they have been reduced considerably by using the smaller
grid spacing.  A measure of the finite-difference errors is the
variance of the residual of the diffusion equation (51), VR.  The
variance is .533 for test P5, Case 1.  This variance is unaccept-
able, because it indicates that the residuals are of the same
order of magnitude as the terms in the diffusion equation.  How-
ever, when the variational technique is applied the variance is
greatly reduced to .000008.  This indicates that the residuals
were reduced more than two orders of magnitude.  While this is
a satisfactory reduction in the residual, it is not reduced to
the limit of accuracy of the computer.  If the last term on the
left hand side of  (51) is omitted, then the residual is further
reduced.

      The concentrations and fluxes for the two central times
have been examined.  They are displayed for the 1.5 m level at
the 37.6 sec travel time in Figs. 19-22.  At this level the ver-
tical flux is much less than the horizontal.  However, at the
top of the puff the two are the same order of magnitude.  The
vertical concentration profile is shown in Fig. 23.  Since there
is no wind shear or non-uniform scavenging allowed in Case 1, the
concentration distribution is Gaussian in the vertical as well as
in the horizontal.

      The analysis performed above could also have been applied
to test P7.  However, as shown in Section 4, the vertical spread
of the puff in this test occurs so slowly that it violates one
of the boundary conditions which is shown in Section 3 to be
valid for a Gaussian puff.  Therefore, it makes little sense to
generate a Gaussian puff which conforms to the diffusion rates
of puff P7.

      Diffusivities may be computed from the final fluxes and
concentrations.  The averaged results for grid points where rea-
sonably large concentration  gradients exist in Case 1  are shown
in Table 10.  Note that, at  the 37.6 and 40.0 sec travel times,
the  averaged diffusivities are very close to the true  diffusivi-
ties, which are given by  (25) for  the non-sheared, uniform sca-
venging case.  This  is to be expected, since the flux  and concen-
tration estimates  satisfy  the diffusion equation exactly in this
case.
                               66

-------
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      The weight ratios are chosen so that the variance of the
diffusivities, Vx, Vy and Vz, respectively, remain at least an
order of magnitude smaller than the diffusivities, while still
forcing the final concentration to be very close to the esti-
mate.  For Case 1 we know that the diffusivities are constant in
space, so the variances should be zero.  Using the weight ratios
Y2/Y1 = .2, YS/YI = 1. and Y4/Yi = 5.9, the variances displayed
in Table 10 are sufficiently small.  The correlation between the
final and estimated concentrations is almost perfect.  Spot
checks were made to ensure that the magnitudes of the two were
also nearly identical.

      If the variance of the diffusivities is small enough, then
the fluxes obtained using the average diffusivities and final
concentrations must be highly correlated with the final fluxes.
As seen from Table 11, the correlation between the fluxes is very
high in Case 1.  This result is anticipated, since we already
knew that in this case the concept of down-gradient flux is a
good one .

      When the correlations in Table 11 are good and the vari-
ances are small in Table 10, then the fluxes are proportional to
the concentration gradients, and the constants of proportionality
are the mean diffusivities.  If the mean diffusivities are such
that (25) represents a good approximation, then the diffusivities
are the diffusion rates for the puff.  The results displayed for
Case 1, a situation where we have an a priori knowledge of the
diffusivities and fluxes, indicates that the fluxes are propor-
tional to the concentration gradients and the diffusivities are
the diffusion rates for the puff.

ANALYSIS OF PUFFS P5 AND P7
      In Case 2  (y_) is generated as described in the last section,
so that it is an estimate of the ensemble average concentration
for puffs P5 and P7.  The same type of analysis of the results of
the variational technique used in Case 1 is performed here.  How-
ever, in this case we do not have an a priori knowledge of the
results.

      The variance of the residual of the diffusion equation is
caused by finite-difference errors and possibly because the flux
and concentration estimates do not satisfy the diffusion equa-
tion exactly in  this case.  However, VR is not increased over
that obtained in Case 1, being .601 for test P5 and .106 for test
P7.  The residuals are again the same order of magnitude as the
terms in the diffusion equation.  When the variational technique
is applied, VR is again greatly reduced, to .000008 for test P5
and to  .00001 for test P7.  Therefore, the residuals are reduced
more than two orders of magnitude for both tests.

      The concentrations and fluxes have been examined for the

                               70

-------
Table 10.  Diffusivities and their variances.

Time Kx K^ Vy ky
37.6 32.6 32.8 .053 3.09
40.0 33.9 34.2 .093 3.54
37.6 32.6 32.0 1.33 3.09
40.0 33.9 33.2 2.01 3.54
66.4 11.7 10.7 1.25 2.21
71.2 12.2 11.0 1.38 2.55
A i dcr _ "";_-, * Vx*
Kx = 2 dt 'Kx - JL
A 1
-------
Table 11.  Correlation between fluxes.

Time
37.6
40.0
37.6
40.0
66.4
71.2
Cx
1.000
1.000
.9995
.9993
.9960
.9939
Cy
.9994
.9988
.9986
.9979
.9966
.9959
Cz
.9992
.9984
.9976
.9965
.9892
.9834
Case
1
1
2
2
2
2
C  = correlation between F  and K v y
 X                        X      X X


C  = correlation between F  and K v y



C  = correlation between F  and K v y
                                 72

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two central times in each test.  They are displayed for the 1.5m
level at the 37.6 and 66.4 sec travel times in Figs. 24-33.
Since the variational technique leaves the concentration virtu-
ally unchanged, Figs. 24 and 19 are nearly identical.  The down-
wind flux for puff P5, in Fig. 25, is virtually the same as the
flux in Fig. 20.  The cross-wind fluxes in Figs. 26 and 21 are
again nearly identical.  The horizontal fluxes and concentrations
also compare very well for the other travel times and levels ex-
amined.  Of course the flux and concentration patterns at higher
levels in Case 2 are displaced downwind from those in Case 1, due
to the effect of wind shear and surface scavenging.  Some deteri-
oration in the comparison of downwind flux was observed at the
highest level examined, 11.1 m, near the top of the puff.

      While the horizontal fluxes did not change much from Case 1
to Case 2, the same cannot be said for the vertical fluxes.  A
comparison of Fig. 27 with 22 shows that the maximum flux more
than doubled for Case 2 at the 1.5 m level.  Furthermore, the
pattern is completely different.  Rather than a symetric upward
flux with the maximum at the center of the grid, the maximum up-
ward flux is displaced well upwind in Case 2.  The downwind por-
tion of the puff is dominated by downward flux in this case.

      The vertical flux pattern has changed completely from Case 1
to Case 2 because the vertical concentration profile is very dif-
ferent in the two cases.  The vertical profiles for Case 2 at the
37.6 and 66.4 sec travel times are in Figs. 32 and 33.  A compari-
son of Figs. 32 and 23 shows how wind shear and surface scaveng-
ing change the vertical profile.  While the maximum concentration
remains relatively unchanged, the largest concentration in the
downwind portion of the puff in Case 2 is aloft, while in Case 1
it is at the surface.  Therefore, the concentration gradient in
the downwind portion of the puff at the 1.5 m level is directed
downward in Case 2, but upward in Case 1.  Since the flux is
down-gradient, Fz also changes direction in this portion of the
puff.  In the upwind portion of the puff, the concentration gra-
dient is larger in Case 2 at the 1.5 m level.  This accounts for
the smaller upward flux in Case 1 in this region.

      An examination of Figs. 24 and 28 shows that while the tra-
vel time for puff P7 is much longer, the concentration in this
puff is only slightly less than in puff P5, because this puff is
diffusing at a much slower rate.  This may be seen from a com-
parison of  the fluxes.  While the shape of F^ is similar in Figs.
25 and 29,  the magnitude is much larger in Fig. 25.  The magni-
tudes of Fy in Figs. 26 and 30 are closer, which accounts for
the difference in the shape of the puff.  Puff P5  is elongated
more than puff P7 because the downwind flux is relatively larger
in test P5.  The vertical fluxes in Figs. 27 and 31 have a simi-
lar pattern, because the vertical concentration profiles in Figs.
32 and 33 are very similar.
                               74

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      The mean diffusivities and the diffusivity variances for
Case 2 are given in Table 10.  The correlation between the fluxes
obtained using the average diffusivities and the final fluxes for
Case 2 are shown in Table 11.  The variances in Table 10 are low
and the correlations in Table 11 are high.  Therefore, the fluxes
are nearly proportional to the concentration gradients, and the
constants of proportionality are the mean diffusivities.  This
result could be anticipated for the horizontal fluxes, because
the ensemble average concentration maintains a near Gaussian dis-
tribution in the horizontal.  Furthermore, it has already been
shown in Section 2 that the diffusivity concept has a physical
validity for the vertical flux near the surface.  However, this
conclusion is not valid for all fluxes;  for example, it may be
shown that the heat flux can be counter-gradient in the planetary
boundary layer (Businger, 1973).

      Table 10 shows that the mean horizontal diffusivities for
Case 2 are close to the diffusivities computed using  (36).  There-
fore, Kx and Ky may be reliably estimated using the horizontal
diffusion rates for the puffs.  However, this is not true for the
vertical diffusivities.  In Case 2 Kz is consistently smaller
than Kz, and for test P7 Kz decreases with increasing travel time.
This result is not surprising since, when the puff is not Gaus-
sian, there is no physical reason why Kz should be the vertical
diffusion rate.

      The magnitude of Kz varies as the weight ratio Y4/Yi chang-
es.  If Y4/Y1 is made infinitely large, then Kz will conform to
KZ exactly, provided the concentration distribution remains un-
changed.  Since the weight ratios used are very reasonable, be-
cause the concentration is relatively unchanged, and the expected
diffusivities are obtained in Case 1, the Kz's computed for Case 2
must be reasonably accurate.  This is born out in a comparison of
the vertical diffusivities in Fig. 1 and Table 10.  An average of
the analytical diffusivities in the lowest levels compares favor-
ably with the Kz's, which may be regarded as average diffusivi-
ties over the first few meters of the surface layer.

ENSEMBLE AVERAGE CONCENTRATIONS

      The ensemble average concentrations obtained are very close
to the  analyzed concentrations.  A comparison of Fig.  24 with
Fig. 15c and Fig. 28 with Fig.  17c shows  that at the  1.5 m level,
where a majority of the data is found,  the concentration patterns
displayed agree very well.  At  levels where  the analyzed concen-
trations are not so close to a Gaussian distribution,  larger dis-
crepancies exist.

      The comparison of  the  ensemble averaged concentration and
the  data may be made in Figs.  6-9.  The ensemble average concen-
trations are at grid points which do not  coincide with the obser-
vation  sites.  In general,  grid points  are close enough  so that

                               76

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                                77

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                             78

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-------
discrepancies caused by this procedure are small.  The concentra-
tions at the 1.5 m level in Figs. 6 and 8 are very close to the
observations.  Fortunately, grid points and observation towers
coincided very well in both tests, and the vertical concentration
profiles also agreed with the data in Figs. 7 and 9.  By using
the concentration estimate described in the last section, the
final concentration is constrained to fit the data.

      The results obtained above are not affected by the use of
an average centroid position at each level.  if such an approach
were not taken, then an advection term would have to be included
in the diffusion equation, as in  (5).  However, for the wind
shear observed in tests P5 and P7, this term is an order of mag-
nitude smaller than the other terms at most levels, and may there-
fore be neglected.
                               80

-------
                           SECTION 7

                          CONCLUSIONS
      The ultimate value of the K-theory approach discussed in
the previous sections rests on the physical validity of the con-
cept of diffusivity.  Lacking this, the prediction of concentra-
tion distributions, which is the ultimate goal of K-theory, re-
duces to rather arbitrary formula-fitting.  It is evident that a
puff will be acted upon by a whole spectrum of turbulent fluctua-
tions.  Only those fluctuations which are small compared with the
existing distribution of material can be represented by the dif-
fusivity concept.  The fluctuations which are on a scale similar
to or greater than that of the puff itself will exert effects
ranging from distortion to bodily movement of the tracer distri-
bution.  Therefore, the diffusivity concept alone cannot account
for the dispersion of an individual puff released from an instan-
taneous point source.

      In light of this, the research performed has answered sev-
eral important questions, the most important being under what
conditions the diffusivity concept does have physical validity.
It is shown in Section 3 that if the diffusivity is considered
to be proportional to the product of a characteristic length and
a characteristic velocity, the physical interpretation is that
the tracer is spread over the characteristic length by the tur-
bulent eddies.  It is further shown that the diffusivities sat-
isfy the diffusion equation and a meaningful set of boundary
conditions when the puff distribution is defined by the Gaussian
model.  Therefore, the concept of the tracer fluxes being equiva-
lent to the negative of the product of the time dependent diffu-
sivity derived in Section 3 and the concentration gradient is
valid under the conditions for which the concentration has a nor-
mal distribution;  a stationary homogeneous flow in the absence
of external boundaries.  The concentration under these conditions
is the ensemble averaged concentration one would expect to ob-
serve in a non-sheared turbulent flow with uniform scavenging
near the surface.

      A second important question is whether or not the diffu-
sivity can be identified with some other physical quantity which
may be determined from easily measured atmospheric variables.  It
was shown in Section 3 that, under the described conditions, the
diffusivity is the rate of spread of the puff.  This is fortunate,
since much work has been accomplished in the determination of

                              81

-------
diffusion rates, by Lin (1960),  and Smith and Hay (1961),  for
example.  There is, of course, too little data currently avail-
able to determine if these results are directly applicable;  how-
ever, a valuable foundation for further research has been laid.

      A stationary homogeneous flow, required for a normally dis-
tributed puff, is unrealistic in the atmospheric surface layer,
and there exists an external boundary in the form of the earth's
surface.  Therefore, an ensemble averaged concentration analysis
is developed which is decidedly non-Gaussian in the vertical.  A
comparison with the data shows that the vertical concentration
profile adequately describes both the effect of wind shear and
also that of surface scavenging.  Furthermore, the near normal
ensemble averaged concentration distribution in the horizontal
is shown to conform to the available data.  Therefore, the flow
conditions implied by the ensemble averaged concentration, i.e.,
stationary, horizontally homogeneous turbulence, appear to be a
reasonable enough approximation of the true ensemble averaged
flow in the surface layer.  This is not surprising since the as-
sumptions of horizontal homogeneity and stationarity are rou-
tinely used in the study of the structure of the surface layer.

      Due to the assumption of horizontal homogeneity, the hori-
zontal diffusivity may still be identified with the rate of
spread of the puff.  Therefore,  horizontal diffusivities which
are time dependent only are likely to have the same physical
validity as in the case of a vertically homogeneous flow for the
shallow puff considered here.

      When the concentration is not normally distributed in the
vertical, equating diffusivity to the diffusion rate, as in  (25),
has little physical validity, since the vertical concentration
profile can no longer be specified by a standard deviation.
Therefore, it is not surprising that the Kz's obtained in Sec-
tion 6 do not agree with their estimates, even though a large
weight ratio  is employed for the vertical flux.  The variational
technique employed in the preceding section guarantees that the
ensemble averaged concentration and fluxes satisfy the diffusion
equation  (Eq. 51).  Since the concentration and horizontal fluxes
are shown to be close to their estimates, as expected, it may be
assumed that  the vertical fluxes are also correct.  Therefore,
the vertical  diffusivities obtained are reasonable approximations
of the average vertical diffusivities in the layer occupied by
the puff.

      Because of the good comparison between the KZ's and the
diffusivities in Fig. 1, it may be that the vertical diffusivity
is well defined by  (14).  The physical validity of this form for
the vertical  diffusivity has  already been established for a puff
released on the surface.  However, the variance of Kz is smaller
than it should be  if  (14) represents the actual diffusivity.  As
seen in Fig.  1, the diffusivity varies rapidly with height close

                               82

-------
to the surface.  Furthermore, in the neutral case the diffusivity
is less than that in the unstable case.  However, Kz was found to
be less in the unstable than in the neutral case.  Eq.  (14) does
not allow a time dependence for Kz.  It may not be necessary,
however, since the dependence upon time obtained from the  avail-
able data is ambiguous.  In test P5 Kz increased with time, while
in test P7 Kz decreased.  It is, therefore, evident that this
research did not reveal the precise nature of the vertical dif-
fusivity in the atmospheric surface layer.

      Since ambient data upon which the profiles in Fig. 1 are
based is very limited, these profiles are subject to change.  It
may be possible to obtain improved profiles by using  (14)  to
estimate vertical fluxes, employ the variational technique des-
cribed in the last section, and determine KZ at each available
level.

      The diffusivity concept appears to be valid for an ensemble
averaged tracer puff diffusing on the surface.  Furthermore, the
diffusivities can be identified with other physical quantities
which may be determined from measurable atmospheric variables.

      The diffusivities may be used to estimate fluxes, which,
together with the concentration estimates, can be employed in the
variational technique to obtain fluxes and concentrations which
satisfy the diffusion equation.  These quantities are assumed to
be the true ensemble average concentrations and fluxes.
                               83

-------
                           SECTION 8

                         BIBLIOGRAPHY
Businger, Joost A., 1973:  Turbulent transfer in the atmospheric
      surface layer.  Workshop on Micrometeorology, American
      Meteorological Society, Boston, Mass.

Gifford, F. A., Jr., 1957:  Relative atmospheric diffusion of
      smoke puffs.  J. Meteorol., 14(5), 245-251.

	, 1968:  An outline of theories of diffusion in the lower
      layers of the atmosphere.  Meteorology and Atomic Energy,
      1968, TID-24190.  Clearinghouse for Federal Scientific and
      Technical Information, 65-116.

Hildebrand, Peter H., 1977:  A radar study of turbulent diffusion
      in the lower atmosphere.  J. Appl. Meteor., 16, 493-510.

Lewellen, W. S., M. Teske, and C. duP. Donaldson, 1974:  Turbu-
      lence model of diurnal variations in the planetary bound-
      ary layer.  Proceedings of the 1974 Heat Transfer and Fluid
      Mechanics Institute.  Stanford University Press.

Linn, C. C., I960:  On a theory of dispersion by continuous move-
      ments.  Proc. Natl. Acad. Sci., 46, 566-570.

        and W. H. Reid, 1963:  Turbulent flow, theoretical aspects,
      Handbuch der Physik, 8, Part 2, 438-523, Springer-Verlag,
      Berlin.

McFarland, M. J., 1975:  Variational optimization analysis of
      temperature and moisture  in a severe storm environment.
      Ph.D. Dissertation, University of Oklahoma, Dept. of Meteo-
      rology, Norman.

Mood, A. M.,  and F. A. Graybill, 1963:  Introduction  to the Theory
      of Statistics.  McGraw-Hill, New York.

Nickola, P. W.,  1971:  Measurement of the movement, concentration
      and dimension of clouds resulting from  instantaneous point
      sources.   J. Appl. Meteor., 10, 962-973.

	, j. v. Ramsdell, Jr., and J. D. Ludwick, 1970a:  An inert
      gas tracer system for monitoring the real time  history of
      a diffusing plume or puff.  J. Appl. Meteor., £, 621-626.

                               84

-------
	, 1970b:  Detailed Time - Histories of Concentrations Re-
      sulting From puff and Short Period Releases of an Inert
      Radioactive Gas;  A Volume of Atmospheric Diffusion Data,
      BNWL - 1272.  National Technical Information Service.

Pasquill, F., 1970:  Prediction of diffusion over an urban area-
      current practice and future prospects.  Proceedings of
      Symposium On Multiple-Source Urban Diffusion Models, Air
      Pollution Controle Office Publication, AP-86, Sec. 3.

	, 1974:  Atmospheric Diffusion.  John Wiley and Sons, New
      York.

Richardson, L. F.,  1926:  Atmospheric diffusion shown on  a dis-
      tance-neighbor  graph.  Proc. Roy. Soc.  (London), AllO,
      709-737.

Roberts, J. J., E.  S. Croke, and A. S. Kennedy, 1970:  An urban
      atmospheric dispersion model.  Proceedings of Symposium on
      Multiple-Source Urban Diffusion Models, Air Pollution Con-
      trol Office Publication, AP-86, Sec 6.

Roberts, 0. F. T.,  1923:  The theoretical scattering of smoke in
      a  turbulent atmosphere.  Proc. Roy. Soc.  (London),  A104,
      640-654.

Sasaki,  Y., 1970a:  Some basic formalisms in  numerical varia-
      tional  analysis.  Mon. Wea. Rev., 98, 875-883.

	,  1970b:  Numerical variational analysis  formulated under
      the  constraints as determined by longwave equations and
      low-pass filter.  Mon. Wea. Rev., 98, 884-898.

	,  1970c:  Numerical variational analysis with weak  con-
      straint and application to surface analysis of severe storm
      gusts.  Mon.  Wea. Rev., 98, 899-910.

	,  P. S.  Ray,  J. S. Goerss, and p. Soliz (1977):  Errors due
      to inconsistency  of finite difference schemes.  Submitted
      to Monthly Weather Review.

Smith, F.  B.,  and J.  S. Hay, 1961:  The expansion of clusters of
      particles in  the  atmosphere.  Quart. J. R. Met. Soc., 87,
      82-101.

Sutton,  O. G., 1953:  Micrometeorology.  McGraw-Hill, New York.

Taylor,  G. I., 1921:  Diffusion by continuous movements.  Proc.
      London  Math.  Soc.,  (2) 20, 196-202.

Tennekes,  H.,  and J.  L. Lumley, 1972:  A First  Course In  Turbu-
      lence.   The MIT Press, Cambridge, Mass.

                               85

-------
Van der Hoven, I., 1968:  Deposition of particles and gases.
      Meteorology and Atomic Energy, 1968, TID-24190.  Clearing-
      house for Federal Scientific and Technical Information,
      65-116.

Wilkins, E. M., 1971:  Variational principle applied to numerical
      objective analysis of urban air pollution distributions.
      J. Appl. Meteor., 10, 974-981.

	, 1972:  Variationally optimized numerical analysis equa-
      tions for urban air pollution monitoring networks.  J. Appl.
      Meteor., 11, 1334-1341.

Wyngaard, John C., 1973:  On surface layer turbulence.  Workshop
      on Micrometeorology.  American Meteorological Society,
      Boston.

Yeh,Gour-Tsyh and Chin-Hua Huang, 1975:  Three dimensional air
      pollutant modeling in the lower atmosphere.  Boundary-Layer
      Meteorology, 9, 381-390.
                               86

-------
                          APPENDIX A

         DERIVATION OF THE EXPRESSION FOR DIFFUSIVITY


      The derivation of the expression for diffusivity,
is shown in order to reveal the nature of the relevant  character-
istic length and eddy velocity.  Mixing length theory could be
used to define the diffusivity.  However, as Pasquill  (1974)
points out, there is a considerable element of vagueness  in the
whole idea of a mixing length.  Therefore, this approach  is not
used since it does not contribute to a clear understanding of the
characteristic length and velocity.

      It is well known (e.g., Pasquill, 1974) that, based on di-
mensional grounds, the diffusivity may be determined by the pro-
duct of a characteristic eddy velocity and a characteristic
length scale.  Since, as shown in Section 3, the diffusivity is
proportional to the perturbation velocity variance at distances
far from the source, it is assumed that the characteristic ve-
locity is the standard deviation of the velocity perturbation.

      Pasquill (1974) states that only those eddies of  a  size
similar to or less than that of the puff are effective  in dif-
fusing it.  It is therefore assumed that the characteristic
length in the downwind direction, lc, is related to ax.   Since
Ox grows indefinitely, but lc's growth may be limited by  the size
of the largest eddies diffusing the puff, the relationship be-
tween lc and ax is taken to be

                        lc = C(t) ox .                      (A.2)

At long travel times C(t) must decrease so that 1  remains con-
stant.

      Since the diffusivity may be determined by the product of
the characteristic length and velocity,

                               ?  ? ^
                        	 /"iTi-i1**"!^                       / •* i \
                      x - C]_LU   axJ  ,                     (A.3)
                              87

-------
where GI is a time dependent proportionality parameter.  The pro-
duct may be replaced by the covariance of £x and u', £xu', since
the correlation between these quantities may be defined as


                                                             (A.4)
When tracer puffs are released many times under identical condi-
tions, and ensemble average concentrations are obtained, the re-
sulting distribution of particles must be identical to the con-
centration distribution.  Therefore, the variance of £x is equi-
valent to the variance of the concentration as
Substitution of  (A. 4) and  (A. 5) into  (A. 3) yields
                        Kx = C3 Axu'  ,                       (A. 6)
where C3 = C1/C2-
      The relationship between &x and u1 must now be examined,
in order to express the diffusivity in terms of measurable quan
tities.  Using the fact that the usual laws of differentiation
may be applied to the mean values of fluctuating variables and
their products,
      It may be seen from a comparison of Figs. 2 and 3 that
x'(tf) ^ £x.  However, the position of the puff centroid with re-
spect to the abscissa, a, does not change as rapidly as the posi-
tion of an  individual particle does.  Therefore, the time rate  of
change of a particle's position with  respect to the puff centroid,
C,  is nearly equivalent  to its rate of change with respect to the
coordinate  system, or

                      dx'   d<£x  + a>    d*x
                       d~t~      dt        at   '                  >

At  short travel  times  the puff  is  small  and  the approximation  is
not a  good  one since the  location  of  the puff centroid changes
rapidly as  large eddies transport  the entire puff.  However, as
the puff becomes larger at longer  travel times the eddies  tend to
diffuse rather than transport the  puff and the approximation be-
comes  better.  Therefore, at longer travel times,


                               88

-------
                           u1 - d* /dt .                     (A.9)
In those cases where  (A.9) is valid  (A.7) becomes


                         	   , ^l
                          V1' = 2 dt- '                     (A-10)

if (A.5) also is used.

      The diffusivity may be related to the rate of spread  of
the puff by substituting  (A.10) into (A.6), to obtain


                             C3 dax
                        Kx = iTdt--                       

                             bl
Using the definition a  = a,t   the diffusivity becomes
                      3t    -L

                            2     ^l'1
                     Kx = ax b-jCgt      .                   (A. 12)


The constant 03 may be evaluated by equating  (A.12) with  (12)
when b~L = 1/2, the condition under which  (12) is valid, to  obtain
C3 = 1.  Therefore,  (A.11) is equivalent to  (A.I), so that, ex-
cept close to the source, the diffusivity expressed by  (A.I) is
in fact proportional to the product of the assumed characteris-
tic eddy velocity and characteristic length scale.  When  the as-
sumption (A.8) is valid, the characteristic velocity is the stan-
dard deviation of the velocity perturbation,  and the character-
istic length scale is shown in (A.2).  The product of the pro-
portionality parameter and C(t), Cl, is equivalent to the cor-
relation coefficient, C2.  Therefore, the diffusivity may be
uniquely determined from Vu1 , 0X and C2-
                               89

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                          APPENDIX  B

             CENTERED FINITE DIFFERENCE ALGORITHMS


      The form of the finite-difference algorithm for non-equally
spaced grid intervals may be obtained  from a  Taylor series expan-
sion.  Let P represent any dependent variable,  while i,  j, k and
£ are the grid indicies  along the x, y, z  and t axes,  respective-
ly.  For derivative evaluation at i, j, k  or  &,  only those sub-
scripts different from i, j, k, or  H are identified.

      Taylor series expansions to approximate P]^_i  and P]^+^ are


                                  (Z -   -*2
      P    = P -
       k-l     -   -  k-l   z         2!            --•-

and                                         9

                                  (zk+l -  Z)
      Pk+l = P +(zk+l -  Z>  *zP + - 21 -  7zzP + •••
Neglecting higher  order terms  (resulting in a truncation error) ,
(B.I) and  (B.2) may be solved  for vzP.   After some manipulation,

                 " z               z ~ zk-l
                  -  


-------
                                + P    - 2P
                                   "U--1
                                      '
Similar results may be obtained in the x, y and t  axes.   in Ap-
pendix C, algorithm  (B.6) is used on the z axis, since the grid
intervals here are non-equally spaced, and the equivalents of
algorithm (B.7) are used for the other axes.

      Significant errors can arise in numerical computations
when a set of differential equations is written in an inconsist-
ent finite-difference form (Sasaki et al. , 1977) .  The inconsist-
ent form, exemplified by using (B.5) and (B.7) together,  results
in a lack of satisfaction of the governing equations which may
be equal to that obtained when the variational technique  is not
employed.  A finite difference analog of the  second derivative
operator of the form
                                       - 2P + P
                 VZ(V P) = 7  P = -   - 5 - —  '         
-------
                          APPENDIX C

         NUMERICAL SOLUTION OF THE ANALYSIS FUNCTIONAL


      The variational functional in Section 5 may be written  in
finite-difference form as

                          2          2          2
        J =  T  Ca^x - x)  + a2(v X)  + 
-------
Since the Euler  equation  is  elliptic,  it may be solved using a
relaxation  algorithm.   Substituting the finite-difference analogs
(B.6) and the equivalents of (B.7)  into (C.4)  and rearranging
yields
            cc^       a-D     oc-3    ao     a^     ct-i
      __, p «^  ^        j    iii        i    ")  ~"

               7    (AY)2   Zl    Z2    (At)2   2


                 / ^     • "~   \      *^   / ~™      ™~   \
                                     2
                                 (Ayr
                                     2
                                 (At)
        + ttl\] = R   »                                        (C.5)

where zl ==  (zk+1 -  z)(z  -  z^.j^)  + (zk+1 - z) 2

and   z2 =  (z - z]c_1) 2 + (z]c+1  - z) (z - z]c_1) .

The over-relaxation  factor F  is  predetermined to speed the re-
laxation process.   The residual  Rv at the v-th iteration indicates
that the ^'s do not  satisfy  (C.5)  exactly on that iteration.  On
the succeeding iterations  the residual may be reduced by choosing
a more appropriate  ^, such that

   -v+1   -v           _      Rv          __        ._ ,..
   v    = v  + - .      (C-6)
   ^      *•
                  (Ax)     (Ay)          Z  (At)

This recursion equation may be  iterated until the residuals at
all grid points are  less  than some  arbitrary value.  The root-
mean-square  (R.M.S.) of the residual is a measure of the relaxa-
tion procedure's  success  in obtaining a solution to the partial
differential equation.  For test P7 the R.M.S. was reduced from
79.94 to .01477 in 18  iterations, while in test P5 it was reduced
from 1709 to .006688 in 2,4 iterations.
                               93

-------
                           APPENDIX D

        NUMERICAL  SOLUTION OF  THE FUNCTIONAL COMBINING

               FLUX AND  CONCENTRATION ESTIMATES
      The finite-difference  form of the variational functional
in Section 6  is

                              2            A   2
                       V   +  Y4(FZ  - Fz>

                       7 F   +VF  + tf F  +
                       V V    \T \7     <7 *7
                       x. x    y y     z z

The observational weights yi» Y2' YS  an<3 Y4 are prespecified con-
stants in this case.   The Lagrange  multiplier,  X, is one of the
dependent variables.

      As in Appendix C, the stationary value of the functional
is found by equating the first variation  to 0.   Therefore,


     6J = 0 =  E   {2Yl(x -  §

  §1!
  «•%*'*• fl»
2*a*

*Ii?
3 5 58'
n ** ^
«.  O tt 

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      5-
          3-
          a
          8-
          <«
                                        t)
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                                        rn
                                               m
                                               C
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                                             O rn


                                             S' <
                                             0) 33
                                         O § o

                                         S §2?
                                               0) W Q)

                                               — « 2
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                                                   o m
3S
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s i
                                             *
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                                           en

                                           m
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                                           <

                                           X %
                                           o o
                                           z to
                                           2 ^
                                           <" «
                                           Z 2
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                                           > >
                                               U
                                               u
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