BACK-SCATTERING AND SELF-ABSORPTION O F @--PARTICLES1

M. S. LXFLEUR
Radiochemistry Laboratory, Department of Chemistry, McGill University, Montreal, Que.
AND

S. KAHANA
AND T . F. MORRIS
Department of Physics, McGill University, Montreal, Que.
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AND

L. YAFFE
Radiochemistry Laboratory, Department of Chemistry, McGill University, Montreal, Que.
Received January 21, 1963

ABSTRACT
The self-absorption of the p--radiation from S3j and P32 has been studied in various com-
pounds. T h e function derived by Gora and Hickey has been shown to fit the data. The
back-scattering of the p--radiation from Pa2 by various elements and compounds has been
examined and a semiempirical treatment used to suggest a n effective atomic number for
back-scattering by compounds.

INTRODUCTION
Can. J. Chem. 1963.41:2283-2293.

There have been many experimental studies dealing with the phenomenon of scattering
and absorption of P--radiation in counters of various geometrical efficiencies. These have
been made t o try to describe these processes adequately and to use the data obtained to
transform measured counting rates into accurately known disintegration rates.
The theoretical description of scattering and absorption of P--radiation is difficult
because of the continuous distribution of ,&-particle energies and the complexity of the
scattering process. I t is known that, when p--particles interact with matter, they are
scattered by elastic collision with atomic nuclei and lose energy by inelastic collision with
atomic electrons. Absorption is due to the combined effects of scattering and energy loss.
In this paper we have studied the probleills of sekf-absorption and back-scattering with
counters of geometrical efficiencies of 2a steradians and less.
( a ) Self-absorption
Self-absorption, the absorption of radiation in the material of the source itself, is the
limiting factor in accurate disintegration-rate determinations where the sample is mounted
in solid form. The absorption of @--radiation is described approximately by the exponen-
tial law

where A is the activity observed when radiation from a source of activity A. has passed
through material of thickness x cm. The absorption coefficient, p, in cm-l, can be related
~ ,the absorber and the end-point energy E oof the p--emitter
to the density, d, in mg ~ m - of
by equations of which the following (1) is typical:

Many self-absorption relations have been based on the approximate exponential

' T h i s work received financial assistance from the National Research Council of Canada.
Canadian Journal of Chemistry. Volume 41 (1963)

2283
 2284 CANADIAN JOURNAL O F CHEMISTRY. VOL. 41, 1963

absorption as shown in equation [ I ] . The general approach has been to consider the absorp-
tion of radiation emitted from a point in the source, then to sum up the contribution from
all possible points. Early self-absorption studies (2-6) were made with counters of very
low geometrical efficiency. The electrons were assumed to travel normal to the source
and the problem was reduced to a one-dimensional type. Equation [I] was integrated
over the sample thickness from x = 0 to x = a and the following relation obtained:
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I t was pointed out ( 6 , 7) that, for thin samples of superficial density less than 1 mg/cm2,
self-scattering is a very important factor. In subsequent publications (8-10) equations
were derived which took this effect into account.
Objections to the simple self-absorption relation expressed in equation [3] were also
raised as self-absorption was studied with counters subtending larger solid angles. Elliot
and co-workers (11-14) showed that, from very thin layers, radiation is emitted iso-
tropically, while from thicker layers the intensity observed a t an angle 0 to the normal
approaches a cos 0 relationship.
According to these results, the activity observed a t an angle 0 is written
Can. J. Chem. 1963.41:2283-2293.

which reduces to the experimental cosine distribution a t large values of a.

Gora and Hickey (15) measured self-absorption in a flow-type counter. They assumed
-isotropic distribution and integrated both over sample thickness from x = 0 to x = a and
over the angles from 0 = 0 to 0 = a / 2 to obtain

E i ( - ~ a ) is the exponential integral of ( - ~ a ) .Gora and Hickey found that the simple
relation described by equation [3] held only if the value of p was varied with the geo-
metrical efficiency of the counter.
Roalsvig and Haslam (16) later derived a similar equation. They irradiated disks of
Cu, Zn, Ni, Mo, and polystyrene of thicknesses ranging from ten to several hundred
milligrams per square centimetre. They found that equation [4]fitted their experimental
results very well for ~ / = d 0.0119E0-~.~~.
Hendler (17) studied the self-absorption of C14 and found that a hyperbolic function
described the situation over the range of investigation. Katz (18) then showed that the
hyperbolic function did not fit his data and Massini (19) pointed out that possibly the
effect of the counting arrangement used by Hendler led to the hyperbolic function.
Self-absorption in counters of geometrical efficiencies of 2a steradians and less still poses
many problems. (The problem of self-absorption in a 4 a counting geometry has been
intensively investigated by Yaffe and co-workers (20, 21) and Campion and co-workers
(22-25).) Most experimental work has concerned itself with the study of self-absorption of
a particular p--emitting nuclide in source material of a particular composition. In the
present work the composition of the source, the energy of the p--emitter, and the geo-
metrical efficiency of the counter have all been varied.
( b ) Back-scattering
The main features of back-scattering observed in counters of less than 2a geometry
 LAFLEUR ET AL.: BACK-SCATTERING A N D SELF-ABSORPTION 2285

have been well examined (26,27) so that the effects of varying the energy of the 0--emitter,
the atomic number, and mass thickness of the back-scatterer are known.
An important experimental fact about back-scattering is that the extent of back-
scattering increases with the thickness of the backing material to a fixed value. The fixed
value defines a condition termed 'saturation back-scattering'. For elements, the saturation
back-scattering is a function of atomic number. For compounds, it has been suggested
that the saturation back-scattering value obtained might characterize an 'effective' atomic
number.
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Various experimenters have defined an 'atomic number' for compounds purely empiri-
cally t o suit their particular experimental data.
Glendenin and Solomon (28) proposed an average atomic number 2 to explain their
back-scattering results:

where Z1. . . Z, are the atomic numbers of the various elements in the compound and
N1 . . . Nn are the numbers of atoms of each in the formula.
Perlman and Friedlander (29) used another definition of an average atomic number
for their self-absorption studies:
Can. J. Chem. 1963.41:2283-2293.

where A , is the atomic weight of the element defined by atomic number 2 , . This is the
form these authors use, although it is referred to as 2 i in their paper.
Saldick and Allen (30), in studying the oxidation of ferrous sulphate in acid solution
by high-energy cathode rays, suggested an effective atomic number,yZE:

[51 2, = C I
[(electron density) ZJ.

Their formula is a special case of the more general formula of Henriksen and Baarli (31):
gEI= [(electron density) z:]"~.
z

hliiller (32) defined an empirical effective atomic number, ZE2, to explain his data for the
back-scattering of 0--radiation by compounds :
Z,,= C [(weight fraction) iZi]
Z

where the effective atomic number is the sum of each atomic number multiplied by the
weight fraction of that atom present in the compound.
Danguy and Quivy (33) studied the back-scattering of electrons by solutions and alloys
and found that their results could be fitted by Muller's effective atomic number.
Gray et al. (34) calculated effective atomic nunlbers according to equations [5], [6], and
[7], and correlation was completed with observed back-scatter intensities. Muller's
effective atomic number (equation [7]) showed the poorest correlation, with marked
 2286 CANADIAN JOURNAL O F CHEMISTRY. VOL. 41, 1963

scatter on the points. The results using equation [ 5 ] were much better. The best results
were obtained using equation [6] for effective atomic number with a value of x = 0.93.
In this paper the back-scattering due t o compounds has been investigated in order to
check the various formulations with regard to effective atomic number.

EXPERIMENTAL
( a ) Self-absorption
Two p--emitters were studied, S35 (Eo= 0.167 Mev) and PS2 (1.71 Mev). T h e self-absorption of the
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p--radiation was measured by varying the composition of the sources and varying the solid angle subtended
by the counter a t the sources.
Sources containing P3=were prepared by precipitating the orthophosphates of Ca, Cu, Ba, and P b from a
stock solution of orthophosphoric acid containing a fixed ratio of the active PZ2 to the inactive P3l isotope.
Similarly, sources containing S35were prepared by precipitating the sulphates of Ba, Sr, and P b from a stock
solution of sulphuric acid containing a fixed ratio of S35 to inactive sulphur isotopes. Aliquots of varying
size of the precipitated salts (orthophosphate or sulphate) in slurry form were transferred to aluminum
planchettes of standard dimensions. T o ensure uniform distribution over the area of the planchette, the slurry
was stirred before evaporation to dryness. Acetone was found to be a convenient slurrying agent for the
unhydrated salts, while water was used for the hydrated salts.
Sources of varying thicknesses and constant area were thus prepared and weighed. The superficial density
of the sources ranged from 0.05 to 35.0 mg/cm2. The activity of the sources was measured with a 27r pro-
portional counter and it1 two positions below a n end-window gas-flow proportional counter. This gave results
it1 geometrical efficiencies of 470, 20%, and 50%. The aluminum planchettes, used as source mounts, were
of sufficient thickness to ensure saturation back-scattering from the aluminum for all sources.
Can. J. Chem. 1963.41:2283-2293.

( b ) Back-scattering
Inorganic compounds were used as baclting material in powder form. The powder, finely ground, was
contained in cylindrical metal boxes of sufficient depth t o ensure saturation back-scattering.
Elements were also used as backing material to provide a standard curve of back-scattering vs. atomic
_number. T h e elements Mere in either foil or powder form.
The high-energy p--emitter, P32,was used as source material. T o obtaiu a point source, 100 microliters of
P32 solution of high specific activity was pipetted on to VYKS film and allowed to evaporate. The VYKS
film, of superficial density 10 pg/cm" was then placed over the circular hole of a n aluminum tray designed
t o fit as a shelf in the end-window counter. The backing material was cemented into position closely behind
the source. Care was taken in all cases to keep the distance from the source to the backing constant. The
activity of the samples mas measured by the end-window counter in a geometrical efficiency of 20%.

RESULTS
( a ) Self-absorption
Experimental self-absorption curves were obtained in the conventional manner by
plotting the logarithm of the 'apparent' specific activity (measured activity per milligram
of compound) versus the superficial density (mg/crn2). The results of measurements in
geometrical efficiencies of 5O%, 20%, and 4% were normalized to the 50% position and
were found to be superimposable.
In Fig. 1 is shown the self-absorption results for the phosphate sources. The points
represent the experimental data. The difference in the self-absorption of the betas of P32
in phosphates of various densities is clearly shown. In Fig. 2 the self-absorption data for
the sulphate sources are shown. Again the effect of density is clearly evident for the various
sulphate sources.
The data have been fitted to the Gora and Hickey (15) function for a value of pa =
0 . 022daEo-I 33 (equation [2]). In Figs. 1 and 2 the solid lines represent the curves thus cal-
culated. The agreement between the experimental and calculated results is very good for
all the data. The error in each experimental point is estimated to be f 5 % . This includes
non-uniformity of samples, statistical fluctuations in activity measurements, and weighing
of samples. No correction has been made for the back-scattered radiation. The back-
scatterer was the same for all sources, and the effect due to it was treated as a constant.
 LAFLEUR ET AL.: BACK-SCATTERING AND SELF-ABSORPTION
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Can. J. Chem. 1963.41:2283-2293.

SUPERFICIAL DENSITY (MG/CM- I

FIG. 1. Self-absorption of P32by various phosphates.

FIG. 2 . Self-absorption of S35by various sulphates.

A further test of this function has been made by Meghir (35),* who studied the self-
absorption of Cll in barium carbonate in a 4n counter which is essentially two 2~ counters.
The results are shown in Fig. 3. The triangles represent the self-absorption data for Cll in

FIG. 3. Test of Gora and Hickey function: A Cn in BaC03. The triangles represent the data obtained
by Meghir (35). The solid line represents the curve obtained from the self-absorption expression. 0 Self-
absorption of C" in polystyrene (36). The solid curve was obtained by Meghir using the appropriate density
corrections.

* W e are grateful to Dr. 3.Meghiv of this laboratory for k i n d l y allowing u s to use his results.
 2288 CANADIAN JOURNAL O F CHEMISTRY. VOL. 41, 1963

barium carbonate. The solid curve (A) is again obtained from the Gora and Hickey
function. Crandall et al. (36) studied the self-absorption of C" in polystyrene. Their data
are shown by open circles, and Meghir obtained the curve (B) shown by use of the above
function with the appropriate density correction.
Back-scattering
The effective atomic number, ZE1,of each compound used was calculated from equation
[6] with x = 1. The empirical effective atomic number, ZEZ,of Miiller (equation [7]) was
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also calculated. The materials used as back-scatterers and their 'atomic numbers' are
given in Table I. I t is seen that the two formulae for effective Z give virtually the same

TABLE I
Effective atomic number of elements and compounds used as back-scatterers

Back-scatterer ZE~ ZE2 (1 Back-scatterer ZE, ZI32

.-
NaF 10.10
Mg 12.00
KCK 13.94
CaO 16.57
Can. J. Chem. 1963.41:2283-2293.

KC1 18.06

result for low 'atomic numbers'. However, a t high 'atomic numbers' there is a significant
difference.
In Fig. 4 saturation back-scattering is plotted versus ZE,. I t is seen that a smooth curve
may be drawn through all the points representing both elements and compounds. In Fig. 5
saturation back-scattering is plotted versus Miiller's ZE2.A smooth curve may be drawn
through the points representing elements and the points representing compounds of low
'atomic number'. The points representing compounds of high 'atomic number' fall below
the curve.
We were not able to reproduce the points of inflection found by Miiller corresponding
t o atomic numbers of the rare gas configurations. Indeed, it seemed possible to redraw
the Miiller data without these points of inflection, especially since the rare gases were not
used as back-scatterers in his experiments.
I t is possible from a crude one-dimensional model* to suggest an 'effective atomic
number' for back-scattering by compounds. This is shown in Fig. 6. The 0-source is
located a t x = 0 on the x-axis. The activity of the source is 2ao. I t is assumed that the
shape of the P-spectrum and the angular distribution pattern of the 0-radiation are vir-
tually unchanged by passage through and absorption in the source. The absorption is
assumed t o be nearly exponential.
In Fig. 6(A), when there is no reflector, the measured activity is ao, as only the activity
in the negative direction reaches the counter. When there is a reflector, as in Fig. 6(B),
the measured activity is the sum of the activity emitted in the negative direction plus
the activity reflected back from the positive direction, i.e. a o f bo. The reflector is imagined
t o be infinite in length in order to describe the case of saturation back-scattering.
R, the reflection coefficient, is equal to the product of the number of scatterers and the
cross section for back-scattering. For elements of low atomic number the screening of the
*A somewhat similar treatment has been given by G. L. Brownell (Preliminary Report No. 8, Nuclear Science
Series, National Research Council, Washington, 1950), but to the authors' knowledge never published elsewhere.
 LAFLEUR ET AL.: BACK-SCATTERING AND SELF-ABSORPTION
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Can. J. Chem. 1963.41:2283-2293.

f D ELEMENTS

FIG. 4. Effective atomic number for saturation back-scattering using formula of Henriksen and Baarli
(31).
FIG. 5. Effective atomic number for saturation back-scattering using formula of Miiller (32).

nucleus can be ignored, Rutherford scattering applies, and

R = NZ2,
where Z = nuclear charge and N = number of nuclei per unit length.
Let ~ d xrepresent the fractional number of electrons that fall below the detection
threshold in the length dx. The loss coefficient, E, will depend principally on small angle
scattering by the electrons and thus, for elements,
E = NZ.
If one considers a point, x, in the one-dimensional reflector, the number of beta particles
moving in the positive direction is
a(x) = aoe-p2
 CANADIAN JOURNAL O F CHEMISTRY. VOL. 41, lYG3

(Al (0)
(3 -SOURCE p- SOURCE WITH REFLECTOR

- - 8

COUNTER4 : COUNTER + 7

SOURCE' 0 iFO +0 bo
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+: +I,
X-AXIS X-AXIS

FIG. 6. One-dimensional representation of back-scattering.

and the number moving in the negative direction is

b(x) = boe-pz.
Can. J. Chem. 1963.41:2283-2293.

T o determine b(x) in terms of a ( x ) , one considers the number of beta particles moving in
the positive direction a t a distance dx from x. Then a(x+dx) will be the sum of the number
transmitted from x and the number reflected from x.

-paoe-Pz = - (R+e)aoe-'"+ Rb ( x )
and

T o find p in terms of R and E, one considers the number of beta particles moving in the
negative direction a t x-dx.
b(x-dx) = b ( x ) - (R+e)b(x)dx+Ra(x)dx

- db
- = -(R+~)b(x)+Ra(x).
dx
Then

and
p = ~/[(R+E)'-R~].
Hence b(x) may be expressed
 LAFLEUR ET AL.: BACK-SCATTERING A N D SELF-ABSORPTIOS

The efficiency of reflection, q, is then

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The percentage back-scattering is given by the efficiency

Therefore back-scattering depends on the ratio E/R.This suggests an effective Z for com-
pounds. For a compound, the reflection coefficient is given by

where N 1 .. . N, represent the particle densities and Z1. . . Z, the atomic numbers of
Can. J. Chem. 1963.41:2283-2293.

elements 1 . . . n.
The loss coefficient is given by

Therefore

This indicates an effective Z as given in equation [6]:

The reflection coefficient may be written

where y is some constant of proportionality. Let S = 1 + Y/ZE1, then

Therefore S = (l+q2)/2q and

The plot of ZE1should yield a straight line.

In Fig. 7, curve (A) shows a plot of q/(1 -q)2 VS. ZEl. However, for ZE1 > 60, the results
are anomalously high. For high values of Z the inner shells will screen the nucleus and
 CANADIAN JOURNAL O F CHEMISTRY. VOL. 41. 1963
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FIG. 7. (A) Plot of q/(1 -q)2 vs. Z E ~(B)

. Plot of q/(1 -q)2 vs. q.

reduce the effective value of Z2 in R. Only the loosely bound electrons will contribute to
Can. J. Chem. 1963.41:2283-2293.

E and hence the value of Z in E is reduced as well. The first effect will tend to reduce the
reflection coefficient, the second to increase it. In curve (B) of Fig. 7 it is seen that the ratio
q/(l- q ) 2 increases for high q, indicating that the second effect is the more important.

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