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SELF-ABSORPTION IN SOURCES PREPARED FOR

4% BETA COUNTING1

Using the 4 r o - y coincidence method the self-absorption of 47rB counting sources prepdred
by a number of source techniques has been n~easuredfor the negatron emitters
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Csl34 (86-kev branch only), Nb", MgZ0',CoGO, ScdG,RbsG,A L I ~Nazi,


~ ~ ,and the positron branch
of CUG'. T h e self-absorption varied from a few tenths of one per cent to about ten per cent
for sources with a mean supcrfcial density of 2 ~ g / c r nfor
~ most of the n ~ ~ c l i d st~~cliecl.
es Sub-
sidiary experiments were carried out to indicate the variation of self-absorption with source
superficial density.

'The comparative simplicity of l a p counting has lecl to its general use for absolute
disintegration rate measurements. I t is \\?ell known that the chief corrections are those
required for absorption in the source and mount. The latter has been extel~sivelydis-
cussed (1, 2, 3) and is small for all but the softest beta emitters if thin source ~llounts
:Ire used. Self-absorption cannot be so readily determined, and this is the principal
uncertainty in -lap counting. I-Ialvkings ct al. (-1) progressively diluted a stock solution,
and observed the activity (expressed in terms of the original solution) as a functioli
For personal use only.

of the dilution factor. .9t sufficiently high clilutions a constant activity was observecl,
~vhichwas taken to indicate that self-absorption had been eliminated. 'This procedure
has been criticized (3) on the grouncls that diluting a stock solution may not decrease
the size of the crystals forming a11 active cleposit but merely increase the distance between
them. Pate and Yaffe (5) have clescribed a distillation technique for preparing unifori~~ly
thin sources ancl have used this ~uethod to set up self-absorption curves for several
isotopes (6). Seliger and Sch\vebel (7) have estimated the self-absorptiol~of a rlumber
of isotopes from electron ~nicroscope lueasurements of the crystal sizes. T h e lap-y
coincidence methocl has been used by Gunnink ct al. (8) to study self-absorptio~lin thin
sources prepared by conventio~~al techniques. A s s u m i ~ ~that
g the observed inefficiencies
are entirely due to self-absorption they have obtained a curve of per cent loss in 4a
counting against maximum beta particle energy. These authors are careful to poi11t out
that these losses are "best" averages, and that the value for any one source may deviate
considerably from the n ~ e a n .
In this laboratory a lap-y coincide~~ce counting system consisting of a l a p propor-
tional counter sancl\viched between two 3 in. X 3 in. sodium iodide crystals (9) has
been used to ii~vestigatethe relative merits of various source preparation techniques. T h e
results of six such techniques appliecl to sevel-a1 isotopes of widely differing maxiinurn
beta particle energy are reported here.
13XPERI MENTAL
In their simplest fornz the ecluations relating the observed counting rates in a coinci-
clence determination to the absolute disintegration rate, N o , are:

'.\Ianuscr~pt rccecvcd AIarclz 11, 1!15!1.


ConLribziLio~tfrom the Physics Division, .4la?11icEnergy of Canada Linl~Led,Chalk Kivrr, OnLarin.
Issued ns .4 .E. C.L. No. 796.
Can. J. Chem. \id. 37 (1059)
1110 CANADIAN JOURNAL O F CHEIMISTRY. VOL. 37, 1959

where iVa, N,, and N, are the observed rates in the beta, gamma, and coincidence scalers
respectively, and E? and E, are the efficiencies for the beta and gamma detectors. I-Ience
it follows that
€0 = N,/N,.

I n practice these equations require several small corrections, the largest of which are
clue to dead time, accidental coincidences, and backgrounds (9). Since the counter has
been sho\vi~to have 10070 of 4a geometry (9), the inefficiency in the beta detector is
due to self-absorption, source mount absorption, and the possibility that the counter-
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alnplifier system inay not detect one ion pair.


T h e following negatroil elllitters C~'~"86-ltev branch only), Nbg5, Hg203,CoGO, Sc46,
RbsG, Aulg8,Na2-I,and the positron branch of C U ~were . ~ used in this study. Aliquots
Lvere deposited 011 VYNS plastic films (superficial density 5 pg/cin2) stretched across
a l ~ ~ n i i n urings
m 1.5 in. outside diameter, 1.0 in. inside diaineter, and 0.022 in. thiclt. The
underside of the plastic film was coated with 15 pg/cm2 of gold. After a sample was
deposited, a similar gold-coated film was placed over the source so that both gold surfaces
were outermost. Provided that the source is not exceptionally thiclc this second film
adheres well to the source material and the first fill11 without forming cavities. The
resistance between the center of a film and the inount ring on the coated and uncoated
side is about 0.2 and 1.5 meg respectively, while the resistance of a film having no
gold oil either side is greater than 600 ineg. This sandwich technique ensures that 110
For personal use only.

active material can flake off the source, and also provides a more durable source mount
for very little increase in total mo~untthickness compared with a single fill11 coated on
both sides.
T h e con-ection for absorptioil in the source mount was determined by observing the
efficiency as a functioil of the number of pairs of gold-coated filins added to the sand-
~vich,and extrapolating the resultant "absorption curve" to zero film thickness. The
are listed in Table I , those for Cs13.', Nbg5, CoGO, and Ka2"vere measured
as described above, while the remainder were fouild by interpolation.
A s~izallcorrection required for the threshold detection energy of the counter-amplifier
system was estimated as follo\vs. I'ulses due to I< X rays froin Ca", Cr"', and Fejj
observed a t the output of the first stage of the ainplifier sho~vedthat the system was
linear in the range 3.3 to 5.9 ltev. Comparison of tlzese pulses with the amplitudes of
suitably shaped signals fed to the amplifier input from a pulse generator which just
failed to register in the beta scaler gave a threshold detection energy of 0.35f 0.1 ltev
when the counter was operated near the center of the plateau. Assuiniiig that self-
absorptioil does not appreciably distort the spectrum, corrections for uildetected particles
below this threshold energy were calculated using theoretical beta spectral shapes. The
correctioils for this effect are shown in Table I.
The determination of the efficiency for the 86-lcev beta branch in Cs13.' presented
some difficulty owing to the complex nature of the Csl" disintegration scheme. The
results for this branch were determined by accepting pulses in the r-cl~annelcorresponding
to the sum pealt a t 1.97 Mev only. In order to increase the efficiency for detecting this
peak t h e outputs of both crystals were added linearly before discrinzination, giving a
gamma efficiency of 0.03% (as compared with 10 to 15% for the other nuclides). The
statistical uncertainty of the efficiency measurement of any one source is estimated to
be f27, for CsL3",while for all the remaining rluclides the corresponding value is f 0.27,.
The values obtained for the positroil branch in C u c h e r e deterrniiied by accepting
pulses corresponding to the 0.511-YIev photo peak i l l the gamma detectors. A correctioil
MERRITT ET AL.: SELF-ABSORPTION 1111

of about 0.3% was necessary for the contribution of the 1.34-Mev galnnla ray lying
under this peak.
T o obtain an indication of the variation of self-absorption with source thiclciless the
beta counting efficiency was measured as a function of the carrier concentration for
AuIg8, Rba6, and Nbg5. The results are given in Fig. 1 where the crosshatched area
represents the spread in self-absorption which was found.
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0 I I I I I I
2 4 6 8 10 12
M E A N SUPERFICIAL D E N S I T Y m g / c m 2

FIG. 1. Per cent self-absorption a s a furlction of the mean superficial density for Aulg8, Rbs6, and Nbgs.
The Aulg8 and Rbs6 sources were prepared using the colloidal silica and insulin treatments respectively,
while both methods were used in obtaining the curve for Nb95. The inset shows the variation of self-absorp-
tion a t low mean superficial densities for Nb".

In order to conlpare the self-absorption of sources prepared by different methods and


with different isotopes, an attempt was made to maintain a lllean superficial density of
2 pg/cm2, but variations in the area of the deposits may have caused deviations of 50%
in this value. In Table I we list the self-absorption, corrected for source mount absorption
and threshold detection energy, for a number of isotopes and source preparation tech-
niques. T h e quoted errors are standard deviations for about five sources. Brief descriptions
of, and cominents on, the techniques follow according to the colunzn headings of Table I.
(a) Simple evaporation method.-Aliquots are dried under an infrared lamp and yield
a roughly circular deposit of about 1 cm? Nlicroscopic inspection shows that this method
often results in clunlping of the source material, usually around the edge of the deposit,
cf. Pate and Yaffe (5). The large errors in this colunl~lshow the poor reproducibility
of the method, especially for the lower energy beta emitters.
(b) Precipitation method.-A drop of distilled water is added to a source which has
been dried as in (a). The source is the11 redried in a n atmosphere of ammonia provided
by rinsing a beaker with concentrated ammonium hydroxide solution and inverting it
1112 C.\N.\DI.\X JOURNAL OF CHEMISTRY. VOL. 37. 1959

I
7'-\BI,E I
I
Per cent self-nb~orption

Source 'I'hresholcl Self-absorption, yo


I\'Ia\imum mount detection -- ---
beta absorption energy Evapo- Precipl- Insulln- "Luclo\"-
energy, correction, correction, ratecl tnted treated treated Sprayed Distilled
Nr~clicle Mev % % (u) (b) (6) (d) (f)
Cs13' 0 O8G 5 1 1 +
39 6 21 4+:3 2 18 i + l 3 G i+0 9
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Nbgj 0 16 2 0 3 20:3+21 0 3&3 5 8 5&l 0


Hg203 0 21 2 0 5 5 6&0 G 1 0&0 5
Co60 0 31 1 0 2 S 7&1 5 :i7+0 5 5 2+1 2 3 6+0 7 I 1 & 0 ti 13&0 5
Sc40 0 36 0 7 0 2 5 3&1 7 2 8+0 8 5 1+1 1 2 8&0 4
CuG1 0 GG 0 0 0 00 0 2+0 2 0 1&0 2
Rba6 0 ti8 0 3 00s 27&l 1 2 3+0 6 1 0+0 2
Aul" 0 $16 0 2 006 lG&OG 1 4+0 ti 0 G+O 4
Na?' 1 39 0 04 0 01 1 0+0 5 0 8&0 :3 0 2&0 2
I
over the source. These sources appear more uniform ancl exhibit higher counting efficiencies
than similar sources prepared by method (a). T h e ammonia treatment is limited to
elements which form insoluble hydroxides, but the technique has been extencled by the
use of hydrogen sulphide in the preparation of precipitated I-Ig20%ources.
(c) Insulin treatment.-Insulin solution used as a \vetting agent improves the uniformity
For personal use only.

of evaporated sources ancl hence their efficiencies, particularly when the solids content
is high. Although the usual practice is to remove (prior to depositing the activity) most
of the insuliil solution from the source mount the solids in the remainder are often
considerably more than those containecl in many high specific activity solutions, ancl
hence the presence of these solids partially offsets the beneficial properties of the insulin.
T h e sources einployecl in these studies containecl about 2 pg of such residual solids
fro111 the insulin. I-lence the mean superficial density of sources listed in column (c) of
Table I is about 4 pg/cm2.
(d) Colloidal silica treatmc.nt."-Aliquots arc delivered into a small amount of silica
sol on a source mount and dried as in (a). A freshly prepared 1:101aqueous dilution
of "Ludox" Si\4 (clu Pont) has been found convenient. A stucly of beta efficiencies as a
function of the a ~ n o u n tof "Ludox" showed that about 10 to 20 of the dilutecl sol
(about 0.2 to 0.4 pg residual silica) is optiinum for most isotopes. Although high ionic
concentrations should be avoicled to prevent gelation of the silica, "Ludox" has been
successfully used with solutions as acidic as 0.3 N.
(e) Spray mrt1zod.-The source preparation technique of Cars\vell and XIilsted (11)
has been used to prepare almost invisible sources on golcl-coated VYNS i11ounts.f T h e
activity is dissolved in acetone, which is then introduced into a fine glass capillary
( N 0.005 in. a t the tip). When about 3 l ~ vcl-c. potential is applied between the source
mount and the tip of the capillary a fine spray is ejected. Conditions are adjusted so
that the droplets forn~ingthe spray evaporate before they reach the source n ~ o u i ~ t .
Although the method is presei~tlynot quantitative, the yields can be made better than
1
1 goy0 and the convenience of the inethod together with the low self-absorption obtained
suggests its use for the technique proposed by Seliger (12) for the standardization of
I
beta emitters having no y-ray in their decay scheme. A thin source is prepared froin
high specific activity material, and counted. T h e deposit is then coinpletely dissolved,
* T l z f s method w a s drveloped b y W . F. Alerritt, w h o zised it to prepare S3jsozirces (10).
I
t W e are indebted to Drs. Frnser a n d llltlton of this laboratory for the zise of thrzr eqziiptnent, w h i c h is a nzodi-
jication of that described b y Carswell nltd Milsted.
MEKRITT ET i\L.: SELF-AUSORI'TIOS 1 1 13

carrier added, and the solution inade up to volume to form a standardized stoclt solution.
This can then be used to calibrate other sinlilar solutions by direct comparison.
( f ) Distillation method.-Some sources of Corn have been prepared by the distillation
inethod of Pate and Yaffe (5)." These are very i~niforindeposits which exhibit about
the saine self-absorption as sprayed sources. For the sources studied the yields were
low, but according to (5) the inethocl may be made very nearly 100yo quantitative.

IIISCUSSION
The self-absorption values obtained by the siillple evaporatio~lmethod and by the
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use of colloidal silica (columns (a) and (d), Table I ) are shown graphically in Fig. 2,
For personal use only.

h'iCY,!riUV BETA E!<ERGf. l.lc\

FIG.2. Per cent self-absorption as A function of beta end point encrgy for sources of Incan superhci,~l
density of 2 pg/cm2. Curves A a n d I3 represent sources preparecl by the simple evaporation ancl colloidal
silica nlethods respectively.

curves A and B respectively. 1;or clarity the results for i~lsulin-treated sources have
not been plotted; inspection of Table I shows that they are very similar to those for
colloidal silica-treated sources. T h e results show a: comparr\tively slllall variation of
self-absorption with beta end point energy above about 400 Itev, but below this value
the absorption rapidly increases. We also note, in agreement with others (8), that the
reproducibility in general tends to decrease as the self-absorption increases. On the
whole there is good agreement between the self-absol-ption values obtained by method (a)
and the experimental results of Gunnink et al. (8). Our values are slightly larger than
those estiillatecl by Seliger and Schwebel ('i), while those obtaihed for the distilled Coca
sources are in agreement with the curve given by Yaffe ((5). The use of colloidal silica
is seen to be particularly advantageous a t low beta end point energies, although no
* W e are illdebled lo D r . IT([ffc rrlrd 11Ir. 3.B. F L S ~ ~ Ifor
Z ( the
L ~ j r c j o r a l ~ o t r O/ these sozirces.
111-k CANADIAN JOCRN.SL O F CHEMISTRY. VOL. 37, 1950

technique that we have investigated to date is capable of reducing self-absorption to


negligible proportioils. There is one notable deviation froin the curves of Fig. 2, viz.
the positron branch of CuG+. This may be explained by the fact that owing to the coulomb
repulsioil effect there are fewer low energy particles in a positroil spectruin than in a
negatron spectruin having the same end point energy and hence self-absorption effects
are smaller.
I t should be emphasized that the rapid variation of self-absorption with source
thickness (Fig. 1) demands that the source preparation techniques and mean super-
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ficial densities be closely similar to those used here if the curves of Fig. 2 are to be used
to estimate even approxi~llateself-absorption corrections for 47rp counting. Further,
Fig. 1 (inset) and Fig. 8 of (5) show that for sources of smaller nzean superficial density
it does not necessarily follow that the self-absorption will be significantly less.

REFERENCES
1. U. B.
SYITI-I, A.E.R.E. Iiept. I/R 1527 (1954).
2. MANN,W. B. and SELIGER,H. H. J. Research Katl. Bur. Standards, 50, 197 (1953).
3. PATE, B. D. and YAFFE, L. Can. J . Chern. 33, 929 (1955).
-4. HAWKINGS, R. C., MERRITT,\V. F., and CRAVEN, J. H. Proceedings of syrnposi~rm.WIainterrance
of Standards, National Physical Laboratory. H.M. Stationery Office, London. 1052.
5. PATE, B. D. and YAFFE,L. Can. J. Chem. 34, 265 (1956).
6. YAFFE,L. Unpublished results.
7. SDLIGER,H. H. and SCHWEDEL, A. h-~rclco~~ics,
12 (NO. i ) , 5-4 (1954).
8. GUNNINK, R., COI.DY,L. J., and COBBLE,J. W. Anal. Chern. To be p~rblished.
9. CAJIPION.P. I. Intern. I. Appl. Radiation and Isotopes, 4, 232 (1950).
For personal use only.

11. CARSWBL'L, D. J . ~ ~ ~ ' M I L S TJ.E DNuclear


, Energy, 4, 51 (1957).
12. MEASUREMENTS AND STANDARDS OF RADIO.ICTIVITY. Publication No. 573. National Academy of
Sciences, National Research Council, Washington, D.C. p. 47 (1958).