.- .’

—

&- .@410924 4 / ~

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copy No.

SPECTROMETRIC ANALYSIS OF GAMMA RADnTION ●

FROM FAL~ UT FROM OPERATION REDWING/

+

9

Research and Development Technical Report USNRDL-TR- 146/’

29 April 1957

by

W. E. Thompson

Stihsnwt AApprovedforpublicrelease:

SAN FRANCISCO 24* CALIFORNIA

1111Sanitizedby Chief,ISIS,DNA

/

m. ..’... ●

SUMMARY

Gamma radiation emitted by selected fallout samplescollected at Operation REDWING was spectrometrical.lyanalyzed for the purpose of determining its characteristics(expressed in terms of absolute photon intensities for eachdisc ernible gamma line) as a function of time after shot.

Since the absolute photon intensitiess are given and most-- samples represent known fractions of the area of the fallout

,1 collectors, one result is that dose rates in the vicinity ofthe collecting site can be calculated.

=?’f

Another important result of the analysis suggests thatNaU becomes an increasingly important contributor to theradiation hazard from fallo-ut at early times after detonation

““lq,]”,

II -,I

,..111

.

ADMINISTRATIVE INFORMATION

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=

I

I

This report is one of a series of technical reports on the gamma-ray spectra of fallout samples collected atvarious weapon tests.Previous data has been reported in this laboratoryts USNRDL-420,31 August 1953, USNRDL- TR-32, 26 January 1955, and USNRDLTR-106,27 August 1956. The sample study reported here was conducted inconjunction with Project 2.6.3, Operation REDWING.

The work was done under Bureau of Ships Project No. NS 081-001,Technical Objective AW- 7, and is a continuation of that described *

* as Subtask 6 in this laboratoryts report to the Bureau of Ships,DD Form 613, July 1956. Similar work is described under Program 9,Problem 1, in this laboratory’s Semi-annual Progress Report,1 July to 31 December 1956, Progress Report USNRDL-P-1,

●

January 1957.a

-Y

r

w—-.e ... . .. ..- . . ..

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ACKNOWLEDGMENTS

~~e author wishes to acknowledge the ass~g$ance of Dr. R.L.N?fher and Dr. C. S. Cook whose suggestioq~ -d critical re -yjcy of the report were greatly appreciated:

~he assistance of Dr. D. L. Love and M~: ~$L. Mackin of~palytica! and Standards Branch of Chem@~ Technology Division

}??PreParlng the calibrated standards iS ~F@@fully acknowledged.

The excellent liaison both in regard tq qprpples and informatio~~e~pe~ Radiological Capabilities Branch ~~ @heroical Technolog- - .~iy$?$~~ and this Section was provided h~ ~~, W. Williamson, J,

The @aussian curve generator was cepqfrpcted by Mr. P.S.Apple baum.

Members of the Electronics Sectioq ~e~p cooperative at alltimes.

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v.

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I

.

I

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.

.

).nzlyzesnave been r.adeat !X::7JLv!tk 3 slfi~le-cil:.nn.;l

.~.~ru~~araysp~ctro~e’~erjof ra5iat20nd

eviitte5by 21 selecte5

ra3.icactivefallout sarlplescollecte5 by Project2.6.3 at

the Sprin~, 1956, weapons test series knovn as Cperation

P=DUI1?Gat tne Pacific Provin~ Groun5s. These r.easure-

ments were made to fleterifiinethe spectrometric character-

istics of the fallout radiationversus time and to compare

these characteristics for consistency among samples from

the same and flifferentshots. *

The present work is a continuation of the spectrometric

analyses of fallout @mna radiation which have been made at

Operation UPS50T-IO!OTi:OiJat the Nevada Test Site in 195312n

Operation CASTE at the Pacific proving Grounds in 1954&,3,4, .,

and Operation TEAPCT at the Nevada Test Site in 1955

takln~ advantage of further refinements in instrumentation

and analyzing technique.

project 2.6.3 collected samples of various types at

several ship, barGe and land stations and returne~ them

to N5DL by air. This rapid return allowed analysis to

begin as early as 51 hours after shot time--a notable im-

provement over the earliest-time receipt of 4 claysaccOm- -

pllshed at Operation CASTLE. Other samples requlrlng

specialized handlin~, i.e. wei:hing, aliquoting, evaporation,.

~’

. . .. -.

●

●

I

.

l,rIL13as te3 ti~;snfter sht ti::2.—— — —.._ _

The results show a’bsolutephoton souuce stren~ths

for each ener~y from the various samples, while in previ-

ous reports only relative line intensities were given.

Since each sample constituted an accurately ~etermined

portion of the material taken from a fallout collector

of known area, an estimate can be made concernin~ the

total gamma source strength per unit area in the vicinity

of the collectin~ site.9?

Other than reportln~ quantitative information on

photons emitte~ per square inch of fallout collection

area, this experiment exeinplifie~better organization

and preparation in other ways. The samples were pre-

pare~ in stan5ar5ized containers so that changing geo-

metry was never a problem. ..Thespectrometer was llwell-

seasonedt]an~ 5epen5able and was use3 without modifica-

tion throughout the course of the experiment. The instru-

ment was improve5 by the substitution of a Moseley X-Y

plotter for the

itself was made

use of a better

Brown recorder. Finally the analysis

simpler anfimore consistent by the

way of measurin: peak areas.

●

2

a.

.

.

A gamma-ray photon is detectable only by means of

the ener~y it loses in an interaction or interactions

~~~thmatter. Gamma-ray photons lose energy by three main

processes: photoelectric effect, Compton effect, an~

positron-negatron pair production. The cross-section for

each effect is dependent on the energy of the gamma-ray

photon and the atomic number of tie detectins material..

The ener~y given up by the gamma-ray photon un~er- ~

going any of these processes ultimately manifests itself

in the molecular excitation of the 5etecting material.

Yany organic crystals(such as anthracene, stllbene, an5

dlphenylbut.a~iene)and many inorganic crystals(such as

thallium-activated sodium iodide, in5ium- or thallium-

activated lithiumtidi5e, ard potassium io3i5e) relieve

*

this excitation in the form of useful scintillations of

light whose pre~omlnant color 5epen5s on the crystal.

The intensity of the light flashes produced In these

materials is dependent (in some cases, linearly) on the

energy of the Incident photon (provide~ it is totally

absorbed). These light pulses are detecteflby a photo-

multipller tube which converts them into electrical pulses.

=?

--

●

✎

a

●

I

.

I

These ~ulses are am~lified then analyzed accordi.ncjtO. .

peak voltage anticounte3.

NaI(Tl) crystals are in wide use today as @n~~a-

ray detectors because of their high efficiency and linear-

ity. The disadvanta~e of their being hyg?oscopic is Iar&jely

overcome by sealing them hermetically In thin-walled al~i-

num containers. .

For this experiment a special sample hol~er was made.

for the-spectrometer which allowed the bottoms of the H’

sample containers to be placed 2 Inches above the top of “

the collimator (a l/2-inch hole through 6 Inches of lead)

and centered without further adjustment.

The q-inch in diameter by

s-inch Du 140ntphotomultlpller

housing (Fig. 1) were the same

sis of the data from Operation

5escribe5 elsewhere.4

b-inch long NaI(Tl) crystal,

tube, preamplifier and

as those used in the analy-

TSApOT3 an~ are more fully

The output of the preamplifier was fed into a Tracer-

lab non-overloading linear

were analyze5 by an Atomic

pulse height analyzer, the

was provided by a helipot,

The output pulses from the

amplifier whose output pulses

Instrument Company Model 510

variable base line bias o; which——... .——— ——.—— —~

motor ~riven thraugh its r~n=e.

analyzer were fed Into

.

a

.

I

.

.

u~sA”pLE—

et’

5

--

.

I

I

.-.

count-rate meter. This count-rate

from 10 countsmeter has 7 scales ran~in~ in sensitivity

per secon5 full scale to 1000 counts per secon~ full

sc21e. The output of the count-rate inter controlle~ the

Y cooriiinateof a l~oseley[+.utografX-Y plotter, vinilethe

X coordinate was varieclby the base line bias of the

analyzer. A mollificationin the form of apotentiometer 1

in series with the X input allowe~ fine afijustments$0 be

ma3e in matching pulse height to particular lines on the

recor5ing paper. A zypical recording made

recorder is shown in Ftc. 2.

The re~ulated hi~h-volta~e

plier tube.

.

“ii2sconstructed from

supply

a UCR~

‘i’hefallout samples were supplied

for

by the ~.y

*the photomulti=

design.

by Project 2.6*3

in s/~-inch tn diameter by 2-inch in length polystyrene

containers each containin~ approximately 50-1000 micro-

curi.estotal activity. Descriptive information about

sample, the effective fallout area it represents, an~

associate5 shot is listed in Tablel-~.— . _._ _____. —

Samples were obtaine~ from 2 types ~S c~llectors

each

its

. The

cloufisample consisted of material caug’nton a filter paper

tl?rou3hwhich a representative sample of air was 5rawn as

an aircraft flew throu~h the Ql_ou5follol’tln&..t~d3$~2tion.———— —.. — ..———— _._ ——----

-.,-. T:he tables n,.Jxsrn: the end i~f’the texto

,

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.

I

,., m,

<

r

.

],,,: ;’

.

6,7collector (CCC) was designe5 to

collect ana hold fallout material while reducing to a

minizm.mthe amount of e-xtraneousmaterial deposited both

before and after the collecting perio~. linentriggered

either by an increase in ra~ioactive back~round or by han~,

the cover of the 5evice opens and a collectin~ tray rises

into the wind stream for the preset exposure time (variable

~n is-minute ~ncrements between O anii81 hours). The traY “

has an effective collectin~ area of about 2.5 square feet--

-dividedInto numerous cells to reduce loss of material du~.

to win~.. Sanples, other than cloud samples, were obtained

from this type of collector mounted on converte~ liberty.

shtps (1~.G’s)j bar~es (YW?B;S) an~ “HOW Island.

After collection the fallout material was flown back

to the Laboratory an5 aliquote5 by Chemical Technology

Division. The aliquots su?plisd to this section for analy-.

sis were placed in the polystyrene containers and prevented,

from shifting, In the case of granular or pulverized samples,

by the addition of a small amount of paraffin.

The machine was calibrated so that on “stan5ZLrd” gain

the total absorption peak of a 100, 200, or SOO, etc., kev

Gamma ray WOU15 be centered on the l/2-inch, l-inch, or 1-l/2-

inch, etc., line on the recqrdlng paper. This calibration

was accomplished first by careful zero-settin~ of the X-y

0

.-

recorder and analyzer, an5 ti-.enby varyin~ the Cain of the

*

.

--

.

.

,.

amplifier an5 the fine pulse-hei:ht aiijustrnenton tl~erecor-

der until total absorption peal:sfrom staniiarclsof kno~?n

20s, Na2~ an~ Cs~amma ener~ies (1-ig 1s7) fell at the appro-

priate positions on the recariiingpaper (Fig. 2). It was

found that this calibration was very stable, requiring only

an occasional small adjustment In the zero-set control of,

the recor5er to allow for variation in paper placement and ,

rulinG defects on the paper. That the equipment was essen-

tially stable in the Y direction was shown by perio~ic-“

checks with the 6@cycle test position of the count-rate -

meter anilby the linearity of the decay curves on semi-

logarithic paper of the calibrate5 standar~s.

Pulse height spectra were recorded for each sample on

standard gain (3 ITEVfull scale) and on “highi’gain--

amplifier gain increase~ by a factor of four (0.75 Mev full

scale)--in tnose cases where the strength of the EWnple

allowed it.

each sample

rate became

depenaed of

HOW long the taking of periocllcrecordings of

could continue after shot time before the count

too low for statistically significant results

course, on the original strength of the sample.

On nearly all of’

~a22 stan5ard source

different color ink,

the standar~-~aln records, a calibrated

was recorded on the same sheet In a

while on the high-gain records a

9

1-.

f

i- ‘

1

203 source was used.calibrated lIg Tnis use of the calibrate~

standards allowed a constant check to be made on the stabil-

Ity of the equipment (see Appendix I).

ANALYSIS OF DATA

The pulse

consists of a

distribution.

height spectrum of a monoenergetic gamma ray ‘

total absorption peak and continuous “Compton”

If the energy of the gamma ray is above 1.02

Mev, pslr production begins to take place and one of two

secondnry pepks Is contributed to, according to whether M—---— --—---J- ---- — —--— - —--- .-—

or both of the annihilation quanta escape from the crystal.

The peaks all have the shape of normal distribution functions

or “Gaussians” because of the statistical nature of the

photoelectric effect and the seconfiary-emisstonphenomenon

inherent h the operation of a photomultlpller tube.

If two Incident gamma energies are present, the lower

# annihilation

the spectrum.

-. .- . -

is superimpose~ adiiitivelyon the continuous Compton dis-

tribution of the higher. An example of the idealized

additton of three different monoenergetic gamma rays”is

shown In Fig. 3. As more gamma energies are added the

resulting confusion becomes progressively worse. (If the

higher energies are above 1.02 Mev, the presence of

rafltation

and thus

escape peaks further complicates

the analysis.)

--

‘

I,,

.

.!, ‘1

.

BACKGROUND

h

I1

Pa

I1I

I

E. E, E,

PULSE HEIGHT, V

Fig. 3 Addltlon of Three Total Absorption Peaksat Different Energies and Their Associated ComptonDistributions Showing the Resultant Spectm (heavy

+’

line).3

11

II1“..

.,,

In order to untan~le these overlappin~ ~istributions

anfiarrive at the basic gamma lines, a method of graphical

unfolding is use~. Gne starts at the highest-energy peak

present (assuming that It is not superimpose~ on the Compton

distribution of a still higher energy) an5 measures the area

under the total absorpticm peak. Then knowtn~ the peak-to-

“ total ratio (the metho3 of ascertaining this ratio is des-

cribed later) for each energy, one can calculate the area

of the Compton distribution. After drawing in the Compton

distribution of the highest energy, the process Is repeated

for the next highest-energy peak using the Compton of the *

highest energy as a base line. The process iS continued

until all the

resolution of

whether there

energies present are analyzed.

the instrument for each energy,

is only one energy contributing

Knowing the

one can tell

to a particu-

lar

the

kev

peak, ‘or two or more unresolveiienergies present, by

wl~th of the peak. The resolution (width of a peak in ‘

at half-maximum height) was determined by measuring the

resolution for several total absorption peaks of

an~ plotting the results (Fig. 4).

In or~er to facilitate the measuring of the

areas and to aid in estimating the relative size

known energy

photopeak

of two s

unresolved peaks,a series of Gaussian curves of predetermine

widths, various heights and,thus, known areas, were ~rawn by

means of a Gaussian curve generator (see Appen31x II). BY

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.

b

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1-

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Fig. 4 Instrument

E (KEV)

Resolution Versus Gamma Energy

E (KEVI

Fig. 5 Crystal Interaction Probability, v, versushmma Energy, E.

13

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Q,,t,-q

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superimposition of the suitable Gaussian on the pulse height

spectrum with the aid of a froste3-glass light table, the

area of each total absorption peak was determined without

tedious measuring

by this measuring

tion

ray,

with a planimeter. For errors lncurre3

system see the sec%lcm on errors. .

absolute photon intensity to total absorp-

aome function of the energy of the gamma

For the 4etimn$nat* of the graphical

relationship between Z\A and E, ltuaa first necessary

ascertain further machine parameters and other energy-

dependent factors- The8e we~:

to

*,(~)’Gzystal Interaction pm~btltty, v. This -I

is simply the fraction of incident photons of a par-

tlcular energy which Interacts In the crystal and Is

given ‘by:.

V= l-””exp(-kx)

Where ~ IB the total linear absoqptlon coefficient

8for gamma raya In soilhuniodide and X IS the crystal

length. “Rara crystal ito.16cm (4 inches) In lengthJ

v versus E la shown plotted In Fig. 5.

(2). Peak-to-totalu?atlo,w. This fector IISdeter-

mined experimentally by-recording the spectra of several

sources ti “knmn gamma energy and measuring areas of the

total abmmpla%m peaks an~ the axwas un!lerthe total Bpec-

trum. The-@e of’%hese areas platted agahst energy

.

., I

.

furnish a fairly smootlicurve. The

curve characteristic of’the machine

peak-to-total

usefiin

experiment is shown in Fis. 6.

(3T Counts per second per square inch

total absorption peak, C. This number is a

of the machine an~ Is foun~ by divitlingthe

counts per secon~ per Inch of deflection In

tion by the channel width In chart inches.

the present

in the

constant

number of

the Y direc-

The channel

width use5 throughout the experiment corresponds to*

0.1 inch on the chart paper and the total Y 5eflection-

1s 10 inches. Then for the 200 c/s scale, C is 200.

(!) Source re~uct16n factor, ~. This factor i$

the fraction of photons leaving the source which enter

the crystal an~ takes into account effects of collimator

. penetration, finite extension of sourc~and soli~ angle

subten3e5 by the

point source and

are aiscussed in

crystal froimthe source,assuming a

an opaque collimator. These effects

some 5etall In a theoretical paper by

9 Derived from informa-R. L. Mlther of this laboratory.

tion containe~ in this paperis Fig. 7, showing K, the

source re5uction factor for a point source, versus r,

the distance of the source from the collimator axis.

To fin~ the average source re~uction factor, ~, to account

.15

*

.

.

If.

,.,,

.

.

1

I .I 1 1 ! I ( 1

‘-+ ‘- 1......1.-32=-=-+ ‘- !- I ! 1J“-- i -1 r: :!-” .1. . 1. I I— f—1

-“1 -J I[ 1

I I 1I1 r 11 I

II 1 ! I !

,

~: !.’,l,:;:x’ 1

1!7 r..- --- .

●. . — [I 1 I

, I r T ,,

0.8 I. -.— -- — ( —.

, 1.- -

! 1 L 1 I I.+ 1 1

—.. /

t-i1

!I \ 1 —. - —-

0.6 ;●

.- ● ExPERIMENTAL FONTS 4 !. I

B 1 1 T I

I i -04 ;

I /l

I I -1 I “A-k-..—. I 1 ,I ._..l..—l.–-,.—-t

I .—— !-- -----—

02‘1 I.–1 .“

; .—-=_l_2_ ~:-: l-::1---:-t”t_—~-~

1“ + —..— —— ——--- ----- -- 1.— — .— -. .--’--- .-.

,

0 1 1 1 40 400 lzm 1600 2CQ0 2400 2800 S200

Fig. 6 Ratio, w, of the Area Under the TotalAbsorption Peak to the Area Under the EntirePulse-lieightDistribution Versus Gamma Energy

I

.

*

.

.

.

%

.

.

‘for the i’inite

to perform the

extension of the source, it was necessary

folloV7inSnumerical i.nte~ration:~ - ——

?rrs

.

--

I. .:

.

....i

.

J~=A#QzJo rdr

where r5 is the radius of the extended source. Tile

follows:

the faCt

r, i.e.:

‘sa/2)___._..—

function of r determined

derive~ from Fig. 9 of

equal to or larger than

determination of ~ is somewhat simplified by

that X Is constant over part of the ran~e of

= b/2)2 (OSrK= a2/16( Z——

where a is the collimator diameter, b the colllmtor

thickness And z the distance from the center of the ~

collimator to the source. Vhen r Is larger than a\2 -

and smaller than az/b, K is some

graphically by interpolation and

Iflathertspaper. For values of r

az/’b,K vanishes.

To make the reduction factor,~, ener~y dependent, “9

i.e.Jto include penetration effects, an approximation

is used. Penetration is a function of Gamma-ray energy

and the increased aperture due to increased energy is

“approximatelythe same as the geometrical aperture of

an opaque collimator two mean-free-paths less tnick.

For the particular geometry involved in the present’

experiment, the values of the’machine parameters are as

.

, 13

. ...- . .. . .

.

.

2= 1/2 inch

z = 5 inches

r~ . 3/8 inch

b= (6 - 2/P-)inches

where l/v is the mean-free-path of gamma radiation

in lead.

1I ~was evaluate~ by means of numerical inteWa-

tion for values of E (an~ corresponding values of

b) at 200-kev intervals between O an3 2 14evand at

1 3 Mev (Fig. 8).-

la

i The absolute photon intensity Is a combination of these

. various correction factors, i.e.:

I = Ac/vwzp,~

. A graph of I/A versus E is shown In Fig. 9.After rea~ing

i{the energetically appropriate I/A from the graph,

the number

was multiplle~ by the area of the total absorption peak of

the correspon~in~ Gamma ray to obtain absolute photon inten-

sity of that line.

*

.

RESULTS

The absolute

errors are listed

Tables 2 and 3.

photon intensities with their estimated

for each gamma llne of each record in

The abbreviate~ sample notation used for

.

.

.

.

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E [KEVI

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brevity in Tables 2 atid 3 is explained in ‘Mbla 1. Table

11 contains the information obtaine~ fro~lthe stan~ar~ Sain

recoriin;s antiT:ble 3 lists the photon intensities fourtl

from the hi~h gain (4X) recor~fn~s. Because of the increase

in resolvin; power some lines which were unanalyzable or

un~etectable on the standard gain records became analyzable

on the high Gain records.

The data have been left in tabular form

information more readily accessible to those

Lt.

.

In actual practice the analysis is more

.

\ “

{!

‘1

to make the

who wish to use

*

difficult than

might be assu.nedfrom the description in the Analysis of

Data section for the followinz reasons:

(1) The shape of the Compton distribution is known

only approximately for a Given energy even though Its

area Is known fairly accurately. Even if the shape

were accurately known, it would be mechanically cllffi-

cult to draw such a distribution in with a predetermined

area. For this reason a straight line is used for the

Compton distribution, with the resultin& rectan~le having

the proper area. It Is found, however, after drawin~ in

this

tion

that

rectangular representation of the Compt~n distribu-

several times and ~ettin~ the “feel” of the machine,

the base line for each succeeding peak can be

estimated with similar accura~y

--——

. . ,,..

an~ consi~erably Greater spee~. Either way, of course,

.

.

3.

i)

.

:! I.

this approximation contributes to the

errors becomlnS progressively greater

energies.

(2) If two or more energies are

together to be resolved, one can draw

Gausstans of the proper wi~th beneath

overall error, the

toward the lower

present too close

two or more

the broa~ peak

representing these unresolved energies, but

ficult if’not Impossible to determine which

gies Is prepon~erant. In this case one can

more than estimate. The ener~tes present

of the ener-

do little5?

in this way-.

therefore have lar~er estimate~ errors associated with

them.

(3) Because of statistical fluctuations due,to the

. low count rate on many samples, the curves Arawn by the

X-Y recorder are not smooth and the size of the peaks

is somewhat questionable. On records where low count

rate exists, therefore, the associated errors are esti-

mated to be lar~er. ._.—— — .—..-_ _— —--—--—-—

I?or comparison betv~eenareas determined by superimposition

of generated curves and areas rie~.sured‘:?iththe plsnimeter, sev-

eral total absorption peaks were measured ty both methods. ‘i’he

* cllsperitybetween those peeks so co.mpsrecl r~nged from O to 3 per-

cent. This error is in sencrql less than the ststistic~l error..

22

-- .,---- .. -. . — . . .. . . ---- -- .—. —

.

.

t: I

!

i

.

foun~ by takin: the

.

square root of the total number of counts

contained in a rectangular area whose wi3th Is 3eternlne5 by

the width of the Gaussian at the point where it ceases to

coincide with the machine-5rawn peak. This area is presume3

to be the actual area compared. The statistical error founcl

in this way varies w15ely (because of the great ran~e in

count rate), but for the peaks tested it vari~s between 2 and

6 percent.

A hindrance to

curves on the total

accurate superimposition of the Gaussian

absorptl.onpeaks, contributing further

to the error, may be the sll~ht non-Gaussian character of the

total absorption peak cause~ by the lack of perfect homoge~ ItyT

of the crystal’s liGht production.

To get some idea of how much of each spectrum occurre~

In analyzable peaks,the total areas of several spectra were

measured with the planimeter an~ compared with the sums of

the total areas assoctate~ with each liste5 energy (foun~by

dividing each peak area by the appropriate peak-to-total

ratio). It was found by this method

cent of a spectrum was accounted for

analys5.s.

that from 70 to 90 per-

in the peak-by-peak

The errors associated with the photon intensities shown

in Table 2 are the result of estimates of the cumulative

errors discussed above. They range from 3 percent for peaks

with goo~ resolution, good count rate,and EO03 fit with the

.

23

—.- .-:-?-!---- . . . . .

I

,1i,-.

.

superirfiposedGaussian curves to 50 percent for peaks poor

in cll respects. Occasionally there is”present an ener;y

which is too small in photon intensity even for a good esti-

mate to be matieas to the quantity. The

in the appropriate column in Table 2 to

ence of such an enerGy. ‘Morerarely the

symboI~O is use3.

indicate the pres-

symbol >>0 is I

use~ to i.n3icatethe presence of an energy too poorly resolve3

(althouGh not necessarily very small in intensity) to warrant

an estimate~ quantitative list:ng.

In some cases there appear to be discrepancies between

photon intensities from the sane lines taken at nearly the=

same time for the two gain settings. Most of these inten-

sities are not discrepant, however, by much more than the

estimated error WOU15 allow. In those cases where the ~if-

ference is too large, the estimateq errors shoul~ be Increasea.

However, some of the ~ifferences seem pre~ominantly

one-sided. This inconsistency is especially noticeable for

some of the 220 kev lines, i.e.,areas recor~eiiat high gain

are lower than comparable areas recorded at stanflar~gain,

sometimes by as much as 30 percent. This effect appears In

the resolution curves of Fig. 4. For many of $he 105 kev

lines compared,the effect is reversed, I.e. the areas recor~e~

at high gain are higher than comparable areas recorded at

standard gain. It is possible to account for the latter

.-,--- ,.-

.

.

effect by considering the ~reater effect an inteGratin~ time

constnnt, such es is used in the count rate meter, has on low

pulse hei~hts.10 No mechanism to explain the former effect

sug~ests Itself, however, and the fact that fair a:reement

exists in most cases between comparable 60-kev an3 280-kev

lines leaclsone to doubt the existence of a consistent energy-

~ependent machine effect to explain the discrepan’cieseI

It may be that

resolution problemsI

gain records, sinced

,i

1

closer to agreement

the ~isagreements

in the low ener~y

in many cases the

are lar~ely Aue to

region of the standard

areas could be brought

by taking from one line and adding to ~.

I.

an adjacent line. This problem Is especially troublesome in”I

tryinG to separate the 60, 105, and 140 kev lines on the●

stan~ar~ gain recor~s.

pi

ii 1-i{~

.

A discussion of the overall performance of the system

in analyzin~ the standar~ sources, including the consistency

of the results,ls foun~ in AppenAix I.

DISCUSSION

It Is of special interest to note the presence of Na24

activity in both the Zuni and Havaho C1OU3 samples (the only

samples to reach this section soon enough for such detection

were the cloud samples from each shot). This activity is

evident from the 1.37-an5 2.75-Mev total absorption peaks

~etectable on the first two or three recordings made with

each of these samples.

..__ . . .

. .

. .

-.

i!’

k’ I

.

.

$1>:’:q

f, JI 1-

t

i .,1

.

.

l?a24 1s a major source of radiation hazard in fallout

‘radiationone day~

There aro several possible mechanisms for the production. Iof Na24 by neutron tnduction: A127 (n,a)Na240 ~(n,p) Na24, I

. ●nd Na23(n,y )Na24 with respective oross seetiona of ●bout

100 mb for 14-Mev neutrons, 191*35 mb for 14.6-&w aeutrons

—

I --1,

.

lxmedlately available to pezmlt intelligent speculation on.

which of these processes predominates. ~

Another Interesting result apparent on most of the

series of recordings begun at early enough t-s 1s the

build-up of the 1.59-Msv aotivity from La140. The faot

that there is evidenoe of an increase in this activity at

●arly times indioates that most of the original fission

product of the mass numbe~140 series was Bal*O or a percursor.

Assuming that ●ll of the Ba140-La140 fisston-product oomplex

was Ba140 originally, the build-up of the 1.59-Mev aotivity

should reach its pax_ at

r

the, Theoreti.oally there

136 hours after shot

should be no build-up in

140activity if the original contribution of La to this

.

parent-daughter complex iS more than 11.5 Percent of the

. total activity of the combination. The evidence ln”the

.recor5sof samples whose analysis was begun early enough

for the build-up to show up,polnts toward their being very

little or no La140

produce~ as an instantaneous fission

.

,.

II

*

product. This conclusion Is borne out by studies of fls-23S 12

sicn product yields from U made by Yaffe,et al.~ and

13Petruska et al. , who report yiel~s of 6.32 i 0.24 percent

of Ba’40140 *

and 6.33 A o.32 percent Of @ ,respectively. - -

Since the tlifferenceis zero within experimental error,140

,La is not pro~uced as an original fission product.~------ ---------—--

The samples collected at ground and ship stations may

be different due to fallout fractionation an~ possible

anisotropies In fission-pr~cluctejection from the weapons.3

That there is evidence that one or both of these mechanisms

are operating can be ascertained by comparison of the spec-

tra of samples collected at cllfferentplaces for the same

shot. No pattern is ~lscernible however, with so few sample

collection locations. Therefore it Is not possible to say

anything more than that there seem to be discrepancies be- .

“tweensamples from the same shot which are too large to

e?cpla~nin terms of measurement error alone, e.g.,the 33G

.

.

kev activities present in records QA2 and RA2 (see Table 1,

for notational definitions) differ by more than n factor of

3 in percentagewise contribution, Also the 105-kev actlvi-S

ties In BA7 and GA2 dlff’erby more than a factor of 3.

Dose rates measured 3 feet above the surface of fiw

Island In the vicinity of the collecting sites have been

plotted as a function of time after burst14 for Shot Zunl.

The dose rates calculated from the photon Intensities, listed

In Table 2, of the two samples received from the How Island

.

*

collection stations (GA and IA)S when compand for th - -

proper times with the curve drawn from the measured dose

rates, agree within experimental error-

I

Approved by:

A. GUTHRIEHead, Nucleonlcs Diviston

For the Sclentltic Director

—..-

APPENDIX I STANDARDS CALIBRATION. .

‘:<=-e.-. —.

Calibrate3 standar~ sources were supplied to this

group by Analytical and Standards Branch of Chemical Tech-

nology Division to allow checks to be

ship between area of total absorption

associated photon intensities, and to

macleof the relatlon-

peaks and their

provide standards of

known energy for record by mcor~ energy callbratlono The

calibrate~ standar~s used were ‘75.6 (i4 percent) mlcrocuries

~se The <of Na’22and 145 (t5 percent) microcurles of Hg*

standards were calibrated on my 18, 1956.

In ofier to use these standar~s”to check the correct-.

ness of the I/A versus E curves, corrections had to be made

in the source strengths listed. In the case of Na22 the

standariiswere calibrate~ in temns of positron emission

alone, so that to arrive at the 1.28 Mev photon intensity,

account had to be taken of the 6toll percent electron cap-

ture 15S● When this correction is applied, the original

.

1.28 Mev photon source strength becomes 80.4t0 84.9 “micro-6 6

curies” or 2.9j’ X 10 to3.14 X 10 photons per second. To

compare this number to that obtained by multiplying the

area of the total absorption peak by I/A for 1.28 Mev, the

c area must first be found by extrapolating the decay curve

back through the calibration 3ate. This area is 1.54 (*2 -

30

-7I

.

i

.

.

6percent) square inches and &ives 2.90 X 10 when multlpl~e~

by the proper I/A from Fig. 9. The latter Intensity Is from

2.5to T.6 percent lower than the intensity determined from

the calibration of the stan~ard, but agrees within the

experimental error.

The comparison of the Hg203

photon intensities proceeds

22slmllarly to the Na comparison. The Hg~3 source strength

was given tn actual disintegrations per second but only ‘78.7

of these disintegrations result in 2Tg-kev g~ ~ys bec~203

of the Internal conversion in Hg . After

corrections are made the photon intensities

the extrapolate~ total absorption peak area6

source strength are 4.15 X 10 (*5 percent)

the approprlate-

obtalned from

and calibrated

and 4.22 X 106

(*5 percent) photons per secon~ respectively. The intensi-

ties obtained by the two methods differ by less than 2 percen%

well within experimental error.

‘3.standard and 94With 54 recordings of the 145 PC Hg

22recordings of the 75.6 wc Na standard made over a period

of several months already available, It was decided to make

a lea8t squares flt of the decay curve to get a quantitative

idea of the machiness stability. It was assumed that the

functional form of the equations relating area to time was

A= exp(-~t) or a polynomial of the fom y = a. + alt (a

straight line) where y * lnA.

--

.

.The coefficients ai were found by solution of the

simultaneous equations:

soao + ‘lal = ‘o

slao + s2a1 = ml

Nz Nk# x tn, yn, and N is the number of

where Sk = ~ . ~ * , ‘k ‘n =1—.—._

measured areas. The details are not shown here but the--

results are as follows:*

.For lig203: y = 1.s022 - ooo154t’

For Na22: y = 0.4336- 0oOO14t..

Areas were computed from the equations for each day

“,,, 1

.

that spectra were made and compared with the measure~ areas.203The average devtat~on for Na22 was O.os ln2 an~- f_o~ Hg _ __—---------

!“ . The everege percentage deviation was 2.0 per-was 0.106 in2.—.—

~ent for NS22 end 5.4 percent for Hg203. The probable reason

for the higher deviation for Hg203 is a combination of fewer

records, shorter half life (requiring progressivelymore

..,,, sena’itivecount-rate scales with consequent loss in statis-

tical accuracy during the latter part of the recording

period) and higher amplifier gain requiring the use of more

. sensitive count-rate scales to provide

height●

.

32

peaks of adequate

.I

.

11

i

APPENDIX II THE GAUSSIAN CURVE GENERATOR

The Gaussian curve generator consisted of a Gaussian

template mounted on a lucl.te~isk which In turn was mounted

like a wheel on the shaft of a potentiometer. With a bat-

tery to provide voltage and another potentiometer to vary the.

amount of voltage across the main potentiometer,thepen of

the X-Y recorder was causeQ to move along the X axis as the

wheel was turne~. The range of the pen~s motton during one

revolution of the wheel was governe~ by the setting of th~*-

secondary potentiometer. A photovoltaic cell ‘tLooking”at

a light through the template was connected to the Y axis

of the X-Y recor~er with another potentiometer controlling

its range. As the wheel was turned by hand an~ the amount

of light reachin~ the cell was varied by the template, a

Gaussian curve of height and width, as determined by the

range-controlling potentiometers, was drawn on the recor~er

paper. The template was ma~e of thin, opaque sheet metalI

and Its shape was determines by plotting a Gaussian curve

on polar graph paper.

By this method several hundred Gaussian curves were.

drawn of various heights for each width. The widths were

. chosen to corresp-on5to the widths at half maximum for the

actual energies present in-the fallout spectra as aetermlne~

. from the resolution versus energy curve. .

I

The areas in square Inches of the Gaussian,curves so

drawn were ~etermlneflby measuring their height an~ wi~th

(the same for each series of heights) an~ applying the

formula (derived from the equation for a Gaussian curve):●

A = l,06w~n(0)

where w~.ls the width in inches at half maximum an~ n(o)

is the maximum height in Inches.

:

.

I

.

1-

Q

REFERENCES

●

1.

2.

.

1! 3.

.

.

I

4.

5.

6.

Bouquet, F. L., Kreger~ W.E. B Mather, R. L. , and Cook~ c.s“Application of the Scintillation Spectrometer to Radioactive Fall-Out Spectra Analysis. (Operation UPSHOT. KNOTHOLE),U.S. Naval Radiological Defense Laboratory Report USNRDL-420,31 August 1953 (CONFIDENTML).

‘Cook, C. S. , Johnson, R.F. , Mather, R. L. , Tornnovec, F.M. ,and Webb, L.A. Gamma-Ray SpectralMeasurements of Fall-out Samples from OperationCAST LE o U.S. Naval RadiologicalDefense Laboratory TechnicalReport USNRDL-TR-32 (AFSWH22),26 January 1955 (CONFIDENTmL-RESTRICTED DATA). = -

Webb, L.A., Tornnovec, F- M. ~ Math=c R. L. ~ Johnson~ ROF“ ~and Cook, C.S. Analysisof Gamma Radiationfrom FalloutfromOperationTEAPOT, U.S. Naval RadiologicalDefense LaboratoryTechnicalReport USNRDL-TR- 106, 27 August 1956 (coNFIDENTIAL-RESTRICTED DATA).

Mather, R. L. , Taylor, R.A. , etal.of thislaboratory. Reportinpreparationon OperationTEAPOT instrumentation”.

Ehat, R. F. Base Line Control and Sweep Monitor for SingleChannel Pulse fhalysis, U. S. Naval Radiological Defense LaboratoryTechnical Memorandum No. 55, 7 February 1956.

AppendixC toOperationPlanforProject2.6*3,@eratiOnREDW~G~. .-ll~nm~ of Standard Instrumentation. it

7. ‘Triffet, T. , LaRiviere, P.D. , Evans, E. C., Perkins, W. W. ,and Baum, S. Characterization of Fallout. “V. S. NavalRadiological Defense Laboratory, Project 2.6.3OperationREDWING, Interim Test Report ITR- 1317, February 1957(SECRET-RESTRICTED DATA).

8. White, G. R. X-ray Attenuation Coefficients from 10 kev to100 Mev. National Bureau of Standards Report NBS- 1603,13 May 1952.

35

.

●

..

I.

t!

.

I

9*

10.

11.

12.

13.

14.

15.

16.

Mather, R. L. of this laboratory. Report inpreparation on!lcoll~ator APer~re with Penetration Effects. “

Mather, R. L. of this laboratory. Unpublished data on ~tTheEffect of an integrating Time Constant on the Record of a MovkgChannel Pulse Height Analyser. ‘~

Endt, P. M. and Kluyver, J. C. Rev. Mod. ‘Phys. ~, ~. ~:95(1954

——*

Yaffe, L., Thode,KG., h4erriti,VJ.F.~ HaW~ngs* R.C~~ iBrown, F. and ,BartholomeW,R.M. Can.J.Chem.3&:103.’7(1954).—.—.._-

Petruska, J. A. , Thode,1 H. G., and Tomtison, R. H.Phys. =693 (1955).

Triffet, T. , LaRiviere, ‘P. D. , Evans, E.C. , Perkins, “W. W.,and Baum, S. Characterization of Falhwt, Project 2.6e3SOperationREDWING, Final Report, WT. 131? in preparation,U. S. Naval Radiological Defense Laboratory. *>-

Kreger, W.E. Phys. &J. %:1554 (1954).

Charpak, G. Journale de Physique et Le Radium 16:62 (1 955).—. .—— .

TABLE 1

Miacellaneoua Sample DataSample

Site AbbreviatedDesignation Designation Collector Collector Lcication Weight or Groud Area

Std Hish Type From GA Volume Representation

Gain Gain @Ll)

Shot Cherokee,

.

Filter Paper Cloud

Shot Zuni,

Std Cloud AA

BAFAGA

IAJA

uLAMANA

OAPARA5AQA

TAUAVAWAXAYA

AB

BB

GBHBlBJB

KBLBMBNB

OBPBRB

QB

TBUBVB

XBYB

W;k!’aper %’%ENEocc(b) 13 mi ENE

Occ 52 NNWOcc 13 mi ENE

Std CloudYFNB “Whim” 1How F-61YACI 40 B-19HOW F-67YAG 40 B-6

10 ml1.36 g0.57 g10ml

7;2194.1

62.5I*.4

Filter Paper CloudOcc 29mi NNEOcc 7.5 mi WNW

Std CloudYAG 39 C-36YFNB- 13-E-56YFNB- 13-E- 54

0.02 g10ml

11.514.4Occ

Shot Navaho..

Std CloudYFNB- 13-E-54YFNB- 13-E-56YAG 39 C-21YAG 39 C-36

Filter Paper CloudOcc 8.5 mi WOcc 8.5 mi WOcc 21 mi NNW

0..?8 g10ml10 mI

60:618.036.0

Occ 21 mi NNW

Shot Tewa,.

Filter Paper GAO udStdCloudYAG 39 C-36YFNB- 13-E-56Y3-T-IC-DYFNB- 13-E-54YAG 39 C-21

Occ - 24 NNW 0.02 g 1.2Occ 10mi SW 0.03 g 9.3Seawater(c)Occ 10mi SW 10ml 14. -I

Occ 24 mi NNW 10 ml 14.4

I (a) Picked up at random from deck of YFNB- 29.(b) Open. clooe collector(c) Evaporated sample from large open tank on deck.

.

37

0.54 ● 100.>1. In030.10Q.L* ● !0O.*O ● 110.20. Is0.,6 . to0.1) . 1%0,i7. zo0.,6.8S0.0, ● }0

,1, *LO%.14.30 :,1.1.

008*+C

1.16. b0.70. 10052.100.29 h IZ0.21 ● 100.1, . 100. IZ *400.13*ZS0.0. ● is0.06 . JO0.04 . so

2.55 . 71.04. .s,.s1. 510..100.41 ● 100.2. . Is0.’ 2+.250,02. 400.02 ● 50

0,1 L * 10O.OJ . 10

4. ZL .151.51 ● 150.99 * 43o.a4 . 100,,. . 3.O.is. Jo0..7 ● 300.10 ● 30

0,Z8 h 10O.Q. . 300.93 . 330.0> * .0

0.i6 ● ZOQ.&z * 10

>0

2.)1 ● 1$0.3, ● 1>0.25 ● i>0.17.20::2: ~

0.01 ● 35

0.?,. 10O.oi ● 25

0,;: ● 20

0.01 ● 40

;:b,.1> . 10

0.,1 . 1>0.71 . 13‘.2. . 150.’0. 1!035.30

>0

O.m . Ls0.10 . JO0.0. . ●O0L?5 *40

>0

0.19. 15O..u. to0,0> ● 15

0.35 ● 4.

S,9* ● 94,, b* 71,1). toi..>. . 100,88 * 100,16 . 20J.21 * JOO.ii * 2.3

..:: ● 50>0

..s7 . Zo0.32. . 150.15 ● tc3.0+ ● to0.03 . 40

0.35 * J5O,io ● 1%O.m * 100.,3 ● 490.0, ● w9.’JJ * so

0.0. ● .?3

0.2. . 20O,ti .250,05 . 400.01 ● 40

1.37. 150,. s * 10O.)>.*,0.4 * 440.04. %0

0.11. 100.17 . )5O.tk . !0ol, .i20.1. . !$0.11 ● 130.81 .20010.250.07 . L$0,06 . 100. Q3ti50

0.20 ● MO,, l*ZOO.oa . 1s

>>0>,0>>00.3. * 100.18. 300.,7,>00.06 ● 10

0.09 ● Zo>0

0.07 * as

0.02 i 3“

0.40. 33w

o.07i 20

>0-

>0

>0-

0,04 i 33>0

>0”

>0

I.oa ● 40

>0

>0

2.57* >1.9?. 7,.,J. JO0.?5. 100.57 * 1,03,.1500,.150.0, . 40O,ob . 15

>>0:::. Zo

>0O.n . m0.11. 100.11 . M0,08 ● 150.05. 1s

l,b2 . )2.,?. ),.7, . 5

1,32. 50,14 . 10O.*6 . 200,1! . Lo0.05 . >00.02 . )5

1,>2. 51.1. . 0, ..8 ● Lo,,01 .100.5. . z%018.20.?.25 . .?00.,0 . 300,0. LO

>>0>>0

0.64 . a>>00.10 . 500,,9.44“,).300.04 ● 53

i% ● mO.vi ● uO.*O● 2s0.48 ● 200.32 ● >4O.il. zoO.0* ● MO.oz 6 w

O.M ● 100.07. m

11.** 103.35 ● 74..?8 . 101.07. 1!0,70. 150.54. Zoo.lt . lo0.30 ● >00.22 ● Zo0.19. Zb

U7>*1OO,si ● Is0.10. Z*0.04.40

O.*?* m0.39 ● 150,08 ● 130.05 ● 20

1.91 ● laO,*L . 100.48 ● 100.39 ● 190.13. 150,08 ● Lo0,03 ● 300.01.40

0.66 ● 150.05 ● 10

0.54 ● Lo

0,;: * 200,01 ● M

1.07 ● lo0.14.200,0..400.01.49

O,%* .400,70 ● ,?93,39 ● 4.... ..100..3 ● 30a.G3 . )s

O,)** M0.01 * 150.07. 15L1.az ● +0

0.”7 * M9.02 ● w

0.08. n0,”5 ● 30>.02. w

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3.,8 * )3Z.IJ . )0448.20i.8i *Loi.Ld* 15.l.*k * 20JJ?* 30O.lL ● MG.12 ● >00.23. 15Q.J3 ● m

0.66 ● i$4.4?. Zo0.29 ● MOAl* ,99.10 ● >0

0.s2 . lJO.** . 10D.3L ● 190,16. ?.00.22 ● *J0.02 ● w

0.0, . 20

0.40 ● Ill0.1$ * Is0.18. ao0.+4 ● w

8.36 ● 101>. *Z9Q.*. 109.ZV . 150..7 ● l.!J.., ● ,0

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D., ? ● 150.6>. 1$0.17. 200.05 ● 85O,oza so

0,?. . to0.8% . LO0,51 . 100.%2 . 150.+0 ● 100>1 .,0O.,. *IO0.0. ● 230.01. 30

0...20O.*. . .?00,17 ● t>O., * . 25020.100,12 ● so

0.:: ● M>0

.

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In192Z4L+347*O

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00.:4.:0.09-.w.0.07 . 50

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0.30 ● 100.11 ● M

0.25 . >0O.D, * Lo

9.6$ ● 104.5b ● 53.5$. 50.72. to0.33. 150.31 ● 100.13.200.1. . 100.0, ● >00.07 * a

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2.79. 103.00 ● 02!.lb. loD,#J . 10O.mv. 100.479 100.47 . to0.23. la0.20. M

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>0

0.:: . 10024.300.,2.)00.10 * >0i

1:0,$1.25 - 0.101 )00.10.20 0.05 = ,0O.o& . 40 0.05 * 20 -

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0,! 4.1! O.lm. zo - U::0,27. .!0 0.1>. >0O.iz .).0 ~ O,loi 10 0.054 30J,05 * 30 0.09. .?0 0.06 * w

0,51 . 25U.Z7 * 300.0. . w0.05 ● 30

O.M ● I* 0.2, . 30 0.3+ . 100.59 ● 10 0.Z6* 10 ‘a::; ::0.09* .?} 0.12. 20O.O.* J9 0.07* 10 a.o~. ~

0.16. LS0.09 ● 300.02. 30

>0

0.18. 100.07, 300.04 ● 400,02 . 39

“.37 ● 19.,)0 .15U. LJ *150.,7 ● 10

1.>5. 100.87. 100.)0. M0.02 ● 49

0.78. 50.>4 * 50.05 ● 250,0. ● ,0

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b.a7* )0z.3a . 51.14. *0,76 ● 100,444 100,[3. 150.04 * 130.01. M

0.74. 7o.; * LO - U.OL ● ZO

0.39 * to0.10.15 0,7> ● 40

0,77. .0 :>0 0.03 ● 30

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0,65 ● 300.1, . goO.0* . 7.00.02 ● .s

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>0

0.57. 100.32 ● 100.15 ● 150.10 ● 20

o,5i ● 100.;:. 20 0.109 150.07* .?0 0.113. Lo0.03 ● M 0.02 ● -

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DATE ISSUED:19 July1957