TID-4500, UC-41 Health and Safety

LAWRENCE LIVERMORE LABORATORY LtiwnitY0lCalfoma/Uvern)0ie,CaifQrria/S45fid

UCRL- 51242

ENVIRONMENTAL LEVELS OF RADIOACTIVITY IN THE VICINITY OF THE

LAWRENCE LIVERMORE LABORATORY JANUARY THROUGH DECEMBER 1971

P. H. Gudiksen C. L. Lindeken

0. Gatrousis L. R. Anspaugh

MS. date: June 14, 1972

-NOTICE-Thi5 report was prepared as an account of work sponsored by the United States Government. Neither the United States nor the United States Atomic Energv Commission, nor any of their employees, nor any of their contractors, subcontractors, or their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, com­pleteness or usefulness of any information, apparatus, product or process disclosed, or represents that its use would not infringe privately owned rights.

UlSTIiiiiUiiOli OF THIS DOCUMENT IS UHUMITEQ

Foreword

This report was prepared for submission to the U. S. Atomic Energy Commission by the Environmental Evaluation Section of the Hazards Control Department at the Lawrence Liverniore Laboratory. The analyses of the samples were performed by various groups within the Laboratory, such as the Hazards Control Department Analytical and Radiation Counting Laboratories, the Radiochemistry Division, and the Bio-Medical Division. Data were also obtained from reliable outside sources.

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Contents

Abstract 1 Introduction 2 Environmental Levels of Radioactivity—Livermore Laboratory . . . . 3

Atmospheric Radioactivity 3 Table 1. Airborne particulate activity within the Livermore

Valley during 1971 6 Table 2. Results of gamma-ray spectral measurements of

Livermore Laboratory per imeter air filters . . . 7 Table 3. Plutonium and uranium concentrations in

Livermore Laboratory per imeter air filters . . . 9 Table 4. Inhalation doses resulting from the air

concentrations shown in Tables 2 and 3 9 SoO 10

Table 5. Activity levels of various radionuclides in soil . . . 1 1 Table 6. Deposition levels of various radionuclides in soil . . . 17 Table 7. Concentrations of uranium in soils 20

Laboratory Sewer Effluent . 2 1 Table 8. Livermore sewage treatment plant sampling resul ts

during 1971 22 Water 21

Table 9. Gross beta activities in Livermore water samples . . . 2 3 Table 10. Tr i t ium activities in Livermore water samples

collected during July-December, 1971 24 Vegetation 23

Table 11. Average radionuclide activities in Livermore vegetation samples collected during 1971 . . , . 2 5

Table 12. Tr i t ium activities in Livermore vegetation samples collected during August, October and November, 1971 . . 26

Milk 26 Table 13. Radionuclide activity observed in milk samples

collected during 1971 27 Accidental Release of Tr i t ium Gas 27 Environmental Radiation Measurements 29

Table 14. Environmental radiation background measurements at the Livermore Laboratory per imeter during 1971 . . 30

Environmental Levels of Radioactivity—Site 300 30 Atmospheric Radioactivity 30

Table 15. Airborne particulate activity at Site 300 during 1971 32

Table 16. Results of gamma-ray spectral measurements of Site 300 air filters 34

Table 17. Plutonium and uranium concentrations in Site 300 a i r samples 35

Table 18. Inhalation doses resulting from the air concentrations shown in Tables 16 and 17 . . . . 35

Soil 35 Table 19. Activity levels of various radionuclides in

soil at Site 300 37 Table 20. Deposition levels of various radionuclides

in Site 300 soils 37 Table 21. Concentrations of uranium in Site 300 soils . . . . 3 8

Water 36 Table 22. Average gross beta activities in Site 300 water

samples during 1971 39 Table 23. Trit ium -• tivities in Site 300 water samples . . . . 3 9

Vegetation 38 Table 24. Radionuclide activities in Site 300 vegetation

samples 40 Table 25. Tri t ium activities in Site 300 vegetation samples . . . 4 0

Appendix—Environmental Activity Guide Levels 41 References 42

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ENVIRONMENTAL LEVELS OF RADIOACTIVITY IN THE VICINITY OF THE

LAWRENCE LIVERMORE LABORATORY JANUARY THROUGH DECEMBER 1971

Abstract

An environmental surveillance program is continuing in the Livermore Valley and Site 300 areas to determine to what extent, if any, the Lawrence Livermore Laboratory has contributed to the levels of radioac­tivity in the surrounding environment. The resul ts of analyses for gross radioactivity and for specific radionuclides of interest in a variety of environmental samples are presented in the repozt. Environmental levels of radioactivity were found to bo below the concentration guide levels in A EC Manual Chapter 0524.

Airborne particulate samples showed gross beta activities s imi lar to those measured during previous yea r s . Gamma spectral measurements of these samples revealed detectable activities of typical gamma emitters observed in global fallout, including fresh fission product debris from the 1970 Chinese a n i French nuclear weapons tes ts . Isotopic uranium analyses of airborne particulates collected at Site 300 indicate that the uranium was

235 depleted in U with respect to natural uranium. This is most likely due to the resuspension of the depleted uranium that has been distributed over the Test Facility as a result of high explosive detonations. The actual airborne ura­nium concentrations, however, were well within the stringent standards set by the AEC. Soil samples collected within the

Livermore Valley and Site 300 were sub­jected to uranium, plutonium, strontium and gamma spectral analyses, which showed that the only activity contributed by the Laboratory was some low level 239

Pu contamination in one small on-site a rea and in one of the holding ponds at the Livermore Sewage Treatment Plant where the Laboratory's liquid effluent is proc­essed. Samples of this effluent were also collected at various stages throughout the treatment plant to detect any possible build-up of activity within the facility. Gross activity analyses indicate that the radioactivity is mainly associated with the solids present in the effluent, hence, the digesters show the highest beta activ­ities with attendant decrease of activity as the efluent moves through the plant. Gamma spectral analyses of milk and vegetation samples revealed no gamma -emitting radionuclides other than those present naturally or in global fallout. The resul t s of the tritium analyses of vegeta­tion samples revealed significant variation from one location to another which may be due to Laboratory operations. The activ­i t ies of samples collected on-site and in off-site a reas generally downwind from the Laboratory are up to 2 orders of mag­nitude higher than those observed in areas where the labora tory ' s contribution should be minimal. However, in spite of these

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variations, the activities a r e still within recommended standards. Water samples collected in the Livermore Valley exhibited normal gross beta and tr i t ium activities, as did those from Site 300, except from one spring with water containing tritium activities that a re about 4 orders of mag­nitude (but less than 1% of standard) greater than the others. This may be due to tritium being leached out of contaminated waste stored nearby. The off-site radiation ex­posure rates measuredbythermoluminescent dosimeters were within the range to be expected from natural radiation sources.

The Lawrence Livermore Laboratory is located about 50 miles southeast of San Francisco in the Livermore-Amador Valley. Shielded from the ocean by the western hills, the valley has a warm, dry climate. Annual rainfall is about 3 4 inches and occurs primari ly during the winter months in connection wiib Pacific s torms. Surface water drainage from the valley is from east to west through various arroyos, with outflow near Sunol in the southwestern corner of the valley. Prevailing winds a re from the west and southwest during April through September and from the northeast during the remainder of the year.

The Livermore Laboratory occupies an a r ea of 1 square mile, situated approximately 3 mi les east of Livermore. The Laboratory plays an integral part in the nation 1 s nuclear weapons development program and makes diversified researches into controlled thermonuclear reactions, industrial appli­cations of nuclear explosives, and the effects of radiation on the biosphere.

Assessment of the doses to an individual frcm the observed environ­mental activities indicates the contri­bution from artificially produced radio­nuclides is small in comparison with that from natural p rocesses . An adult who breathes air, drinks water and milk, and eats vegetation containing the activities shown in this report will receive less than 1 m r e m / y r from the artificially produced radionuclides,

144 with the exception of Ce, which may deliver s tvera l m r e m / y r to the organs of interest.

Much of the mater ia l s testing and high-explosive diagnostic work of the Laboratory is car r ied on at Site 300, a 10 square mile a rea about 13 miles southeast of Livermore in the sparsely populated hills of the Siablo range which separa tes the Livermore and San Joaquin Valleys.

In order to ca r ry out these programs, the Laboratory handles a variety of poten­tially hazardous radioactive materials . A s t r ic t effluent control program, which places maximum emphasis on controlling the effluents at the source, has been in continuous existence since the Laboratory began operation. To ensure that this effluent control program is indeed res t r i c t ­ing the release of radioactivity from the Livermore Laboratory and Site 300 to concentrations below the standards set forth by the U. S. Atomic Energy Commis­sion, an environmental surveillance pro­gram is conducted. This program is capable of detecting increases in radio­activity above natural environmental

Introduction

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background levels as a resul t of Laboratory operations. The program includes the collection of airborne part iculates, soil, water, sewer effluent, milk, and vegeta­tion samples. These samples a re analyzed for gross radioactivities as well as for the activity of specific radionuclides of interest . In addition, environmental background radiation is measured at numerous locations in the vicinity of the Livermore Laboratory by means of thermoluminescent detectors.

The resul ts of the analyses a re pro­vided in this report. When appropriate for the sake of brevity and clarity only the

ATMOSPHERIC RADIOACTIVITY

The concentrations of various airborne radioactive substances were measured at 16 a i r sampling stations situated through­out the Livermore Valley. Their locations a re shown in Figs. 1 and 2. The six samplers located on the Laboratory per imeter use 80 square-inch Whatman 41 fi l ters. The average sampling ra te is 25 cfm. The remaining samplers , located off-site, use 36 square-inch HV-70 (cellulose-asbestos) fi l ters and operate at an average flow rate of 4 cfm. These air samplers are situated in such a man­ner that they provide a reasonable assurance that a significant re lease of airborne particulate radioactivity from the Laboratory would be detected regard­less of the local meteorology at the time of the re lease . Fi l ters a re changed weekly during the winter months and twice weekly during the summer to avoid

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maximum and average concentrations are given. E r ro r limits, when included, only reflect the uncertainties in the analyses at the 68% confidence level due to counting s ta t is t ics . An attempt has been made to a s se s s the impact resulting from the ob­served environmental activity levels of artificially and naturally produced radio­nuclides by calculating the whole body or cr i t ical organ doses that may be delivered to an adult by the various radionuclides of interest . Thus, one may in a limited manner compare the dose produced by man 1 s activity to that produced by nature.

excessive mass loading. An automatic radiation detection system with gas flow proportional detectors is used to deter­mine gross alpha and beta activities deposited on the filters after radon decay. The fi l ters are also assayed for gamma-emitting radionuclides by means cf a specially designed Ge(Li) detector equipped with a Compton suppression sys tem.

No gross alpha activity above the 0.001 pCi /m detection limit was ob­served on the filters. The gross beta activities averaged over three-month periods and tlie annual average activities a re shown for each sampling location in Table 1, where they may be compared with the appropriate recommended con­centration guide (RCG). In addition, the weekly average beta activities on the air fi l ters from all the Livermore stations a re shown in Fig. 3. A significant fraction of the beta activities deposited

Environmental Levels of Radioactivity — Livermore Laboratory

:i <fr^W iM..

C~) Air sampling stations 2\ Sewage sampling points I I Water sampling points Q_/ Vegetation sampling areas

TER J '

t-r- v ,i . . .. . . a • f-? . V i -' r * ^ '

% , i I »

+ >,© - 4^fch©E

Valley •5?* / A f 1A

Livermore

X\ ?*J,, < J - ^ ^ , / . .,- ^~;....:JijZ/? ' . -: v . ' - - . c- . - -f-

2 l f - « . ^ ' - ' - • • > : " "" ;• ' ' ^ ^ i p , ~ . • ••'""'''' v ~. .v7 .-;i" /f>-L •- - .-:. ^ ' ^

Fig. 1. Lawrence Livermore Laboratory off-site environmental sampling locations.

v; on the fil ters is due to global fallout produced by nuclear weapons t e s t s and by cosmic-ray interactions with the a tmos­phere. This is shown in Table 2 which l is ts the activities of the more abundant gamma-emitting radionuclides in monthly composite samples collected by the six Laboratory perimeter sample r s . These data exhibit the typical spring increase in

surface a i r radioactivity due to the en­hanced transport of relatively high activity s t ra tospheric air into the troposphere during this time of year . In addition, the data shows the influence of the French and Chinese atmospheric nuclear weapons t e s t s of 1970 which injected significant quantities of fresh debris into the s t ra to­sphere . This is illustrated in Fig. 4 by

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S . fl a, \\R. a I

Fig. 2. Lawrence Livermore Laboratory on-site enviromnental sampling locat 'ons.

analyses by dry ashing and complete dis­solution of the filtsrs and subsequent radiochemical separation of the elements. The plutonium was isolated by ion exchange techniques and detected by alpha spec­t rometry . The isotopic uranium analyses were performed by mass spectrographic methods. The results a re provided in Table 3. Inspection of the data reveals

the Z r / Cs ratios which increased to a maximum value during ine spring, due to the addition of relatively large

95 quantities of ' Zr from these t e s t s and then decreased at ?. ra te approaching the 65 day half-life of Zr as e'cpected with little o r no further addition of fresh debris.

These monthly composite samples were also subjected to plutonium and uranium

Table 1. Air borne particulate activity within the Livermore Valley during 1971.

G r o s s b e t a a c t i v i t y ( p C i / m )

Sampl ing J a n u a r y - . klarch Apr i l - J u n e J u l y - S e p t e m b e r

M a x i m u m Average O c t o b e r - D e M a x i m u m

c e m b e r A v e r a g e

Annual a v e r a g e

P e r c e n t R C G °

Sampl ing ?.i>x c i u m A v e r a g e Maximum A v e r a g e

J u l y - S e p t e m b e r

M a x i m u m Average O c t o b e r - D e M a x i m u m

c e m b e r A v e r a g e

Annual a v e r a g e

P e r c e n t R C G °

1 0 .45 t 1% 0.10 0.24 ± 1% 0 .18 0.22 ± 4 7 , 0 .13 0 .090 ± 2% 0.050 0.12 12 2 0 .25 r 1% 0.083 0.25 ± 1% 0.18 0.22 ± 1% 0.12 0.12 ± 5% 0.042 0.11 11 3 0 .15 X 6% 0 .073 0.17 ± 3 % 0 .13 0 .15 ± 3 % 0.083 0 .044 ± 9% 0.027 0.080 8 4 0.55 ± 2% 0.14 0.31 ± 2% 0.23 0 .29 ± 2% 0.16 0 .083 ± 5% 0.056 0 .15 15 5 0.34 ± 2% 0.084 0.26 ± 2 % 0.16 0 .22 ± 2% 0.11 0 .040 ± 10% 0.026 0 .095 10

a 0.30 ± 2% 0.14 0.17 ± 3 % 0 .12 0 .28 ± 2% 0.093 0 .051 ± 8% 0.031 0.096 10 7 0.05J ± 12% 0.031 0.16 ± 3 % 0.12 O.l.i 1 3% 0.075 0 .051 ± 87. 0.027 0.063 6 8 0.10 ± 6% 0.042 0.24 ± 2% 0.13 0.19 ± 3 % 0.091 0 .053 ± 7% 0.023 0.072 7 9 0.35 ± 2% 0.098 0.22 ± 3 % 0.18 0.19 ± 3 % 0.10 0 .071 ± 67. 0.040 0.11 11

10 0.13 ± 3% 0.096 0.24 ± 2% 0 .13 0.13 ± 3 % 0.067 0 .050 ± 87o 0.027 0.080 8 11 0.31 ± 2% 0 .073 0.19 ± 3% 0.12 0 .18 ± 3 % 0.071 0 .049 ± 8% 0.024 0.072 7

12 0.4:. ± 1% 0 .11 0.28 ± 1% 0 . 2 1 0.29 ± 2 % 0.15 0 .089 ± 3% 0 .051 0 .13 13

13 0.33 + 2% 0.10 0.28 ± 1% 0.19 0.22 ± 2% 0.13 0 .15 ± 2% 0.053 0.12 12

14 0.81 ± 1% 0.20 0.56 ± 1% 0 . 4 1 0 .45 ± 2 % 0.26 0 .15 ± 27„ 0.080 0.24 24 15 0.38 ± 1% 0.097 0.26 ± 1% 0 .19 0.24 ± 2% 0.13 0.09 ± 3% 0.048 0 .12 . 12 16 o.;.3 ± 2% 0 .11 0.24 ± 3% 0 .16 0 .22 ± 3% 0.10 0 .064 ± 67° 0.037 0.10 10

a See Figs. 1 and 2 for sampling locations. b The RCG is 1 p C i / m 3 .

U

0.1 -

0.01

Fig. 3. Weekly average beta activities on a i r filters from Livermore sampling stations.

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Table 2. Results of gamma-ray spectral measurements of Livermore Laboratory perimeter air filters (activities in pCi/m3).

1 4 4 c e 1 4 1 C e 1 2 5 S b 7 B e 1 0 3 R u 106-Ru 1 3 7 C s 9 5 Z r

January 9 ,BX10' 3 ±3.% 3 .4X10~ 3 ± 8% 7.8X10" 4 ±18% 5.5 X 10" 2 ±4% 3 .9X10~ 3 ± «% 3 .6X10" 3 ±25% 9.8 X 10" 4 ± 9% 3 .PX10" 3 ±4%

February 1 .6X10" 2 ±3% 4 . 9 X 1 0 " 3 ± 5% 1.3X10" 3 ±20% 5.4 X 10" 2 ± 5% 7.1 X 10" 3 ± 8% 6.2X10" 3 ±26% 1.2X10" 3 ±12% 7.6 X ID" 3 ±3%

March 4 . 7 X 1 0 " Z ± 1 % 1.8X10~ 2 ± 2% 2 . 8 X 1 0 " 3 ± 1 1 % B.3X10" 2 ±4% 2.6 X 10" 2 ± 2% 2 .1 X1 0 " 2 ± g% 3.6 X 10" 3 i 5% 3.6 X 10" 8 ± 1%

April 6 . 2 X 1 0 " 2 ± 1 % 1.5X10" 2 ± 2% 3.3 X 1 0 " 3 ± 15% 0.8 X 1 0 " 2 i 5 % 1.6 X 10~ 2 ± 3% 2.8 X 10" 2 ±12% 4.6 X 10" 3 ± 6% 5.D X 1 0 " 2 ± 1 %

May 1.4 X 1 0 _ 1 ± 1 % 2 . 0 X 1 0 _ 2 ± 2% 9 .2X10" 3 ± 1% 1.3 X 10" 1 ±4% 4,0 X 1 0 " 2 ± B% 4 . 8 X 1 0 _ 2 ± 9% l .QX10" 2 ± 5% 9.5 X 10" 2 ± 1%

June 7.3 X 10~ 2 ±2% 7 . 3 X 1 0 " 3 ± 6% 3.7 X 10~ 3 ±22% 5.7 X 10" 2 ±9% 1.4 X 1 0 " l ± 5% 3.2 X 1 0 " 2 i 17% 5.0 X 10~3 ± 10% 3.7 X ID" 2 ±2%

July 6 . 8 X 1 0 _ 2 ± 1 % 3 . 8 X 1 0 - 3 ± 1 2 % 3.5 X 10" 3 ± 10% 6.3 X 10~ 2 ±6% i . i x i o ~ 2 ± 7% 2 .9X10~ 2 ± 7% 4 . 6 X 1 0 " 3 ± 5% 3.0 X 10" 2 ±2%

August 1.0 X 10" 1 ± 1% 2 .2X10" 3 ±19% 6 .6X10" 3 ± 9% 1.6 X 1 0 _ 1 ± 3 % 7.7 X 1 0 " 3 ± 8% 4.3 X 10" 2 ± 8% 7 ,1X10~ 3 ± 5% 3.4 X 10" 2 ±2%

September 5 .6X10" 2 ±2% 1.8X10" 3 ±25% 4.0 X 10 " 2 ± 14% 1.8 X l f l " 1 * ^ . 2.8 x i o " 3 ± ; 20% 2.2 X 1 0 " 2 ± 15% 4 . 3 X 1 0 " 3 ± 8% 1.3 X 10" 2 ±3%

October 1 .5X10" 2 ±3% 6.4X10" 4 ±27% 9.7 X10" 4 ±26% 8.2 X 10" 2 ±4% 4.8 X 10" 4 ±42% 1.0X10" 2 ±10% 1.3X10" 3 ±12% 3.3 X 10" 3 ± 5%

November 3 . 4 X 1 0 " 2 ± 3 % 5.3X10" 4 ±58% 2.5X10~ 3 ±22% 2 . 2 X 1 0 " 1 ± 3 % i . 6 x i o " 3 ± : 32% 1.6 X 10" 2 ±17% 2.7 X 1 0 " 3 ± 11% 5.5X 10" 3 ±5%

December 5.5 X 10" 3 ± 4% 5 .4X10" 3 ± 2% 5.1 X 10~ 4±27% 4,OX10" 2 ±4% B.2X10" 3 ± 3% 1.3 X 10~ 3±32% 6.1 X 1 0 " 4 4 11% 8.9 X 10~ 4 ±7%

Annual average 5.2 X 10" 2 6.9 X 10" 3 3.3 X10" 3 1.0 X 1 0 _ t 2.2 X 10~ 2 2.2 X 10" 2 3 .8X10" 3 2.6 X 10" 2

RCG a 2X 10 2 5X 10 3 9 X 1 0 2 4 X 10 4 3 X 10 3 2 X 1 0 2 5 X 1 0 2 IX 10 3

Percent RCG 2.6 X 10" 2 1.4X10" 4 3.7 X 1 0 " 4 2.5 X 10" 4 7.1 X 1 0 " 4 1.1 X 1 0 " 2 7.8 X 10" 4 2.6 X 10" 3

Assumes the activity is in an insoluble form.

Fig. 4. The measured 9 5 Z r / Cs activity ra t ios on air filters from LLL perimeter samplers.

238 that the relative activities of Pu and 239

Pu approximate those normally ob-

the recent atmospheric weapons tes ts , as poo

-wall as depletion of the Pu produced served in global fallout. The decreasing by the 1964 SNAP generator burn-up. The values of the ratio undoubtedly a re a

239

po e 2SR TJ/ V ratios approximate the values

resul t of the addition of f resh Pu from observed in natural uranium.

Table 3. Plutonium and uranium concentrations in Livermore Laboratory perimeter air filters.

Act iv i ty ( p C i / m 3 )

2 3 S P u / 2 3 9 P u

3 M a s s ( n £ / m )

1971 Month 2 3 8 P u 2 3 9 p u 2 3 S P u / 2 3 9 P u 23 5 D 2 3 8 D 235JJ.23BJJ

J a n u a r y 3.4 X 1 0 " S ± 6% 2.4 X 1 0 " 5 ± 3 % 1.4 X i O " 1 2.2 X I O " 4 ± 2 % 4.7 X 1 0 " 2 ± 1% 4.7 X 1 0 " 3

F e b r u a r y 8.3 X 1 0 " T ± 6% 9.2 X 1 0 " 6 ± 3% 9.0 X 1 0 " 2 7.0 X 1 0 " 5 ± 1% 1.0 X 1 0 " 2 ± 2% 6.8 X 1 0 " 3

M a r c h 3.6 X 1 0 ~ 5 ± 6% 3.4 X 1 0 " 4 ± 4 % 1.1 X I O " 1 1.3 X 1 0 " 3 ± 1 % 1.7 X 1 0 " 1 ± 1% 7.6 X 1 0 " 3

A p r i l 9 .1 X 1 0 " 6 ± 7% 7 .9 X 1 0 ~ 5 ± 4 % 1.2 X 1 0 " 1 2 . 5 X 1 0 " 4 ± 1% 3.6 X 1 0 " 2 ± 2% 6.9 X I O " 3

May 5.7 X 10 " S ± 7% 1.1 X 1 0 " 4 ± 4 % 5.4 X 1 0 " 2 6.3 X 1 0 " 4 ± 1% 1.0 X 1 0 " 1 ± 1% 6.3 X 1 0 " 3

J u n e 3 .4 X I O " 6 ± 1 0 % 7.6 X I O " 5 ± 5 % 4 . 5 X 1 0 " 2 3.3 X 1 0 " 4 ± 2% 4 .9 X 1 0 " 2 ± 2% 6.6 X 1 0 " 3

Ju ly 3.0 X 1 0 " 6 ± 10% 6.5 X I t ? " 5 ± 5% 4.6 X I O " 2 4 .7 X 1 0 " 4 ± 1% 7.4 X 1 0 " 2 ± 2% 6.3 X 1 0 " 3

Augus t 2.2 X 1 0 " 6 ± 10% 4.7 y. 1 0 " S ± 5% 4.7 X 1 0 " 2 4 . 2 X 1 0 " 4 ± 1% 6.2 X 10 " 2 ± 2 % 6.6 X 1 0 " 3

S e p t e m b e r 2.1 X I O " 6 ± 1 7 % 4 .9 X 1 0 " 5 ± 4 % 4.3 X 1 0 " 2 2 .6 X 1 0 " 4 ± 1% 3.6 X 1 0 " 2 ± 1% 7.2 X 1 0 " 3

O c t o b e r 1.5 X 1 0 " 6 ± 15% 2.6 X 1 0 ~ 5 ± 6 % 5.7 X 1 0 " 2 3.0 X 1 0 " 4 ± 1% 6.4 X 1 0 ' 2 ± 1% 4.7 X I O " 3

N o v e m b e r 1.1 X 1 0 " 6 ± 14% 2.7 X 1 0 " 5 ± 4 % 4.1 X 1 0 " 2 4 .7 X 1 0 " 4 ± 1% 4.7 X 1 0 ' 2 ± 1% 1.0 X 1 0 " 2

D e c e m b e r 3.0 X 1 0 " 7 ± 12% 4 . 7 X 1 0 " 6 ± 4 % 6.4 X 1 0 " 2 4 . 7 X 1 0 " 5 ± 1% 6,7 X 10 " 3 ± 2 % 7.0 X 1 0 " 3

Annual a v e r a g e 5.7 X I O " 6 7.1 X I O " 5 4 .0 X 1 0 " 4 5,8 X 1 0 " 2

R C G a 1.0 1.0 1.9 X I O 3 l .S X 1 0 4

P e r c e n t R C G 5.7 X 1 0 " 4 7.1 X 1 0 " 3 2 .1 X I O " 5 3.9 X 1 0 " 4

Assumes the activity is in an insoluble form.

The calculated annual lung doses to an adult resulting from inhalation of the radionuclides listed in Tables 2 and 3 a re shown in Table 4. These were obtained

2 by using the ICRP Lung Model, and making the following assumptions:

• The radionuclides a r e present in an insoluble form,

• The mean particle activity diameter is one micron, and

« The activities of the radionuclides within the various body organs have attained equilibrium.

We feel the first two assumptions are reasonable in view of the fact the activities may be situated in insoluble silicate matr ixes within part icles that may range in s ize from one-tenth to severa l microns in diameter . This is the range usually observed in air pollution studies. Also,

Table 4. Inhalation doses resulting from the air concentrations shown in Tables 2 and 3.

Calculated annual Radionuclide lung dose (mrem)

1 4 4 C e 2.6 i 4 1 C e 4.8 X 10" 2

1 2 5 S b 3.2 X 10" 2

7 B e 6.4 X I O " 2

1 0 3 R u 2.2 X 10" 1

1 0 6 R u 3.6 X1C" 1

1 3 7 C s 6.0 X 10~ 2

9 5 Z r 5,4 X 1 0 " 1

2 3 8 p u 1.2 X I O " 2

2 3 9 p u 1.4 X 1 0 " 1

23 5V 1.6 X 10" 3

2 3 8 u 3.2 X 10" 2

9-

since global fallout has been with us fc: upwards of two decades, the third assump­tion should be valid for most radionuclides since their half lives in the lung are short relat ive to the long exposure t ime. The data in Table 4 shows that the resulting inhalation doses a re minor with the greatest contribution (2.6 mrem) being

144 due to **Ce.

SOIL

A soil sampling program is currently underway to determine the surface distr i ­bution of various radionuclides that have been deposited within the Livermore Valley as a result of global fallout from atmospheric weapons tes t s as well as from possible Laboratory effluents. A core sampling method was used to obtain the soil samples at various depths down to 20 cm for activity/depth profile studies. Each sample was collected over a surface

2 2 area ranging between 250 cm to 1000 cm by combining a minimum of 10 separate

2 cores obtained over an approximate 30 m area .

The samples were thoroughly dried and homogenized before undergoing analyses for the radionuclides of interest . During the initial phases of the program, a mini­mum of 50 grams of soil were subjected to either the HASL acid leach method or a complete dissolution method by various outside contractors for the analysis of 2 3 8 P U j

2 3 9 P u , and 9 0 S r . Analysis of the leach residues from severa l samples for quality control purposes indicated that approximately 90% of the total plutonium activity in the samples was removed by this leach method. However, because of the possibility of large variations in the

chemical and physical state of the pluto­nium that may '-ppear in the environment, a capability was developed within LLL to completely dissolve 100-gram soil samples by acid dissolution techniques to gain in­c reased analytical sensitivity and sample homogeneity. Standard ion-exchange techniques and alpha pulse height analyses a r e used to quantitate the plutonium con­tent of the soil. Gamma spectral analyses were made by placing approximately 300 g rams of soil on a Ge(Li) detector equipped with a Compton suppression sys­t em. These analyses provided quantita­tive data regarding the concentrations of 1 3 7 C s , 1 4 4 C e , 9 5 Z r , and 4 0 K in Livermore soils.

The resul ts of the analyses a re pro­vided in Table 5, and the sampling loca­tions a r e shown in Fig. 5, The depth profile studies at sampling Locations 9, 10, 11 and 15 indicate the artificially p ro ­duced radionuclides do penetrate appre­ciably into the soil, probably as a result of leaching or mechanical mixing. Gen­eral ly the activity in the 15-20 cm layer is about a factor of 10 l e s s than that in the top 1-cm layer, although wide varia­tions may be observed. As expected, the

40 activity of K seems to be distributed fairly homogeneously with depth. Our analytical techniques generally made it

239 possible to detect the activities of Pu, 9 0 S r , 1 3 7 C s , and 4 0 K to a sampling

95 depth of about 20-30 cm, while Zr and 144

Ce could only be detected in the top 1-cm layer . The resulting deposition values a re shown in Table 6. Most of

23° the "Pu deposition levels a re of the order of 1 mCi/km , but some locations indicate values that a re appreciably higher. For instance, the elevated levels -10-

Table 5. Activity levels of various radionuclides in soil (pCi/g).

to£C ?cm)h 2 3 B P U

2 3 9 P u 9°Sr 1 3 7 C s 9 5 Z r " 4 C e 1°J<_

l a 0-1 4 . 8 X 1 0 " 1 ± 6% 2.6 ± 16%

0-24 5 . 8 X 1 0 " 3 ± 5% 5 . 8 X 1 0 " 2 ± 4% 1.5 X 10" 1 ± 13% 2.6 ± 16%

2 a

3 . S X 1 0 " 3 ± 5% 8 . 8 X 1 0 " 2 ± 4%

0-15 2 . 2 X 1 0 " 2 ± 2% 3 . 4 X I o " 2 ± 2% 1.5 X 10" 1 ± 7% 2.9 X 10" 1 ± 10% 4.8 ± 12%

3 a 0-15 1 . 5 X 1 0 " 2 ± 3% 1 . 0 X 1 0 _ 1 ± 3% 1.4 X 10" 1 ± 4% 2.2 X 10" 1 ± 12% 4.6 ± 12%

4 a 0-15 8 . 6 X 1 0 " 2 ± 3% 3 . 0 X 1 0 _ 1 ± 3% 1.0 X 10" 1 ± 2% 1.6 X 10" 1 ± 14% 3.9 ± 14%

5 a 0-15 2 . 7 X 1 0 _ 1 ± 4% 8 . 6 X 1 0 _ 1 ± 4% 1 . 1 X 1 0 " 1 ± 7 % 1 . 9 X 1 0 _ 1 ± 1 2 % 4.6 ± 12%

6 a 0-15 2 . 4 X 1 0 " 3 ± 5% J>,5X10" 3 ± 3% 1 . 4 X 1 0 _ 1 ± 7% 1.6 X 1 0 ' 1 ± 12% 2.7 ± 15%

7 a 0-15 4 . 2 X 1 0 " 3 ± 3% 1 . 3 X 1 0 " 2 ± 3% 1 . J X 1 0 " 1 * 4% 1.6 X 10" 1 dfc 12% 3.3 ± 12%

8 0-15 1.3 X 10" 3 ± 5% 8.6 X 10" 3 ± 3% 8.2 X l O - 2 ± 13% 1.6 X 10" 1 ± 12% 5-0 ± 1 0 %

9 „_ ! 1.0 X 10" 2 ± 14% 1.8 X 10" 1 ± 13% 2.8 X 10" 1 ± 8% 5.3 X 10" 2 ± 20% 1.4 X 10" 1 ± 34% 1.3 X 1 0 1 ± 5%

! . 5 7 . 7 X 1 0 " 3 ± 1 2 % l.OX 10" 1 ±20% 3.6 X 1 0 _ 1 ± 7% 1 .1X10 ± 6%

5-10 3 . 2 X 1 0 ' 3 ± 3 5 % 1 . 0 X 1 0 " 1 ± 2 0 % 1.3 X 10" 1 ± 16% 1 .2X10 ± 7%

2 . 3 X 1 0 " 3 ± 2 0 % 5 . 5 X 1 0 " 2 ± 2 5 % 1 .3X10 ± 6%

6 . 4 X 1 0 " 3 ± 2 2 % 1 . 8 X 1 0 " 2 ± 2 5 % 3.7 ± 14%

1 0 0 . ! 6 . 8 X 1 0 - 3 ± 5% 1 . 6 X 1 0 _ 1 ± 3% 3.6 X 1 0 _ 1 ± 7% 6.2 X 1 0 - 2 ± 17% 1.4 X 1 0 " 1 * 5% 1 . 2 X 1 0 ^ 6%

1-5 5 . 0 X 1 0 " 3 ± 5% 1 . 0 X 1 0 _ 1 ± 3% 1.9 X 10* 1 ± 11% 1 .4X10 ± 5%

5-10 3 . 3 X 1 0 " 3 ± 7% 1 . 0 X 1 0 " 1 * 3% 2.0 X 10" 1 ± 13% 1 .1X10 ± 7%

10-15 1 . 4 X 1 0 " 3 ± 1 2 % 5 . 0 X 1 0 " 2 ± 3% 6.1 X l O " 2 * 29% 1 .1X10 ± 7%

15-20 7.3 X 10" 4 i 13% 1.7 X 10" 2 ± 5% 3.3 X 10" 2 ± 43% 1.3 X 10 ± 6%

11 0-1 1 . 0 X 1 0 _ 3 ± 3 2 % 9 . 6 X 1 0 _ 3 ± 7% 2 . 0 X 1 0 _ 1 ± 1 B % 3 . 4 X 1 0 " ^ 8% 4 . 7 X 1 0 _ 2 ± 2 7 % 2 . 0 X 1 0 " 2 ± 3 3 % 1.1 X 10 1 ± 6%

1-5 3.3 X 10" 4 4 59% 8.2 X 10" 3 ± S% 1.3 X 10" 1 ± 18% 2 . 7 X 1 0 _ 1 ± 1 0 % 9.9 ± 8%

5-10 7 . 7 X 1 0 " 4 ± 3 6 % 7 . 7 X 1 0 " 3 ± 7% G . 0 X 1 0 " 2 ± 2 1 % 9 . 6 X 1 0 " 2 ± 2 1 % 1 .2X10 ± 7%

10-15 9 . E X 1 0 ' 4 ± 2 8 % 1.6 X 1 0 " 2 * 6% 5.0 X 1 0 * 2 ± 18% 4.6 X 10" 2 ± 35%

15-20 2 . 1 X 1 0 " 4 ± 9 9 % 4 . 6 X 1 0 " 3 ± 8% 1.0 X 1 0 " 2 ± 50% 9.9 ± 8%

10-15

15-20

Table 5. (Continued) Sampling location

Depth (cm) 238 Pu 2 3 9 P u 9 0 S r 1 3 7 C s 9 5 Z r l 4 4 C e 4 0 K

12 0-1 6.8 X 10 " 4 ± 1 3 % 8.2 X 1 0 " 3 ± 4% 1 . 0 X 1 0 _ 1 ± 2% 1.8 X 1 0 " 1 * 1G% 7.0 X 10" 2 ± 24% 4.6 X 10"'±22% 9.9 ± 48%

1-15 1.0 X 10 '* ± 40% 2.7 X 1 0 ~ 3 ± 4% 6.7 X 10" 2 ± 2% 6,3 X 10" 2 ±24% 1.9 ± 20%

13 0-1 3.3 X 10 " 4 ± 25% 5.1 X 10" 3 ± 4% 1.5 X 1 0 _ 1 ± 2% 2.3 X 10" J ± 11% 1.3 X 10"'± 12% l . G X 1 0 " 1 ± 4 8 % 3.0 ± 15%

1-15 1.0 X 10 '* 140% 2.5 X 10" 3 ± 4% 7 . 5 X 1 0 " 2 ± 2% B.7X 10" 2 ± 17% 4.1 ± 10%

14 0-1 7.3 X 10 ' 4 ± 10% 7.1 X 10" 3 ± 3% 1.8 X 1 0 " 1 * 2% 2.3 X 10"'± 13% 1.3 X 10" 1 ± 14% 5.7 X 1 0 _ 1 ± 16% l.B ± 26%

1-15 0.3 X 10' 5 ±54% 2.8 X 10" 3 ± 5% 7.5 X 1 0 " 2 ± 2% 5.7 X 10" 2 ± 25% 2.1 ± 18%

IS 0-1 1 . 2 X 1 0 ' 2 ± 5% G.7 X 10" 2 ± 6% l .BX 1 0 " l ± 15% l .BX 10" l ± 13% 5.9 X I 0 _ 1 ± 19% 1.2 ±41%

1-5 5.4 X 10* 3 ± 6% 5.5 X 1 0 " 2 ± 5% 9 . 5 X 1 0 " 2 * 17% 3.D ± 12%

5-10 2.9 X 1 0 " 3 ± 7% G.3 X 10" 2 ± 4% 8.8 X 10" 2 ± 19% 3.5 ± 14%

10-15 2.5 X 1 0 * 3 ± 8% 5.3 X 1 0 " 2 ± 5% 8.9 X 10" 2 ±21% 3.0 ± 17%

15-20 1.0 X 1 0 * 3 ± 10% 3 . 0 X 1 0 " 2 ± 4 6 % 4.4 ± 12%

16 0-1 7.1 X 1 0 ' 3 ± G% 1.1 X 1 0 _ 1 ± 3% 1.8 X 10" 1 ±18% 1.4 X 1 0 _ 1 ± 2 1 % 3.2 X 10"'±38% 5.1 ± 1G%

1-20 1.2 X I 0 " 3 ± 8% 4 . 8 X 1 0 " 2 ± 4% 3.4 X 10" 2 ±34% 5.6 ± 8%

20-25 6.0 X 10" 4 * 20% 2.4 X 1 0 " 2 ± 7% 6.G ± 9%

17 0-1 1.1 X 1 0 " 2 ± 5% 6.8 X 10" 2 ± 3% 2.1 X 10" *± 14% G.2X 1 0 " 2 ± 2 3 % 3.0 X 19%

1-20 3.6 X 1 0 " 3 ± 10% 8.4 X 1 0 " 2 ± 5% 8.7 X 10" 2 ± 20% 3.G ± 14%

20-25 1.6 X 10" 3*- 15% 2 . . X 10" 2 ± 0% 2.9 X 10" 2 ±56% 1.4 X I Q ' ^ 3 6 % 4.4 ± 13%

18 0-1 7,3 X 10" 3 ± 5% 1.5 X 1 0 _ 1 ± 16% 3.5 ± 15%

5.0 ± 11%

0-20 2 . 8 X 1 0 " 3 ± 1 0 %

20-25 9 . 0 X I 0 ' 4 ± 1 5 % 5 . 1 X 1 0 " 2 ± 3 2 %

19 0-1 1 . 9 X 1 0 " 1 ± 1 4 % 8 . 4 X 1 0 " 2 ± 1 7 % 2 . 0 X 1 0 _ 1 ± 4 7 % 5.7 ± 11%

0-20 5.0 X 10" 3 ± 5% 8.8 X 10" 2 ± 25% 5.0 ± 13%

20 0-1 1.4 ±4% 1.1 X 10" 1 * 14% 2 . 0 X 1 0 _ 1 ± 4 4 % 4.0 ± 14%

0-20 3 . 8 X 1 0 " 3 ± 1 0 % 7 . I X 1 0 " 2 ± 5% I . O X 1 0 " 1 ± I 7 % 3.0 ± 15%

Table 5. (Continued) Sampling location toS? 2 3 B P u 2 3 9 P u B 0 S r 1 3 7 C s 9 5 Z r 144 Ce 4 0 K

21 0-1 5.1 X 10" 1 ± 6% 1.0 X 10" 1± 14% 3.0 X 10 _ 1 ± 2 6 % 4.1 ± 14%

0-20 2.8 X 10 " 3 ± 15% 5 . 2 X 1 0 " 2 ± 9% 6.0 X 10" 2±2G% 3.4 ± 14%

22 0-1 1.0 ± G% 1.3 X 1 0 _ 1 ± 18% 4.9 X 1 0 * ^ 2 5 % 3.3 ±23%

0-20 7.8 X 10* 3 ± 5% 1.9 X 10" 1 ± 14% 4.6 ± 14%

23 0-1 1.4 X 1 0 _ 1 ± 19% 2.1 X 1 0 _ 1 ± 3 7 % 4.0 ± 16%

0-20 3.0 X 10* 3 ± 15% 8 . 0 X 1 0 " 2 ± 9% 8 . 5 X 1 0 " Z ± 2 5 % 3.5 ± 16%

24 0-1

0-20 B . 7 X 1 0 " 3 ± 5%

5.0 X 10" 1 ± 7%

9.7 A ID" 2 ±20%

8.9 X 10" 2 ± 16% 2.9 X 10' 1 ± 30% 4.1 ± 15%

3.7 ±10%

25 0-1 2.2 X 1 0 _ 1 ± 1 1 % 7.6 X 1 0 " 2 ± 15% 2.0 X 10' 1 ± 38% 4.4 ± 12%

0-20 1.9 X 10" 3 ± 20% 7.P X 10" 2 ± 3% 4.9 X 10" 2 ±28% 3.2 ± 13%

36 0-1

0-20 4.4 X 10" 3 ± 10%

1.8 X 10" 1 ± 11%

1.5 X 1 0 _ 1 ± 15%

2.B X 1 0 * 2 ± 3 1 % 3.3 ± 13%

2.7 ± 18%

27 0-1 4.8 X 10" 1 ± 7% 4.3 X 10" 2 ±25% 5.7 ± 11%

0-20 3.4 X 10" 3 ± 10% 1.1 X 1 0 _ 1 ± 2 2 % 1.4 X 1 0 _ 1 ± 3 5 % 3.2 ± 18%

28 0-1

0-20 3.1 X 1 0 " 3 ± 10%

2.9 X 1 0 _ 1 ± 15%

7.0 X 10" 2 ±27%

9.9 X 10" 2 ±21% 7.7 ± 10%

3.5 ± 15%

29 0-1

0-20 1 . 2 X 1 0 * 2 ± 5%

4.2 X 1 0 _ 1 ± 12%

1.1 X 1 0 _ 1 ± 1 8 %

4.1 ±20%

3.9 ± 14%

30 0-1 7 . 3 X 1 0 _ 1 ± 6% 8.9 X 1 0 _ I ± 4 0 %

0-20 5.9 X 10" 3 ± 5% 7 . 5 X 1 0 " 2 ± 5% 9.4 X 10" 2 ±20% 9.2 X 1 0 _ 1 ± 4 0 %

31 0-1 2.1 X 1 0 _ 1 ± 1 1 % 3.5 ± 13%

0-20 3 . 4 X 1 0 " 3 ± 15% 3.7 X 10" 2 ± 10% 9.2 X 10" 2 ±16% 4.2 ± 10%

32 0-1 2.8 X 1 0 _ 1 ± 1 0 % 1.4 X 1 0 _ 1 ± 4 1 % 3.9 ± 14%

0-20 2 . 5 X 1 0 " 3 ± 1 5 % 3.8 X 1 0 " 2 ± 7% 4.6 X 10" 2 ±30% 4.7 ± 10%

Table 5. (Continued) Sampling location

Depth (cm) 2 3 8 P u 2 3 9 p u 9 0 S r 1 3 7 C s 9 5 Z r 144 Ce 4 0 K

33 0-1 4 . 1 X 1 0 _ 1 ± 7% 4.1 X 1 0 " 2 ± 2 5 % 2.0 X 10 _ 1 ± 3 7 % 2.6 ±15%

0-20 1.2 X 10" 3 ± 10% 6.6 X 1 0 " 2 ± 6% 9.0 X 1 0 _ 2 ± 18% 3.3 ± 13%

34 0-1 9.2 X 1 0 " 2 ± 2 1 % 3 . 5 X 1 0 " 2 ± 3 3 % 6.1 ± 10%

0-20 1.1 X 10 " 3 ± 10% 7.5 X 1 0 " 2 ± 3%, 1.0 X 10" 1 ±20% 4.2 ± 14%

35 0-1 4 . 2 X 1 0 _ 1 ± 7% 7.7 X 10" 2 ±17% 4.3 ±11%

0-20 6 . 5 X 1 0 " 3 ± 5% 4 . 5 X 1 0 ~ 2 ± 7% 1.6 X 1 0 ' 1 ± 15% 4.7 ± 13%

36 0-1 l . S X 1 0 " 1 ± 13% 4.2 X 10" 2 ±28% 5.6 :c 9%

0-20 3.4 X 10" 3 ± 5% 6.9 X 10" Z ± 6% 7.5 X 10" 2 ±26% 4.8 ± 13%

37 0-1 2.6 X 1 0 _ 1 ± 12% 3.5 X 10" 2 ±46% 2.2 X 10" - 1 ± 4 5 % 3.0 ± 17%

0-20 4 . 5 X 1 0 ~ 3 ± 5% 6.1 X 10" 2 ± 6% 9.5 X 10" 2 ± 19% 3.3 ± 14%

38 0-1

0-20 2.1 X 10" 3 ±10%

3.3 X 1 0 _ 1 ± 1 0 %

7.5 X 10" 2 ± 28%

8.7 X 10" 2 ±30% 6.0 ± 11%

5.6 ± 12%

39 0-5 1 . 2 X 1 0 " 2 ± 5% 1.1 X 1 0 - 1 ± 16% 2.0 X 1 0 _ 1 ± 13% 1.1 X 1 0 X ± 7%

5-10

10-15

7.3 X 1 0 " 3 ± 10%

5.5 X 10" 3 ±10%

8 . 2 X 1 0 " 2 ± 18%

6.4 X 10" 2 ± 18%

9 . 6 X 1 0 " 2 ± 2 1 %

9.4 X 10" 2 ±24%

1.3 X 1 0 1 ±

9.6 ±8%

6%

40 0-24 3 . 5 X 1 0 " 3 ± 5% 8.8 X 10" 2 ± 4%

41 u-1

0-24 2.0 X 10" 1 ± 5%

1 . 4 X 1 0 " 1 ± 14%

4.2 X 10~ 2 ±40%

6.6 X 10" 2 ±34%

42 0-1

0-24

4.3 X 10" 3 ± 10%

2.5 X 10 " 3 ± 10%

1.3 X 1 0 " l ± 14% 2.0 X 10" 2 ±45%

43 0-1

0-24 5 . 5 X 1 0 " 3 ± 5%

4 . 8 X 1 0 _ 1 ± 8% 2 . 9 X 1 0 " 1 ± 30%

44 0-1

0-24

3.0 X 10 " 3 ± 10%

3.2 X 10" 3 ± 3%

T a b l e 5. ( C o n t i n u e d )

B o n * g 2 3 8 P u 2 3 9 P o ~ 3 r 1 3 7 C 5

9 5 Z r » 4 C e

45 0-5 3.6 X10" 1 :!: 5%

5-10 1 . 2 X 1 0 " 2 ± 5%

10-15 9 . 0 X 1 0 " 3 * 5%

15-25 1.2 X 1 0 ' 3 ± 5%

46 0-25 2.6 X 10" 3 ± 5% 6.7 X 10" 2 ± 5%

47 0-25 1 . 8 X 1 0 " 3 ± 6% 6 . 1 X 1 0 " 2 ± 9%

48 0-25 2 . 2 X 1 0 " 3 ± 7% 6 . 2 X 1 0 " 2 ± 6%

49 0-25 2.5 X 10" 3 ± 5% 6.B X 10" 2 ± 5%

50 0-25 l.B X 10" 4 ± 14> 2.8 X 10" 3 ± 4% 9.2 X 10" 2 ± 4%

51 0-1 1 . 2 X 1 0 " 3 * 8% 3 . 0 X 1 0 " 2 * 4%

1-25 2 . 6 X 1 0 " 3 ± 7% 1.0 X 1 0 _ 1 ± 3%

52 0-1 7 . 2 X 1 0 " 4 ± &% 5 . 9 X 1 0 " 3 ± 8%

1-25 3 . 5 X 1 0 " 3 ± 9% 8 . 8 X 1 0 " 2 ± 5%

53 0-1 1 . 8 X 1 0 " 3 ± 8% 1 . 6 X 1 0 " 2 ± 4%

1-25 1.3XM>" 2 ± 4% 2 . 2 X I 0 " 1 * 3%

54 0-1 1 . 6 X 1 0 " 3 ± 7% 1 . 8 X 1 0 " 2 ± 4%

1-25 1 . 4 X 1 0 " 2 ± 5% 4.2 X 1 0 " 1 * 4%

55 0-30 1.4 X 10" 4 ± J.5% 3 . 5 X 1 0 " 3 ± 47.

56 0-25 5.B X 1 0 ' 4 ± 11% B.3 X ID" 3 ± 4%

57 0-25 1 . 4 X 1 0 " 4 ± 1 5 % 2 . 1 X 1 0 " 3 ± 4%

58 0-25 2 . 3 X 1 0 " 4 ± 1 2 % 7 . 6 X 1 0 " J ± 3%

59 0-25 1 . 4 X 1 0 " 4 t l 4 % 2 . G X 1 0 " 3 * 4% "Sample Locations 1 through 7 are located on-sito. All others are off-site.

Fig. 5. Livermore Valley soil sampling locations.

shown at on-site Locations 1 to 7 are due to their close proximity to the area being used for solar evaporation of low-level radioactive waste liquids. These levels are undoubtedly due to a number of low-level spills that occurred in this area several years ago in connection with the solar evaporation operation. This con­tamination, however, has not spread off-site as indicated by the plutonium levels observed at Locations 8, 9. and 11 which are situated immediately off-site from the contaminated area. In addition, the holding pond at the Livermore Sewage Treatment Plant, Locations 41, 45, 51 through 54 also indicate elevated 239

Pu activities. These values have resulted from routine and accidental releases of small amounts of piutonium over long time periods through the sani­tary sewer system which carries the Laboratory's biological and industrial effluents to the Livermore Sewage Treat­ment Plant.

In order to gain a better perspective of the contribution that the Laboratory operations have had on the environmental levels of plutonium within the Livermore

239 Valley, the Pu deposition values were plotted in Fig. 6. The data were found to fit two separate distributions. The upper distribution represents data obtained from the on-site locations in the vicinity of the solar evaporation area and from the hold­ing pond at the Livermore Sewage Treat­ment Plant. The low&r distribution, on the other hand, represents the remainder of the data obtained from areas where the Laboratory'? contribution has been mini­mal, if any, and therefore represents predominantly the contribution due to global fallout from atmospheric weapons tests . This distribution exhibits a mean

o value of 1 mCi/km , which is almost a factor of 2 less than the mean value ob-

4 tained from the data of Hardy and Krey. Their measurements of global fallout pro-

239 duced Pu deposition levels at tnirteen

- 1 6 -

Table 6 Deposition levels of various -adionuolides in soil (activities in raCi/km ).

Sampling location 238_ Pu 2 3 9 p u 9 0 S r 1 3 7 C s 9 5 Z r 144 C ,

l a 1.7 17 36

2 a 4.8 7.5 33 64 3 a 3.4 22 31 49

4 a 18 63 21 34 5 a 56 180 23 39 6 a 0.65 2.6 38 44 7 a 1.2 3.7 29 33 8 0.29 1.9 18 36 9 1.1 17 15 0.71 1.9

10 0.76 20 36 0.84 1.9 11 0.16 2.6 19 30 0.63 0.27 12 0.028 0.65 ie 15 0.70 4.4 13 0.024 0.57 17 20 1.5 1.9 14 0.018 0.65 17 14 1.4 6.3 15 0.55 11 20 1.5 5.0

16 0.49 18 12 1.9 4.3 17 1.25 26 28

18 0.90 19 1.4 25 1.1 2.6

20 0.93 18 25 1.1 2.0

21 0.73 13 15 1.2 3.6

22 1.7 40 1.0 3.9

23 0.76 20 21 1.5 2.2

24 2.1 23 0.98 3.3

25 0.48 18 13 0.91 2.3

26 1.14 40 0.36 27 0.82 28 0.53 28 0.80 19 1.3 29 3.0 28 30 1.151 21 26 31 0.97 11 27 32 0.71 11 13 33 0.32 18 23 0.51 2.5

34 0.26 18 24 0.42 35 1.7 12 42 0.97 36 0.89 18 20 0.57 37 1.3 17 27 0.42 2.7

38 0.57 20 1.1

-17

T a b l e 6. (Continued)

Sampl ing loca t ion

39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59

238 Pu

0.88 1.2 4.6 5.4 0.057 0.19 0.044 0.079 0.047

2 3 9 „ Pu

1.8 1.1

60 0 .81 1.9 1.2

27 0 .91 0 .65 0.76 0.87 0.98

34 33 78

162 1.5 3.0 0 .68 2.7 0.9

90 Sr 137 Cs

18 27

23 22 22 24 33

27

12

Z r

0.83

144 Ce

Sample L o c a t i o n s 1 th rough 7 a r e o n - s i t e . All o t h e r s a r e o f f - s i t e .

s i t e s t h roughou t t h e United S ta te s r a n g e d o

f rom 0 . 7 - 2 . 4 m C i / k m . Since m o s t of t he global fallout con t r ibu t ion h a s b e e n by wet depos i t ion , t h i s f ac to r of 2 d i f f e r ence i s quite r e a s o n a b l e in view of t h e L i v e r m o r e Va l l ey ' s low annua l ra in fa l l of abou t

137 14 i n c h e s . L ikewi se , t he m e d i a n Cs depos i t ion l e v e l of 26 m C i / k m i s abou t a f ac to r of 3 be low the m e d i a n d e p o s i t i o n

137 l e v e l t h a t one m a y d e r i v e f r o m t h e C s e x p o s u r e r a t e s in a i r m e a s u r e d b y L o w d e r and McLaughl in a t many l o c a t i o n s throughout the United S ta t e s . The a c t i v i ­t i e s of Z r and Ce a r e a p p r e c i a b l y lower than tha t of 1 3 7 C s and 9 0 S r p r i ­

m a r i l y due t o t h e i r r e l a t i v e l y s h o r t half-l i v e s . One would expect t h e i r a c t i v i t i e s to be m a i n l y due t o the r e c e n t F r e n c h and Ch inese a t m o s p h e r i c n u c l e a r w e a p o n s t e s t s . T h u s , t h e L a b o r a t o r y ' s c o n t r i b u ­t ion t o t h e s e f i s s ion p roduc t a c t i v i t i e s is neg l ig ib l e .

The s a m p l e s co l lec ted o n - s i t e in the v ic in i ty of t h e a r e a being u s e d fo r s o l a r e v a p o r a t i o n of low l eve l r a d i o a c t i v e l iqu ids w e r e in add i t i on subjected to i s o t o p i c u r a n i u m a n a l y s e s by m a s s s p e c t r o g r a p h ^ m e t h o d s . T h e r e s u l t s a r e shown in Tab le 7. T h e t o t a l u r a n i u m c o n c e n t r a t i o n s a r e l e s s

3 t h a n t h e g loba l a v e r a g e of about 4 X 10 ng/g

- 1 8 -

1000

E

8. m Q

1.0 30 50 70 90 Cumululative percent of samples

98 99.5 99.9 99.99

Fig. 6. 239 T Distribution of * u Pu deposition values in Livermore Valley so i l s . The upper distribution represen ts data obtained from on-si te locations and from one of the holding ponds at the Livermore sewage treatment plant. The lower diirtri-bution represents data obtained from a r ea s where the Laboratory's contribution has been minimal.

• 1 9 -

Table 7. Concentrations of uranium in soils (ng/g).

Sampl ing l o c a t i o n

Depth (cm) 2 3 4 u 2 3 5 U 2 3 8 U

Tota l u r a n i u m 2 3 5 u / 2 3 8 u a

2 0-15 1.14 X 1 0 - 1 ± 4% 1.34 X 10 ± 1% 1.86 X 1 0 3 ± 2% 1.87 X 1 0 3 ± 2% 7.2 X 1 0 " 3

3 0-15 1.15 X 1 0 _ 1 ± 5% 1.35 X 10 ± 1 % 1.88 X 1 0 3 ± 2 % 1.90 X 1 0 3 ± 2 % 7.2 X 1 0 " 3

4 0-15 1.10 X 1 0 _ 1 ± 3% 1.36 X 10 ± 1% 1.88 X 1 0 3 ± 2 % 1.93 X 1 0 3 ± 2 % 7.2 X 1 0 " 3

5 0-15 1.50 X 10 ± 1% 1.48 X 10 ± 1% 2.05 X 1 0 3 ± 2% 2.07 X 1 0 3 ± 2% 7.2 X 1 0 " 3

6 0-15 1.14 X 1 0 _ 1 ± 9% 1.20 X 10 ± 2 % 1.69 X 1 0 3 ± 2% 1.70 X 1 0 3 ± 2% 7.1 X 1 0 " 3

7 0-15 1.00 X 1 0 " X ± 2% 1.25 X 10 ± 2 % 1.75 X 1 0 3 ± 2 % 1.76 X 1 0 3 ± 2 % 7.1 X 1 0 " 3

8 0-15 1.03 X 1 0 _ 1 ± 2% 1.21 X 10 ± 1% 1.69 X 1 0 3 ± 2 % 1.71 X 1 0 3 ± 2 % 7.2 X 1 0 " 3

11 0 -1 7.25 X 1 0 " 2 ± 1% 9.70 ± 1% 1.36 X 1 0 3 ± 2% 1.37 X 1 0 3 ± 2% 7.1 X 1 0 " 3

1-5 8.50 X 1 0 " 2 ± 1% 1.12 X 10 ± 1% 1.55 X 1 0 3 ± 2 % 1.56 X 1 0 3 ± 2 % 7.2 X 1 0 " 3

5-10 7.00 X 1 0 " 2 ± 14% 8.80 ± 1% 1.22 X 1 0 3 ± 2 % 1.23 X 1 0 3 ± 2% 7.2 X 1 0 " 3

10-15 8.00 X 1 0 " 2 ± 3% 1.06 X 10 ± 1% 1.48 X 1 0 3 ± 1% 1.49 X 1 0 3 ± 2% 7.2 X 1 0 " 3

15-20 8.10 X 1 0 " 2 ± 4% 1.10 X 10 ± 4 % 1.53 X 1 0 3 ± 2 % 1.54 X 1 0 3 ± 2% 7.2 X I D " 3

aThe 235u/238u ratio in natural uranium is 7.2 X 10" 3

235 238 and the U/ U ratio approximates that in natural uranium, indicating that the solar evaporation operation has not contributed any measurable uranium activ­ity to the environment in this part icular a rea .

Environmental radiation levels due to the gamma-emitting radionuclides dis­tributed in the soil may be inferred from these measurements by using the data of Beck and de Flanque. Detailed calculations have not been completed a t th is t ime, but preliminary results indicate that the mean

137 exposure rate in a i r due to the Cs activity in the soil at a height of 1 meter above the ground within the Livermore Valley is approximately 0.1 juR/hr (0.88 mR/yr ) . The exposure r a t e s due to

95 144 the Z r and Ce activities in the soil 137 a re insignificant relative to that of By using the data of Wollenberg, et al„ and the data in Tables 5 and 7, one may

Cs. 7

determine the mean natural background exposure rates due to the activities of

K and U ser ies in the soil to be 0.7 /uR/hr (6.2 mR/yr) and 1.4 fiR/hr (12.3 mR/yr) , respectively, at a hsight of 1 m e t e r above the ground. Thus, the natural contribution to the exposure rate due to gamma emitters in the soil is far g rea te r than that due to the artificially produced radionuclides. To determine the environmental impact due to the elevated plutonium deposition levels is very diffi­cult. Fo r these particular si tes the p r i ­m a r y concern to man is that due to r e -suspension of the plutonium and subsequent inhalation. Since resuspension factors vary over many orders of magnitude, it is difficult to calculate a meaningful expected airborne concentration. However, we anticipate that these airborne concentra­tions will not be significantly above back­ground levels.

20-

LABORATORY SEWER EFFLUENT

The low level radioactive wastes from the Laboratory are discharged into the City of Livermore sanitary sewer system. This effluent is processed at the Livermore Sewage Treatment Plant where the liquid and sludge a re separated on entering the plant. The sludge passes into one of two digesters where it is broken down by bacterial action. Methane gas is evolved and burned, and the remaining sludge is released to large sludge ponds and r e ­tained for subsequent use as a soil con­ditioner. The purified water is used for irrigating the Livermore Golf Course and nearby agricultural land; the excess is discharged into the Los Positas Arroyo.

Weekly samples were collected from each digester, the aeration tank and the liquid effluent discharged from the plant in order to determine if any significant build-up of radioactivity occurred within the plant. These samples were subjected to gross alpha and beta analyses by com­plete dissolution, electrolytic deposition and direct proportional counting. The tritium analyses were performed by sub­jecting 1 ml of each sample to direct liqaid scintillation counting. In addition, a monthly composite sample of the effluent

90 was analyzed for Sr by radiochemical separation and beta counting. The con­centrations observed during 1971 averaged over 1 month periods are given in Table 8. Most of the gross alpha and gross beta activities are associated with the sludge present in the effluent. Thus, samples obtained from the digesters show the highest activities with the expected attendant decrease in activity as the relatively purified liquid passes through

the aeration tank and is finally r e ­leased from the plant.

WATER

Monthly samples were collected from various water sources in the Livermore Valley. These samples were analyzed for gross alpha and gross beta activities by techniques similar to those used for sewage effluent samples. No sample showed an alpha activity above the limit of detection of 1.2 pCi/ l i ter . Quarterly averages for beta activities are given in Table 9. Loca­tions 7, 14 through 18 and 21 through 24 represent surface sources such as ponds, creeks, reservoirs, and aqueducts. Livermore rainfall is sampled at Loca­tion 20. The remainder of the locations are domestic water sources. The activi­ties are reasonably homogeneous with the highest value occurring in the rainfall sample collected over a 3-month period. This is most likely due to its exposure to the relatively higher concentrations of the various natural and artificially produced radionuclides present in the atmosphere.

The samples collected during the first 6 months of 1971 were analyzed for tritium activity by direct scintillation counting.

4 The maximum activity was 1.1 X 10 ± 8% pCi/1 with an average value of 4.0 X 10 3 pCi/1 (the limit of detection) which is 0.1% of the off-site RCG of 3 X 10 pCi/1. Because of these low activ­ities, the samples collected during the last 6 months were vacuum distilled and elec-trolytically enriched before scintillation counting. The results of these analyses are shown in Table 10. Inspection of the data indicates that the samples also ex­hibit rather uniform tritium concentrations

Table 8. Livermore sewage treatment plant sampling results during 1971. Gross alpha act iv i ty (pCi/1)

Digesters Aeration tank Effluent Month High Average High Average High Average Percent R C G a

January 380 ±20% 250 57 ± 19% 43 22 ±50% 13 13 February 230 ± 24% 160 29 ± 26% 27 80 ±50% 26 26 March 180 ±42% 150 49 ± 41% 39 32 ±50% 14 14 April 190 ± 23% 190 31 ±27% 29 11 ±50% 54 54 May 350 ± 20% 210 74 ± 22% 49 27 ± 50% 11 11 June 510 ± 13% 280 52 i 21% 48 5.6 ± 50% 2.7 2.7

July 300 ± 16% 220 320 ± 13% 140 7.4 ± 50% 3.3 3.3 August 440 ±19% 260 73 ± 19% 45 13 ±50% 5.9 5.9 September 530 ± 24% 280 99 ± 15% 61 13 ±50% 5.3 5.3 October 220 ± 21% 110 66 ± 17% 50 11 ±50% 5.9 5.9 November 440 ± 21% 220 42 ± 26% 30 14 ±50% 8.2 8.2 December 260 ± 22% 180 80 ± 18% 47 11 ± 50% 6.5 6.5

Average

Gross beta activity (pCi/1) Diges ters Aeration tank Effluent

Month High Average High Average High Average P e r c e n t RCG b

January 1.4 X 1 0 3 ± 5% 5.3 X 1 0 2 60 ± 4% 49 48 ± 15% 17 17 February 9.7 X 1 0 2 ± 4% 3.6 X 1 0 2 45 ± 5% 27 37 ± 80% 19 19 March 1.1 X 1 0 3 ± 6 % 5.8 X 1 0 2 120 ± 5% 71 88 ± 14% 35 35 April 1.0 X 1 0 3 ± 4% 5.3 X 1 0 2 84 ± 5% 48 40 ± 9% 17 17

May 3.4 X 1 0 2 ± B% 2.8 X 1 0 2 5Z ± 5% 37 31 ± 17% 17 17 June 1.1 X 1 0 3 ± 4 % 3,9 X 1 0 2 41 ± 5% 36 17 ± 24% 15 15

July 4.0 X 1 0 2 ± 7% 2.9 X 1 0 2 55 ± 4% 36 19 ± 22% 14 14 August 6.0 X ID 2 ±7% 3.8 X 1 0 2 76 ± 4% 52 19 ± 22% 14 14 September 4.3 X 1 0 3 ± 2% 1.0 X 1 0 3 55 ± 4% 47 20 ± 20% 15 15

October 4.2 X 1 0 2 ± 8% 2.5 X 1 0 2 48 ± 5% 43 44 ± 13% 19 IB

November 4.0 X 1 0 2 ± 8% 2.8 X 1 0 2 38 ± 6% 35 24 ± 19% 17 17

D e c e m b e r 1.0 X 1 0 3 ± 4% 3.8 X 1 0 2 58 ± 4% 48 43 ± 13% 22 22 Annual

average 4 .4 X 1 0 2 44 18 18

Tritium activity (pCi/1)

Effluent

Sr activity (pCi/1) Effluent

Month High Average Percent RCG C Average Percent RCG

January 1.4 X 10* ± 5% 1.1 X 10* 0.37 0.5 ± 50% 0.17

February 4.1 X 1 0 3 ± 5 0 % 3.6 X 1 0 3 0.12 1.5 ± 20% 0.50

March 2 . 4 X 1 0 8 ± 3% 4.3 X 1 0 4 1.43 0.6 ±21% 0.20

April a.o x io 3 ± 14% 4.2 X 1 0 3 0.14 1.6 ± 18% 0.20

May 3.4 X 1 0 8 ± 2% 5.6 X 1 0 4 1.87 0.4 ± 50% 0.13 June 1.8 X 1 0 3 ± 50% 1.7 X 1 0 3 0.06 0.6 ± 50% 0.20

July 1.5 X 1 0 4 ± 5% 6.3 X 1 0 3 0.21 0.5 ± 50% 0.17 August 3.9 X 1 0 3 ± 16% 2.2 X 1 0 3 0.07 2.3 ± 50% 0.77

September 1 . 1 X 1 0 5 ± 1% 1.5 X 1 0 4 0.50 1.3 ± 25% 0.43 October 2.0 X 1 0 4 ± 4% 5.8 X 1 0 3 0.19 1.1 ±38% 0.37

November 1.2 X 1 0 4 ± 6% 3.5 X 1 0 3 0.12 3.3 ± 30% 1.10

December 1.2 X 1 0 4 ± 6% 3.9 X 1 0 3 0.13 0.8 ±21% 0.30

Annual average 1.3 X 1 0 4 0.43 1.2 ± 42%

a R C G (alpha activity) = 100 pCi /1 . b R C G (beta activity) = 100 pCi/1 . CRCG (HTO) = 3 X 10 e pCi/1. dRCG ( G 0 Sr) = 3 X 10 2 pCi/1.

-22-

Table 9. Gross beta activities in Livermore water samples.

January- March April-June Activity Activity

Location (pCi/1) Location (pCi/1)

1 — 11 7.4 2 — 12 3.9 3 2.9 13 3.2 4 2,2 14 7.0 5 2.7 15 4.9 6 2.0 16 12.3 f 3.1 17 4.9 8 2.4 18 9.2 9 2.6 19 3.4 10 — 20 23.7 11 — 21 4.7 12 4.3 22 9.1 13 3.6

Average 2.9 7.8 Percent

RCGa 10 2f aRCG (beta activity) = 30 pCi/1.

that are well below the recommended con­centration guide value. The table also includes an estimate of the dose that may be delivered to an adult consuming water containing the listed tritium concentrations. The doses, which are typically l e s s than 0.1 mrern, are based upon a daily water

q consumption of 1 liter per day and the

g model of Anspaugh, et al.

VEGETATION

Vegetation samples (usually native grasses) were collected from nine loca­tions in the Livermore Valley during January, April, and May. The samples were dried in ambient ail for about a week and then pressed into 5-inch diameter and

July-September October-December Activity Activity

Location (pCi/1) Location (pCi/1)

11 3.7 11 3.0 12 3.3 12 2.0 13 3.4 13 2.0 14 — 14 — 15 2.3 15 2.9 16 7.1 16 5.9 17 6.0 17 5.2 18 3.7 18 3.1 19 2.1 19 2.9 20 — 20 — 21 2.0 21 3.0 22 8.2 22 7.6 23 2.2 23 2.4 24 4.8 24 6.1

4.0 3.8

13 13

1-inch thick pellets weighing approximately 200 grams. The pellets were analyzed for various gamma-emitting radionuclides by placing them between two 8 X 4 inch Nal(Tl) crystals. A portion of each sample was also freeze dried and the collected water was analyzed for tritium activity by direct scintillation counting. These techniques were changed in the middle of the year after the development of improved ana­lytical facilities. During the months of August, October and November samples were collected from 13 locations in the Livermore Valley. The samples collected during a particular month were dried and composited. A 100-gram portion of the composite sample was counted on the Ge(Li) detector used for analyzing the

-23-

Table 10. Tritium activities in Livermore water samples collected during July-December, 1971 (activities in pCi/1).

Sampling location Maximum Average Percent RCG

Calculated annual adult whole body radiation dose

(mrem)

11 3.2 X 10 2 ± 6% 2.6 X 10 2 8.6 X 10" 3 1.0 X 10" 2

15 3 . 2 X 1 0 2 ± 7 f l 2.8 X 10 2 9.3 X 10" 3 1.1 X 10'2

16 1 .1X10 3 ±4% 8.7 X 10 2 2.9 X 10" 2 3.5 X 1 0 * 2

17 2,1 X 10 Z ± 8% 2.0 X 10 2 6.7 X 10" 3 8.0 X 10" 3

18 — 2 a

2.7 X 10* 9.0 X 10" 3 1.1 X 10" 2

19 I . 7 X 1 0 2 ± 8 % 1.6 X 10 2 5.3 X 10" 3 6 . 5 X 1 0 " 3

20 _, 2 a

8.1 X HT 2.7 X 10" 2 3.2 X 10" 2

21 — 2 a

2.7 X 10* 9.0 X 10" 3 1.1 X 10" 2

22 4 .1X10 2 ±67o 4.0 X 10 2 1.3 X 10" 2 1.6 X 10" 2

23 7 . 2 X 1 0 2 ± 5 % 3.7 X 1 0 2 1.2 X 10 " 2 1.5 X 10* 2

24 1.2 X 10 3 ± 4ft 6.0 X 10 2 2.0 X 10" 2 2.4 X 10" 2

Average 4.1 X 10 2 1.4 X 10" 2 1.6 X 1 0 " 2

aSingle sample collect at these locations. bRCG (HTO) = 3 X 10 6 pCi/1.

airborne particulate samples. 'The tritium concentrations in the water, obtained by freeze drying these samples, were deter­mined by electrolytic enrichment and subsequent scintillation counting.

The results of the gamma spectral analyses are shown in Table 11. These activities exhibit their highest values during the spring months; this is un­doubtedly due to the higher ambient at­mospheric concentrations during this time of year. Using these data one may calcu­late the annual radiation dose received by man from direct ingestion of these radio­nuclides assuming the observed activities are typical of those in edible vegetation. The calculated adult whole body or critical organ doses due to the gamma emitters

shown in Table 11, are based upon an adult consumption of 400 grams per day of

o

vegetation with a moisture content of 80% and the data of Ng, et al., regarding the dose received per unit of radioactivity consumed under equilibrium conditions. With the exception of global fallout-produced 1 4 4 C e and natural 4 K activities, these radionuclides deliver appreciably less than 1 mrem/yr to the whole body or critical organ as a result of direct inges -

144 tion of edible vegetation. The *"Ce and 4 0 K activities, on the other hand, may easily deliver up to 10 mrem/yr to the lower large intestine and whole body respectively.

The results of the tritium analyses are shown in Tables 11 and 12. The data of -24-

Table 11. Average radionuclide activities in Livermore vegetation samples collected during 1971.

Average activity (pCi/ R )

Calculated annual dose via direct ingestion

(mrem) Critical organ

Samples collected during Jan.,

Apr. and May: 1 3 7 C s 1.8 X 1 0 " 1 3.2 X 10" 1 Whole body 1 4 4 C e 1.4 11.0 Lower large intestine 9 5 Z r / 9 5 N b 6.3 X 10" 1 — — 7 B e 1.8 9.C X 10~ 2 Lower large intestine 3 H 2.5 X 10 4 pCi/1 4.0 X 10" 1 Whole body

Samples collected during Aug.,

Oct. and Nov.: 137

103 Cs

Ru 144 Ce 95 Zr 7 B e 4 0 K

8.0 X 10

1.3 X 10"

5.9 X 10

5.3 X 10"

2.1

3.0

- 2

-1

1.4 X 10

1.4 X 10

4.6

1.3 X 10"

1.0 X 10"

4.2

-1 Whole body

Lower large intestine

Lower large intestine

Lower large intestine

Lower large intestine

Whole body

Table 12 show significant variation from one location to another which may be caused by Laboratory operations. From Fig. 2 one may expect the effect of the Laboratory's operation on the environment to be minimal at Locations 4, 7, 13, 17, 18 and 19 because the prevailing wind is from the southwest. Samples collected at these locations exhibit tritium values ranging from 1.6 X 10 2 to 4.5 X 1 0 2 pCl/1, which may be considered environmental background levels. However, Locations 10 and 11 are on-site and Locations 5, 15, 16 and 20, which show elevated levels, are situated in a generally downwind direction from the Laboratory, thus exposing the

vegetation in these areas to the low level gaseous effluent released routinely from the Gaseous Chemistry Building. The samples collected at Location 12 represent grass that has been watered by the liquid effluent from the Livermore Sewage Treat­ment Plant. The resulting whole body doses to an adult, shown in the tables, were derived from the model of Anspaugh,

Q

et al. These are also based upon the direct daily consumption of 400 grams of vegetation. This mass of vegetation, however, is assumed to be equivalent to the same mass of water containing the tritium concentrations shown in the tables under equilibrium conditions. One may

25-

Table 12. Tritium activities in Livermore vegetation samples collected during August, October and November, 1971.

S a m p l e l o c a t i o n 3

T r i t i u m ac t iv i t i e s (pCi/1) C a l c u l a t e d annual whole body dope

( m r e m ) S a m p l e l o c a t i o n 3 M a x i m u m A v e r a g e

C a l c u l a t e d annual whole body dope

( m r e m )

4 4.6 X 1 0 2 ± 51% 3.3 X 1 0 2 5 X 1 0 " 3

5 9.8 X 1 0 3 ± 3% 4.7 X 1 0 3 8 X 1 0 " 2

7 6.1 X 1 0 2 ± 31% 4 . 5 X 1 0 2 7 X 1 0 " 3

10 2.8 X 1 0 4 ± 2% 1.1 X 1 0 4 2 X 1 0 " 1

11 1.2 X 1 0 5 i 1% 3.9 X 1 0 4 6 X 1 0 " 1

12 3.3 X 1 0 3 ± 7% 1.8 X 1 0 3 3 X 1 0 " 2

13 4.4 X 1 0 2 ± 44% 3.0 X 1 0 2 5 X 10~ 3

15 1.7 X 1 0 3 ± 12% 1.4 X 1 0 3 2 X 1 0 " 2

16 9.0 X 1 0 3 ± 4% 3.5 X 1 0 3 6 X 1 0 " 2

17 1.7 X 1 0 2 ± 103% 1.6 X 1 0 2 3 X 1 0 " 3

18 2.8 X 1 0 2 ± 65% 2.8 X 1 0 2 5 X 1 0 " 3

19 2.6 X 1 0 2 ± 68% 2.2 X 1 0 2 3 X 1 0 " 3

20 6.8 X 1 0 3 ± 4% 6.4 X 1 0 3 1 X 1 C - 1

A v e r a g e 5.3 X 1 0 3 8 X 1 0 " 2

The sample locations a r e shown in Fig. 1.

readily observe that, in spite of the slightly elevated levels, the calculated annual whole body doses a re st i l l very smal l .

MILK

During the first 8 months of 1971, m a k samples were collected each month from two dai r ies , one located ir. the Livermore Valley about 6 miles west of the Laboratory and the other in the San Joaquin Valley about 6 miles southwest of Tracy. In August, 1971, the Livermore Valley dairy ceased operations. Since no other dairy was available, milk sampling was restricted

to the San Joaquin Valley dairy during the r e s t of the year. Before analysis, the samples were concentrated by means of a vacuum operated, foam entrainment evap­orator so that about 9 l i te rs of whole milk were condensed to 2 l i t e r s . The resulting samples were subjected to gamma spectral analyses by inserting them between two 8 X 4-inchNaI (Tl) crysta ls . In addition, each sample was analyzed for tri t ium activity by counting 1 mil l i l i ter of the distillate directly in a standard liquid scintillation detector. The activities of 1 3 7 C s , 1 4 4 C e , 3 H and 4 0 K a r e shown in Table 13. Also shown a re the calculated annual adult whole body or cr i t ical organ

-26-

Table 13. Radionuclide activity observed in milk samples collected during 1971.

Maximum (pCi/1)

Average (pCi/1)

Calculated annual adult

radiat ion dose (mrem) Cri t ica l organ

L i v e r m o r e Val ley Dairy Jan. -Aug. :

1 3 7 C s 9.1 4.5 2.6 X 1 0 " 2 Whole body 1 4 4 C e 19 11 2.8 X 1 0 " 1 Lower l a r g e intestine

3 H 1.0 X 1 0 5 1.7 X 1 0 4 5.4 X 1 0 " 2 Whole body

San Joaquin Val ley Dairy Jan. -Aug. :

1 3 7 C s 5.6 3.8 2.2 X 1 0 ~ 2 Whole body 1 4 4 C e 56 13 1.4 X 1 0 " 1 Lower l a r g e intest ine

3 H 6.7 X 1 0 3 4.3 X 1 0 2 1.3 X 1 0 " 3 Whole body

S e p t . - D e c :

1 3 7 C s 2.9 2.7 1.6 X 1 0 " 2 Whole body

1 4 4 C e 26 18 4 .6 X 1 0 " 1 Lower l a r g e intest ine

3 H 1.3 X 1 0 3 6.2 X 1 0 2 1.9 X 1 0 " 3 Whole body 4 0 R 1.3 X 1 0 3 1.2 X 1 0 3 5.4 Whole body

doses delivered to man via the milk path­way. These calculations a r e based upon

D

a daily intake of 260 grams/day and the models previously referenced. As ex­pected, the only significant dose to an

40 individual is that from K.

ACCIDENTAL RELEASE OF TRITIUM GAS

Continuous air sampling is maintained on the stack effluent from the Gaseous Chemistry Building. On April 12, 1971, an accidental release of 240 Ci of t r i t ium occurred. Because the tr i t ium was ex­pected to be in the vapor form, an exten­sive sampling program was conducted to

evaluate the impact of the r e l ea se on the environment. Vegetation, atmospheric water vapor and water samples were col­lected and analyzed for t r i t ium activity. The vegetation samples were freeze-dried and the collected water was subjected to scintillation counting. Other samples were counted directly in the same manner. Detectable activities were observed in some off-site vegetation and water vapor samples . The maximum activity in

5 vegetation samples was 1.6 X 10 pCi/ l i ter with the average activity of

4 all the samples being «2.5 X 10 pCi / l i te r . The atmospheric watervapor samples indicated a maximum activity

-27-

=^tJ^_^._ .. _.U.„_. ___ ___.

1 mile

— • — " — Perimeter of LLL

O Locations of TLD" s

Fig. 7. Locations of thermoluminescent dosimeter locations m the vicinity of ttte Lawrence Livermore Laboratory.

' 3 of 5.9 X 10" pCi/m and an average value of 2 X 10 3 pCi/m 3 .

A hazards analysis was performed in order to determine the potential exposure to a hypothetical individual standing down­wind at the point of maximum surface air concentration during cloud passage. Using standard atmospheric diffusion calcula­tions and tritium uptake estimates, one may calculate that it would have been pos­sible for this individual to have received a maximum of 1.5 mrem during cloud passage. An estimate was also made of the maximum potential doses that a child could have received from drinking milk produced by cows grazing on vegetation contaminated with tritium at the maximum observed concentration. Using the model of Anspaugh, et al„ the maximum poten­tial dose via this pathway to an infant would have been 0.18 mrem and that to an adult 0.03 mrem.

ENVIRONMENTAL RADIATION. MEASUREMENTS

Environmental radiation background measurements were made at 12 Laboratory perimeter locations shown In Fig. 2, and at 40 off-site locations in the immediate vicinity of the Laboratory shown in Fig, 7. These measurements were made with CaF^rDy (TLD-200) thermolamicescent dosimeters placed at a height of 1 meter above the ground. Exposure periods were usually 3 months. The resulting exposure rates reflect the sum of terrestrial and cosmic radiation sources. Based on past experience, the exposure rates in the Lxvenaore Valley due to terrestrial sources -rary between 4 and 7 fiR/hr de­pending upon the location, while that due to cosmic radiation, according to the data

of Lowder and Beck, is approximately 4 /xR/hr. Table 14 shows the exposure rates obtained at the perimeter locations during three periods in 1971. This data is also expressed as projected annual millirem dose rates (1 fiR/hr = 7.612 mrem per year). Inspection of the data reveals

<P

• 1 0 -

Dose rate interval, April-ifcme, 1971 — mrem/yr

#

30

20

10

' I ' I ' I ' I • I Median. =

_ 71 nrem/yr I

s l _ j L • I . ' I I 45 55 65 75 85 95

Dose rate interval, August-November, 1971 — mrem/yr

30

^ 20

r—j—T—p-Median =

_ 75 mrem/yr

I 10 nJ J_ X a _L

45 55 65 75 85 95 Dose rate interval,

November-December, 1971 — mrem/yr

Fig. 8. Seasonal frequency distribution of environmental radiation back­ground dose rates from the measurements at the locations shown in Fig. 7.

-29-

Table 14. Environmental radiation background measurements at the Livermore Laboratory perimeter during 1971.

April -June August--November November MR/lu­

-December Location *<R/hr mr em/year n R / h r mrem/yea r

November MR/lu­ m r e m / y e a r

1 10.3 78 9.1 69 l l . 1 85 2 9.6 73 P.4 72 11.9 91 3 11.1 85 10.4 79 11.7 88 4 9.S 73 95 72 11.1 85 5 14.4 110 10.4 79 8.9 68 6 9.6 73 — — 9.3 71 n I 7.9 60 8.7 66 — — 8 8.8 67 8.0 SI 9.5 72 9 7.9 60 8.1 62 9.5 72

13 — — 10.5 80 12.1 92

14 — — 9.1 69 12.3 94 15 — — 11.3 86 13.2 100

Average 9.9 75 9.5 72 11.0 84

that Location 5 during the April-June period and Locations 13, 14, and 15 during the November-December period show above-average exposure rates. Location 5 is adjacent to a cyclotron building and Locations 13, 14, and 15 are near a linear accelerator facility.

Figure 8 consists of a series of histo­grams showing projected annual dose rates observed at the 40 off-site monitoring locations during the three measurement periods. The median dose rates are com­parable with the average dose rates shown in Table 14.

Environmental Levels of Radioactivity — Site 300

ATMOSFHERIC RADIOACTIVITY

The concentrations of various particu­late airborne radioactive substances were measured continuously at 11 air sampling locations as shown in Fig. 9. Ten of the samplers are located within the boundaries of Site 300, and the eleventh is located in Tracy, the primary population center of concern. The on-site samples are col­lected on 8 X 10-inch Whaiman-41 filters at a flow rate of about 25 cfm. Samples

in Tracy are collected on 4 X 9-inch HV-70 (cellulose-asbestos) filters at a flow rate of about 4 cfm. Filters are changed weekly during the winter months and twice weekly during the summer to avoid exces­sive mass loading. The filters are ana­lyzed by the method previously described for filters used in the Livermore Valley.

No gross alpha activity above the 3

0.001 pCi/m detection limit was observed on these filters. The gross beta activities, averaged over 3-month periods, are listed

- 3 0 -

HutSprinicx^ I ON v . ~: A N D

o Air samoling stations

I I Water sampling points

\ J Vegetation sampling i

Tracy

SHAIWt. ! * « • » DCPOT i

.|,v K;IT°2 ^„„_(!

J.*.

! Site 300 ~*{1

..' - .!• — J

i. *.

0

Fig. 9a. Air, water, and vegetation sampling locations in the Site 300 area. See Fig. 9b for sampling locations inside Site 300 boundry.

-31-

^ J Air sampling stations f l Wafer sampling points (_) Vegetation sampling areas

a c ; o c = r

Fig. 9b. Air, water, and vegetation sampling locations inside Site 300 boundrj.

Table 15. Airborne particulate activity at Site 300 during 1971. Cras« beta aeilvliy (pCI, mJ>

Sampling locat ion 3

January-Maximum

March • \ v e n e e

•>pril-Jutie July-Scnteir.ber Miximum V.-eraae

October-OcceraUer Maximum -Iverafifc

Annual sverafie

t'ereem l(CG b

Sampling locat ion 3

January-Maximum

March • \ v e n e e Maximum Average

July-Scnteir.ber Miximum V.-eraae

October-OcceraUer Maximum -Iverafifc

Annual sverafie

t'ereem l(CG b

1 0.42 ± I S 0.090 0.33 ± I S 0.26 0.34 = I S 0.20 0.13 i 6S 0.057 0 .15 15 2 0.40 z 17. 0.005 0.34 s I S 0.22 0.43 i IS 0.21 0.12 s S S 0.054 0.14 14 3 0.33 i I S 0.086 0.29 ± I S 0.30 0.40 t I S o.ia 0.11 = 6 S O.OSl O.U 13 4 0.18 ± 2S 0.065 0.30 i I S 0.23 0.42 i IS 0.2! 0.30 : OS 0.076 0.15 IS 5 0.43 ± 1% 0.090 0.27 t I S 0.20 0.60 : 2S o.ia 0.076 t 7 S 0.041 0.13 13 6 0.43 ± 2 S 0.13 0.31 : 3 S 0.23 0.40 i 2S O.IC S.I2 : ? ? . 0.065 O.U 14 7 0.38 i I S 0.089 0.32 i I S 0.21 0.41 : I S 0 .19 0.082 t OS 0.04G 0.13 13 8 0 .27 ± I S 0.077 0 .29 s I S 0.24 0.49 : IS 0.27 0.20 : 7 S 0.12 0.10 ID

a 0.65 ± I S 0.13 G.4S : I S 0.33 0.B2 * IS 0.2B 0.14 S 4 S 0.061 0.2P 20 10 0.44 ± IS 0.11 0.39 ± I S 0.29 0.46 i IS 0.23 0.13 i SS 0.099 O.ia 111 i t 0.28 ± I S 0.10 0.61 t I S 0.37 0.B3 i IS 0.28 0.12 i 7 S 0.059 0.20 20

See Fig. 9 for sampling locations. bThc RCC is I pCl/m 3.

-32-

I

in Table 15 for each sampling location. Figure 10 shows the weekly average activities deposited on air filters front all the sampling locations. These average activities are slightly higher than those measured In the Livermore Valley. Gamma spectral measurements made on monthly composite samples of the filters collected on-site reveal measurable quantities of various gamma-emitting radionuclides as may be seen In Table 16. These activity levels are essentially iden­tical with those measured in the Livermore Valley and may readily be accounted for as being due to global fallout. The results of Isotopic plutonlum and uranium analyses, performed by the techniques described previously, are provided in Table 17. The relative abundance of 2 3 8 P u to 2 3 9 P u is approximately that expected in global fall­

out. The uranium content of airborne debris, on the other hand, is appreciably depleted relative to that of natural uranium and the concentrations are at t imes signifi­cantly greater than those measured in the Livermore Valley. This is not unexpected in view of the sizeable quantities of de­pleted uranium that have been expended over the years as a result of the high ex­plosive detonations at the Site. However, these concentrations are nevertheless far lower than the current concentration guide levels.

The calculated annual lung doses to an adult resulting from inhalation of the radio­nuclides listed in Tables 16 and 17 are shown In Table 18. These were derived in a manner similar to that used to obtain the values in Table 4. Again, these inhalation doses are extremely

a.

0.01

Fig. 10. Weekly average beta activities on air filters from Site 300 air samplers.

-33-

Table 16. Results of gamma-ray spectral measurements of Site 300 air filters (activities in pCi/m 3). '<*C H , C e 1 2 S S b 7 B e W 3 P . u W 6 R u 1 3 7 C s 9 5 Z r

January 8.8 X 10" 3 ± 2% 2.0 X 10" ! ± 7% 6.4 X 10"* ± 12% 4.1 X10" 2 ±3% 2.2 X 10" 3 ± 7% 4.0 X 10" 3 ± 12% 9.7 X 10"* ± 5% 2.8 x i o " 3 : :«,'.

February 1.5X10" 2 ± 2% 4.BX10" 3 ± 4W 1.1 X W"3 ±14% 4.7 X 10" 2 ± 4% B.4 X 10" 3 ± 4% 4.4 X10" 3±19% 1.4 X 10" 3±7% 7.4X10" 3 ±2%

March 4 .7X10" 2 ± 1% 1 .8X10" 2 * 2% 2.6 X 10* 3 ± 10% B.9X10* 2 ±3% 2.BX10" 2 ± 2% 1.8X10" Z ± 8% 3.0X10" 3 ±4% 3.3 X 10" 2 ± 1%

April 4 . 0 X 1 0 " 2 * 1% 1.1X10" 2 ± 2% 2 .2X10" 3 ± 2% B.l X10 ' 2 ±4% 1.9X10" 2 ± 3% 9.5X10" 3 ±10% 3.3 X 10"3±B% 3.3X10" 2 ±1%

May 1 . 2 X 1 0 _ 1 ± 1% i . e x i o " 2 ± 7% 0.8 X10" 3 ± 7% 1.2X10"'±3% 3.3 X10" 2 ± 2ft 5 . 0 X 1 0 " 2 * 5% a . a x i o ' 3 ± 3 % 7.1 X 10" 3 ±1%

June B.7 X10" 2 ± 13% B.4X10" 3 ± 3% 4 .7X10" 3 ± 13% 7.0 X 10 " 2 ± 5% 1.8 X 10" 2 ± 3% 4.o x io" 2± a% 5.0 X 10~ 3 t 0% 4 .7X10" 2 ± 1%

Juty 1 . 4 X 1 0 _ 1 ± 1% 8.1 X 10" 3 ± 7% 8 .1X10" 3 ± 5% 2.0 X 1 0 * ^ 3 % 1.0 X 10" 2± 4% 5 .0X10" 2 * 4% 0.7 X 10" 3±3% G.4 X 10" 2 ± 1%

August 9.1 X 10 " 2 ± 1% 2 .9X10" 3 ± 9% 5 .4X10" 3 ± 7% 1.5 X 1 0 _ 1 ± 2 % 6.4 X 10" 3 ± 6% 4 .0X10" 2 ± 6% 6.7 X 10" 3 ± 4% 3.1 X 10* 2 ± 1%

September 5.9 X 10" 2 ± I* 1.9 X 10" 3 ± 15% 3.4 X 10" 3 ± 10% 2.0 X 10"'±2% 3.5 X 10" 3 t 10% 2 .9X10" 2 ± 7% 4.7X10" 3 ±5% 1.5 X 10" 2 ± 2%

October 2 . 6 x i o " 2 ± 2% 7.5X10"* ±30% 1.4 X 10" 3±22% 1.5X10' 1 ±3% 1.0 X 10" 3 ± 25% 9.4 X 10" 3 ± 9% 1.9 X 10" 3 ± 0% 5.0 X 10" 3 ± 4%

November .? .4X10' Z ± 2% 2.7X10"* ±76% 2.4 X 10" 3 ± 17% 2 .2X10" l ±2% 0.4X10"* ±39% 1.3X10" 2 ±16% 2.8X10" 3 ±8% 5.6 X 10" 3 ± 4%

December !.8 X10" 2 ± 3% 1.6X10" 2 ± 2% 1.8X10" 3±16% 1.3 X 10" 1 ±3% 2.1 X 10" 2± 2% 1.0 X 10" 2 t 16% 1.8 X 10"3±B% 2.B.X10"3±551

Annual average 5.8 X 10" 2 7.6 X 10 " 3 3.!) X 10" 3 1.2 X 10"' 1.3 X 10" 2 2.4 X 10" 2 4.3 X 10" 3 2.1 X 10" 2

RCGa 2 X 1 0 2 5 X 1 0 3 S X 10 2 4X 10* 3 X 1 0 3 2X 10 2 5X 10 2 1 X 10 3

Percent RCG 2.9 X 10" 2 1.5 X 10"* 3.7 X 10 " 4 3.0 X 10'* 4.3 X 10"* 1.2 X 10 " 2 8.6 X 10"* 2.1 X 10 " 3

Assumes the activity is in an Insoluble form.

Table 17. Plutonium and uranium concentrations in Site 300 air samples .

Activity (pCi/m 3 ) 2 3 8 F u / 2 3 9 P u

Mass (ng/m ) 1971

Month 2 3 8 P u 2 3 9 P u 2 3 8 F u / 2 3 9 P u 2 3 5 u 2 3 8 u 2 3 5 U / 2 3 8 D

January 3.5 X 10~ 6 ± 6% 2.7 X 10" 5 ±3% 1.3 X 10" 1 1.8 X 10" 3 ±2% 9.3 ± 2% 2.0 X 10" 4

February 3.8 X 10" 6± 6% 3.1 X 10" 5 ±3% 1.2 X 10" 1 1.5 X 10" 4 ± 2% 5.4 X 1 0 " 2 i 2 % 2.8 X 10 " 3

March 8.2 X 10" 6 ± 7% 9 . 5 X 1 0 " 5 ± 4 % 8.6 X 10" 2 3 . 4 X 1 0 " 4 ± 1 % 8.3 X 10" 2 ± 1% 4.1 X 10" 3

April 4.8 X 10 " 6 ± 6% 6 . 7 X 1 0 " 5 ± 4 % 7 .2X10" 2 1.9 X 10~ 3 ±1% g.OXlO" 1 *!?" 2.1 X 10 " 3

-way 4.5 X 10" 6 ± 7% 7 . 4 X 1 0 " 5 ± 4 % 6.1 X 10" 2 2.5 X 10~ 4 ±4% 6.5X10" 2 ±4% 3.8 X 10" 3

June 4.4 X 10" 6 ± 10% 8.3 X 10" 5 ± 5% 5.3 X 10 " 2 4.1 X 10" 4 ±2% 1.8 X 1 0 _ 1 ± 2 % 2.3 X 10" 3

July 3.1 X I d " 6 * Wk U X IQ" 4 ±3% a.a x io" 2 1.2 ¥. 10" 4 42°fc 2.5 % U T 1 ± Vn 2.9 X 10" 3

August 1.8 X 10" 6 ± 15% 7 .0X10" 5 ±6% 2.3 XIO" 2 3.9 X 10" 4 ±1% 9.8 X 10" 2 ±2% 4.0 X 10" 3

September 2.8 X 10" 6 ± 6% 5 .4X10" 5 ±3% 5.2 X 10" 2 2.7 X 10" 4 ±1% 4 .9X10" 2 ±1% 5.5 X 10" 3

October 1.2 X 10" 6±12% 3.5 X 10" 5 ±4% 3.4 XIO" 2 3.1 X 10" 4 ±1% 8.0 X 10" 2 ± 1% 3.8 X 10" 3

November 1.9 X 10" 6 ± 6% 2.6 X 10" 5 ±3% 7.3 X 10" 2 2.8 X 10" 4 ± 1% 4.4 X 10" 2 ± 2% 6.4 X 10" 3

December 8 . 2 X 1 0 " 7 ± S% 1 .4X10" 5 ±4% 5.8 X 10" 2 8.6 XIO" 5 ±1% 2.7 XIO" 2 ±2% 3.6 X 10" 3

Annual average 3.4 X 10" 6 5.7 X 10" S 5.8 X 10" 4 9.3 X 10" 1

RCGa 1.0 1.0 1.9 X 1 0 3 1.5 X 10 4

Percent RCG 3.4 X 10" 4 5.7 X 10" 3 3.1 XIO" 5 6.2 XIO" 3

"Assumes the activity is in an insoluble form.

Table 18. Inhalation doses result ing from the air concentrations shown in Tables 16 and 17.

Radionuclide 144,

141, Ce

Ce 125, Sb

? B e 103 Ru 106 Ru 137 Cs 95

238

239

235

Z r

Pu

Pu

U 238 T

Calculated annual lung dose (mrem)

2.4

5.0 X 10

3.2 X 10

7.6 X 10"

1.3 X 10

4.0 X 10"

6.8 X 10"

4.4 X 10"

7.4 X 10"

1.2 X 10

2.4 X 10"

5.6 X 10"

- 2

-2

-1

-1

small with the greatest contribution being due to 1 4 4 C e .

SOIL

A limited number of soil samples were collected at several locations near the site boundary. These locations a re shown in Fig. 11. The samples were collected and analyzed by the same techniques a s those collected within the Livermore Valley. The concentrations of the various rad io­nuclides of interest are given in Table 19 and the resul t ing deposition levels a r e shown in Table 20. Inspection of the data reveals that the activities of the artificially produced radionuclides may reaaDy be accounted for as due to global failouj with no detectable contamination a s a resul t of Laboratory operations. The data in Table 21, however, indicates the

-35-

—I -

i » o 8 ' « i * S T u

Fig. 11. Site 300 soil sampling locations.

5U/a"'uXJ ratios are slightly depleted 235^/238. 235 in U with respect to those observed

within the Livermore Valley. This may possibly be due to the depleted uranium being expended in the high explosive deto­nations at the site although more data will be required to definitely ascertain this relationship.

WATER

Monthly samples were collected from on-site wells supplying Site 300 and from

various on-site and off-site springs, ponds and creeks. The locations of these sites are shown in Fig. 9. Locations 1 through 7 represent deep-well sources, Locations 11 and 14 are off-site creek sources, and rain water i s collected at Location 20. The remaining locations pre on-site ponds or springs. The samples were subjected to gross alpha and beta analyses. No sam­ples showed a gross alpha activity above the limit of detection of 1.2 pCi/liter. The gross beta activities averaged over 3-month periods are given in Table 22. These

-36'

Table 19. Activity levels of various radionuclides in soil at Site 300 (pCi/g). S^nii'- tag Depth location (cm)

0-1

0-24

0 - i

0-24

0-1

0-24

0-24

0-1

0-24

0-24

0-25

0-25

0-25

0-25

0-25

0-25

4

5

G

7

8

9

10

11

12

" " P u

3.3 X 10" 3 i 5?.

2.6 X JO' 3 i I0«^

1.3 X 10" 3 t 10°".

2.3 X 10" 3 i SO"-.

5.3 X 10" 3 ± 5«".

*Ce

2.5 X 10" 3 ±

2.7 X 10" 3 ±

1 . 7 X 1 0 ' 3 ±

1 . 7 X 1 0 " 3 !

G.GX 10" 3 ±

2.0 X 10

3 . 1 X 1 0 ' 3 ±

4.7 X 10 " ; 4=".

5.1 X 10 '" z 67.

G.2 X 10 _ * 5=".

O.G X 10" 2 ±67«

, - 3 ,

67.

Cf.

5H

47.

s*» or.

2.8 X 10" 1 ±387«

o.i x io - i 3 2 7 ,

5 . 3 X 1 0 " ' r G7. ! 2 X 1 0 " 1 ; 2 G e ;

9.4 X 10" 2 : 191

3 . G X 1 0 " ' i 75. 6.2 X 1 0 ' 2 ± 3G7= 2.3 X 10" 1 ± 407,

5.0 X 10" 8 ±31T.

1.0 X 10"' ± 177.

5.G X 10" 1 r 77.

4 0 K

4.6 ± 115

2.7 ± 197.

4.7 ± 117.

1.5 ± 3«i

5.6 ± ST,

4.3 ± 11^

Table 20. Deposition levels of various radionuclides in Site 300 soils (activities in mCi/km2).

Sampling location 2 3 9 p u ^ S r l 3 7 C s 95™ a Zr 1 4 4 C e

1 0.89 14 <! 0.78 25 1.5 3.5 3 0.48 13 12 0.78 2.9 4 0.72 15 25 5 1.7 19 6 0.81 22 7 0.93 8 0.68 9 0.56

10 2.3 11 0.74 12 1.2

activities show little variation witt ime and location and are similar to those ex­hibited by the water samples collected within the Livermore Valley.

These samples were also subjected to tritium analyses by electrolytic enrich­ment and subsequent scintillation counting. The results cl the analyses are shown in

-37

Table 21. Concentrations of uranium in Site 300 soils (ng/g).

Sampling Depth location (cm) 234 U 235 U 238 r 2 3 5 u , 2 3 8 u

c l

1 0-24

2 0-24

3 0-24

4 0-24

5 0-24

6 0-24

7 0-25

8 0-25

9 0-25

10 0-25

11 0-25

12 0-25 'The 235u/238fl

1 . 1 6 X 1 0 _ 1 ± 2% 1 .80X10 1 ±1%

1.15 X 1 0 _ 1 ± 10% 1 .46X10 1 ±1%

1.19 X 1 0 _ 1 ± 1 0 % 1 .40X10 1 ±1%

7.10 X 10~ 2 ± 10% 9.04 ± 1%

7.73 X 10" 2 ± 10% 9.50 ± 1%

1 . 2 6 X 1 0 _ 1 ± 1 0 % 1.55 X 10**1%

1.51X10~ X ± 10% 1 .73X10 1 ±1%

1.16X10" 1 ±12% 1 .56X10 1 ±1%

8 .85X10" 2 ±11% 1 .10X10 1 ±1%

1.01X10" 1 ±12% 1.42 X I O 1 * ^

1.38 X lO" 1 ± 10% 1.59 X 10 1 ± 1%

1.09X10" 1J:11% 1.36 X 10**1%

2.60X10 ±1% 6 .9X10

2 . 1 0 X 1 0 3 ± 1 % 6 .9X10

1 .99X10 3 ±2% 7.0X10"

1 .29X10 3 ±2% 7.0X10"

1.37 X 10 3 ± 2% 6.9 X 10

2 .2 4 X 1 0 3 ±2 % 6.9X10"

2 . 4 5 X 1 0 3 ± 1 % 7.1X10"

2 . 3 3 X 1 0 3 ± 1 % 6.7X10"

1 .60X10 3 ±2% 6.9X10"

2.13 X 10° ±1%

2.27 > 10 3 ± 1%

2.00 X 10 ? ± 1%

-3

-3

-3

6.7 X 10 -3

7.0 X 10 -3

6.S X 10 -3

ratio in natural uranium is 7.2 X 10" 3 .

Table 23. With the exception of samples collected at Location 25, these samples contain tritium activities that are com­parable with those observed in water samples collected within the Livermore Valley. The elevated tritium activities observed at Location 25 appear to be due to tritium being leached out of contami­nated wastes that have been stored at a nearby location. Adjacent to this spring is a deep-water well at Location 6 which apparently has not been contaminated.

Table 23 also includes the calculated whole body doses to an adult consuming ths water containing the listed tritium con­centrations. These doses were derived in a raanner similar to that used to com­pute the values listed in Table 10. As one would expect, the doses are insignificant with the exception of Location 25 where it

would be possible for 23 mrem to be de­livered to an individual consuming 1 liter per day from this spring. It is quite un­likely, however, for any individual to drink this water directly, since the water perco­lates back into the ground a few feet from the spring.

VEGETATION

During the last quarter of 1971, vegeta­tion samples were collected on a monthly basis at 7 sampling locations shown in Fig. 9. Dried monthly composite samples were subjected to gamma spectral analyses yielding the activities of l Cs, " * C e , QR 7 4fl

Zr, Be, and K. The average activi­ties are shown in Table 24. Also shown in the table are the calculated whole body or critical organ doses delivered to an adult

-38.

Table 22. Average gross beta activities in Site 300 water samples during 1971 (activi­t ies in pCi/1).

Sampling location January-March Apri l -June July-September October-December

1 5.5 3 .0 5.2 2.8 2 11.0 4 .2 4.9 6.2 3 8.7 5.5 6.5 7.7 4 5.9 4.8 4 .6 4.0 5 4.8 5.9 5.1 5.2 6 6.2 5.1 4.8 4.5 7 4.0 4 .2 5.4 5.4

11 8.2 9.7 6.8 6.3 14 4.8 4.1 2.8 4.1 20 — — — 15 21 — — 9.8 9.0 22 — — 22 — 23 — — 7.6 7.8 24 — — 5.3 7.9 25 — — 2.9 2.8 26 — — — 5.5

Average 6.6 5 .2 6.7 6.3 Percent KCG a 22 17 22 21

RCG (beta activity) = 30 pCi/1.

Table 23. Tritium activities in Site 300 water samples.

Location Tritium activity (pCi/1) Maximum Average Percent RCG

Calculated annual adult whole body radiation d o s e

(mrem)

1 1.8 X 1 0 1 ± 50% 1.6 X 1 0 1 1.6 X 1 0 " 5 6.4 X 10~*

3 4.1 X 1 0 1 ± 22% 2.6 X 1 0 1 2.6 X 1 0 " 5 i.oxio" 3

4 1.8 X 1 0 1 ± 50% 1.6 X 1 0 1 1.6 X 1 0 " 5 6.4 X 1 0 " 4

6 3.6 X 1 0 1 ± 25% 3 .1 X 1 0 1 3.1 X 1 0 ~ 5 1.2 X M » - 3

7 1.5 X 1 0 2 ± 12% 3 .5 X 1 0 1 3 .5 X 1 0 " 5 U 4 X 1 0 " 3

8 3 .6 X 1 0 1 ±25% 2.0 X 1 0 1 2.0 X 1 0 ~ 5 8.0 XVT*

11 8.1 X 1 0 1 ± 11% 6.0 X 1 0 1 2.0 X J Q * 3 * 8.4 X M f 3

14 3.6 X 1 0 1 i 25% 2.8 X 1 0 1

-** 9.3 X VT* l a x w"3

22 8.3 X 1 0 1 ± 13% 6.0 X 1 0 1 6.0 X 1 0 ~ 5 2.4 X 1 0 " 3

23 3.3 X 1 0 1 ±26% 2.9 X 1 0 1 2.9 X 1 0 " 5 1.2 X 10""3

24 6.7 X 10* ± 13% 5.8 X 1 0 1 5.8 X iO" 5 8.3 X 1 0 " 3

25 7 . 2 X 1 0 5 ± 2% 5.8 X 1 0 5 5.8 X 10" 1 2.3 X 10"

26 7 . 5 X 1 0 2 * 4% 7.4 X 1 0 2 - 2 a

2 . 5 X 1 0 * 3 .0 X l O " 2

Average 4 .5 X 1 0 4 1.8 Off-site locations:

Off-site RCG (HTO) = 3 X 10° pCiA. On-site RCG (HTO) = 1 X 1 0 s pCiA-

- 3 9 -

Table 24. Radionuclide activities in Site 280 vegetation samples.

Radionuclide Average activity

fpCi/g)

Calculated annaai radiation dose to man via

direct iogesttoa dmremj Critical! organ:

m C s 1.4 x ia~l 2.6 X I 0 " 1 WbatebEKfy K i C e 7.0 X 10~ l 5.6 Lower large intestine

9 5 2 r 7.8 X 10" 2 1.8 X 10~* Lower large irSesfcine

*Be 2.1 1.1 X i o ~ l Lower large intestine

^ 4.T 6.4 Whole body

Table as. Tritium activities in Site 300 vegetation samples.

location

Average tritium activity

Calculated annual adult

radiation dose fmremj

4 S . 3 X 1 0 2 ».T X 1 0 - 3

S 7 . C X 1 6 2 1.1 X 1 0 - 2

S 2.8 X 1 0 3 4.5 X 1 0 ~ 2

7 8.3 X 1 0 2 1.3 X 1 0 ~ 2

8 T . 4 X U 2 1.2 X 1 0 ~ 2

10 6.7 X 10* 1.1 X « T 2

12 6.8 X I S 2 1.1 X I © ' 2

Average 1.0 X 1ft3 1.6 X VT2

by direct ingestion of 406'grains per day of edible vegetation coataijuog 80H> water and the listed activities. Again, the data

40 144 reveals that K and Ce are the anaior contributors via this pathway.

These samples were also subjected to triiiom analyses by freeze drying and sufasetyient electrolytic enrichment and scintQIatBon counting of the resulting water. The average activities measured at each location are shown in Table 25. With the exception of Location 6. the activities show remar&ab*y little fluctuation a s com­pared with the results obtained irons s imi­lar samples collected within the Evermore Valley. Location 6 represents a waste disposal area where tritium-contaminated waste i s stored. The table also includes the resulting whole body doses delivered to an adult by the tritium activities based upon the models referenced previously. As one would expect these doses are insignilicsnt.

- 4 G -

Appendix

Environmental Activity Guide Levels

The JSandards for Radiation Protection (ABC Sfe&aal Cfeapter 0524. i ssaed 11 S 68) s tate that if t h e r e i s a mixture in a i r aod water of radionuclides whose identity and concentrations a r e unknown, the average activity should not exceed the following ralaes; 1. Air (controlled area) 6pCi in 2 . Air (uccortrolled area) 0.02pCt/m 3 . Water (controlled area) 400 pCi l i t e r 4 . Water {uncontrolled area) 30pC^l i ter

!f S i s known that alpha emi t t e r s and 22T

Ac a r e not present , the following guide values may b e used t o determine the p e r ­missible average activity: 5. Air (controlled area) 30nC^B» J

6. Air {uncontrolled area) IpCt&a If it i s known that 129, 2 2 S R a . and

: a r e not present, the following values m a y b e used: 7. Water (controlled area) 3000 pCi/liter *. Water (uncontrolled area) 10QpCi4iter

The a i r and water samples a r e s u b ­jected to g r o s s alpha and g ross beta m e a s ­urements . The average annual alpha activities may not exeeed those l i s ted under points 1 through 4 above. Since the alpha emi t te rs have been accounted for in the g ross alpha measurements, and the

1'9 227 assumption i s made that I. Ac.

T l a , and Rs a r e not present in the samples, the anaiial average g ros s beta activities of the samples may not exceed the act ivi t ies listed under points 5 through 8 above. The assumption that 1 2 9 1 . 2 2 7 A c ,

and a r e not present in a i r and water samples i s reasonable in view of the minute quantities of these r ad io ­nuclides available at the Laboratory. AEC Manual Chapter 0524 also s tates that the -veraf-s t r i t iom activities in off-site water samples may not exceed 3 X 1C pCi/liter.

Since analysis for L Ra. and act ivi t ies is? made on samples col­

lected from the Laboratory's sewage effluent a t t he point of discharge into the Livermore ci ty sanitary sewer system, the g ross alpha and beta activities in the samples collected from the effluent d i s ­charged from the Livermore sewage treatment plant should not exceed the 100 pCi l i t e r l is ted under point 3 above.

The annual external whole body radia­tion dose to workers in controlled a r e a s may not exceed 5 r e m : while that to an individual in an uncontrolled a rea may not exceed 500 m r e m . An average annual dose of 170 m r e m may not be exceeded for a group of individuals in an uncon­trolled a r ea .

- 4 1 -

References

1. P. L. Phelps, K.O. Hamby, B. Shore, andG.D. Potte.-." A Ge(Li) Gamma Ray Spectrometer for High Sensitivity and Resolution, for Biological and Environmental Counting.." Advances in Chemistry No. 93 (Radionuclides in the Environment), American Chemical Society, Washington, D. C . 1970.

2. "Task Group Report on Lung Dynamics for Committee II of the International Radiological Protection Commission, Deposition and Retention Models for International Dosimetry of the Human Respiratory Trac t , " Health Physics 12 (1966).

3. N. Y. Chu, "Plutonium Determination in Soil by Leaching and Ion Exchange Separation," Anal. Chem. 43_(1971).

4. E. P. Hardy and P. W. Krey, "Determining the Accumulated Deposit of Radio­nuclides by Soil Sampling and Analysis ," Proceedings of the Plutonium Symposium held at LASL August 4-5, 1971, Los Alamos Scientific Laboratory Rept. LA-4756 (1971).

5. H. L. Beck, et a l . . Further Studies of External Environmental Radiation, USAEC Health and Safety Laboratory, New York, N. Y., Rept. HASL-170 (1966).

6. H. L. Beck and G. de Planque, The Radiation Field in Air Due to Distributed Gamma-Ray Sources in the Ground, USAEC Health and Safety Laboratory, New York, N. Y„ Rept. HASL-105 (1968).

7. H. A. Wollenberg, et al., "Natural and Fallout Activity in the San Francisco Bay Area," Health Physics 17_(1969).

8. Agriculture Statistics, 1969, United States Department of Agriculture, U. S. Government Printing Office, Washington, D.C. (1969).

9. L. R. Anspaugh, et al.. The Dose to Man Via Food Chain Transfer Resulting i rom Exposure to Tritiated Water Vapor, Lawrence Livermore Laboratory, Rept. UCRL-73195 (1971).

10. Y.C. Ng, et al . . Prediction of the Dosage to Man from the Fallout of Nuclear Devices, IV; handbook for Estimating the Internal Dose from Radionuclir es Released to the Biosphere, Lawrence Livermore Laboratory, Rept. UCRL-5Q163 (19 ).

-42-

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