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Declassified record · U.S. Department of Energy

Operation Castle - Project 2.6A, Chemical, Physical, and Radiochemical Characteristics of the Contaminant (Deleted)

Dated
Sep 30, 1955
Document type
Report
Length
152 pages
Open the original scanArchive record OSTI ID 16036916 · public domain

Archive description

The bomb debris from surface, land and water shots at operation castle was studied to determine the physical, chemical, and radiochemical cha racteristics. The fallout from the surface land shots consisted chiefl y of irregular white particles 25 micro to 2 mm in diameter. They were derived from coral and had the radioactivity concentrated near their s urfaces. About 5 per cent of the activity in the solid fallout was wat er soluble; 95 per cent dissolved in dilute acetic acid. The fallout f rom the surface water shots was invisible both in the air and after it had deposited. It was collected on special filters and on a film by el ectrostatic precipitation. The filters and film and their autoradiogra phs were studied microscopically. These studies showed that the fallou t consisted of microscopic solid crystals and small droplets. The auto radiographs indicated the presence on the filters of many particles wh ich were invisible under the microscope. The major part of the radioac tivity was associated with crystalline aggregates and droplets up to a bout 2 mm in diameter. Water dissolved from 60 to 90 per cent of the r adionuclides from this type of fallout. Fallout and cloud samples from land and water shots were analyzed chemically for major constituents a nd trace elements including many of the radionuclides. Coral and sea w ater contributed the major constituents, bomb products being present i n trace concentrations. Radiochemical analysis showed the valley of th e fission product yield curve was about 20 times higher and the heavy wing at mass 156 about 6 times higher than the yield curve from therma l neutrons on u-235. The important induced radionuclides were u-239, u-237, and u-240. The presence of these had a marked effect on the decay curves and energy spectra especially at intermediate times after detination. The neptunium was distributed between oxidation states; iodine occurred principally as iodide. The information obtained from these studies has aided in (a) an understanding of the mechanism of formation of the fallout, (b) assessing the radiological situation in fallout areas, (c) synthesizing simulants for laboratory studies, and (d) interpreting data obtained in proof tests of countermeasures for ships. This document is a deleted version.

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Machine-read from the scan, so expect some errors. Lines that couldn’t be read are left out.

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Chemical, Physical, and Radiochemical Characteristics of the Contaminant Pacific Proving Grounds Headquarters Field Command Armed Forces Special Weapons Project Sandia Base, Albuquerque, New Mexico This is an extract of WT-917, Operation CASTLE, Project 2.6a, which remains as of this date. Extract version prepared for: DEFENSE NUCLEAR AGENCY

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Chemical, Physical, and Radiochemical Characteristics of the Contaminant U.S. Naval Radiological Defense Laboratory San Francisco, California Headquarters Field Command Armed Forces Special Weapons Project Sandia Base, Albu,querque,New Mexico Approved for public release; unlimited distribution. s. TYPE or RLPOWT a PCRIOO COVEREO IO. PROGRAY ELLYE~T.PROJCCT. TASK 7. OISTRIBUTION STATEUENT (ot the l brrrrcl cnlrred In BJock 70. II dllf~rml lrom Report) This report has had the classified information removed and has been republished in Jnclassified form for public release. This work was performed by KarnanTempo under zontract DNAOOl-79-C-0455 with the close cooperation of the Classification Management Division of the Defense Nuclear Agency. ~__-.___ Operation CASTLE Bomb Debris

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This report has had classified material removed in order to make the information available on an unclassified, open publication basis, to any interested parties. This effort to declassify this report has been accomplished specifically to support the Department of Defense Nuclear Test Personnel Review (NTPR) Program. The objective is to facilitate studies of the low levels of radiation received by some individuals during the atmospheric nuclear test program by making as much information as possible available to all interested parties. The material which has been deleted is all currently classified as Restricted Data or Formerly Restricted Data under the provision of the Atomic Energy Act of 1954, (as amended) or is National Security Information. This report has been reproduced directly from available copies of the original material. The locations from which material has been deleted is generally obvious by the spacings and "holes" in the text. Thus the context of the material deleted is identified to assist the reader in the determination of whether the deleted information is germane to his study. It is the belief of the individuals who have participated in preparing this report by deleting the classified material and of the Defense Nuclear Agency that the report accurately portrays the contents of the original and that the deleted material is of little or no significance to studies into the amounts or types of radiation received by any individuals during the atmospheric nuclear test program.

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GENERAL SHOT INFORMATION shot I Shot 2 Shot 3 Shot 4 Shot 5 Shot 6 DATE I March 27 March 7 April 26 April 5 Moy I4 May ( Unclassified ) Brovo Romeo Koon Union Yankee Nectar Bikmi, West of Bktni, on Barge ot IntersectIon of Arcs with Radrc of 6900’from Dog (Yurocht ) and 3 Statute Miles Emwetoh, IVY Make TYPE Land Barge Lond Barge Barge Barge

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The bomb debris frcm surface, land and mater shots at Operation CASTLEwas studied to determine the physical, cbamlcal, ard radioThe falloutfmm the surfacelarrdshota aonsistedchieflyof irregularwhite particles25 p to 2 mm in diameter. They were derived from coral and had the radioactivityaoacentmted near their surfaces. About 5 per cent of the activityin the solid falloutwas water soluble; 95 per cent dissolvedin dilute acetic acid. The fallout fran the surfacewater shots was invisibleboth in the air and after it had depsited. It was collectedon special filtersand on a film by elsctroataticprecipitation.The filtersand film ati their autoradiograqhs were studiedmicroscopically.These studiesshowed that the fallout comisted of microscopicsolid crystalsand small droplets,,,The autoradiographsindicatedthe presenceon the filtersof many particles which were invisibleunder the microscope. The major part of the radioactivitywas associatedwith crystallineaggregatesand dropletsup to about 2 mm in diameter. Water dissolvedfrom 60 to 90 per cent of the radionuclidesfrom this type of fallout. Falloutand alo*A samplesfrom land and water shots were analysed chemicallyfor major constituentsand trace elemen+,sincludingmany of the redionualides,Coral and sea water contributedthe major aonstituents, bomb productsbeing presentin trace eonaentrations.Radiochemical analysisshowed the valley of the fissionproductyield curve was about 20 times higher and the heavy rringat mass 156 about 6 times higherthan the yield curve from thermalneutronson 0235. The importantinduced had a marked effect on the decay curvesand energy spectraespecially at intermediatetimes after detonation. The neptuniumwss distributed The inf'onuationobtaiaedfromthese studieshas aided in (a) an lante for laboratorystudies,ard (d) interpretingdate obtainedin proof tests of countermeasuresfor ships.

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Thfs report 58 one of the report8 pm8nting the lwultrr of the 34 projeotlr participating in the Yilltaw Ef’fwt8 Torta Progmmnof Operation CASTLE, which in&&d six tort detonations. For reader8 l,nterrated in other pertinent te8t fnfonbation, reference is made to Yilltary Effeats Program. This 8mmary report includer the following infomtion of possible general interest. a. & over-all description of each detonation, lncludlng field, height of burst, ground son, loaation, time of detonation, ambient atPaoapheric conditiona et detonation, eta., for the c. A sumnary of eaah project, incltiing objective8 aad X98tllts. d. A completelisting of all report8 covering the Military The treatment and analyses of samples and the intemretation of the results in determining the characteristic8 of the baob debri8 from Operation CASTLErequired extensive partlaipation by many iadivlduals. and (c) Radiochemical Studies 8-w Dmsented in Chapters 3,4, and 5, respectively. The participation in each phase of the work is described The Chemical Studies consisted of observations and measurements made at the site and analyses for major ard minor constituent8 at the U.S. Naval Radiological Defense Laboratory (USNRDL). The field studies and the preparationof Chapter 3 were directed by C.F. Miller. D.Sam, . The Physical State Studiesmrs performedby R.Cale who also prepared the portion of Chapter 3 posenting the resultsof these studies. The oxi&-

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stituents in the falloutsamplesand the background sam~~les of coral and sea water)R.W. Rinehartaided by J.A. Seileranalyzed them for the trace elements. An ion exchangeprocedurefor separatingsome of the radionuclideswas developedat the site by C.F. aillerand J.F. Pestaner, Studiesof the physicalpropertiesof falloutmaterialinvolved developmentof collecting devices, collectionof samplesin the field, and analysesof sampl6~ at USNBDL. This work was done under the direction Adams, In it are discussedthe measurementsof the physicalproperties of the falloutmade on samplesfrom an electrostaticprecipitator,liquid dropletcollector,and filter samplers. The sample collectionswere made precipitatorwas developedby N.R. Farlow and F.A. French. Chapter 5 which described ths Radiochmical Studies was p~~~pared by LA Bumep and C.F. Miller aided by B. Singer, L.H. Gevantxanand W.J. Heiman. St=tdissof neutron induced rsdionuclides were dizwted by L.9. Cevantmlln.The decay and adsontion measurements were startedat times at USNRDL by L.D. McIsaac,L.R. Bunney ard E*R. Roberta. The interpretation of these data as presented in this report was made by R.J. Heiman. The gamma analyser was converted from an alpha analpaer sampleswe= made by all members of Project 2.6~ present at the site. R.J. Heiman and C.F. Killer interpreted the data for the report. !I%e analysis of K& was performed by B. Singer. Radiochemicalanalymes for fissionproduct and heavy element radionuclides were perfoxsed at out the plan&q and execution of the project. Capt. Be Be= tdc,m, contributedboth bp his advice ssd aid in making the saintillation

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3.1.2 Samples from Shot 2 ............... 3.1.3 Samples from Shot 3 ............... 4.1.2.5 PhysicalState of Activityon Air

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Gamma Decay of PhysicalState Fractiousof Sample Lead AbsorptionCurvee at 8.3 Days for Sample 251.03, Lead AbsorptionCurves at 3.6 Days for Sample 244, Lead AbsorptionCurves at 5.3 Daya for Sample2-A4, DensityDlatrilmtionof Davioe Arotion for Shota 1,2, Diatributloaof tha Batik of tbo RadlatlonField to the Distributionof the Ratio of Um RadiationField to ths Distribationof the Ratio of the Radi.ationField t0 tie

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Size Distributicnof Active AerosolPartlcloofxa Photcmlcrographa of Fkdiculctive Areas of Hlllipo_reFillms, Gmss Beta Decay of FalloutSanplos from Shots 1,2,3, Gross Gamma Decay of FalloutSampler froplShot8 1,2,3, Decay Curve of Na24 Sample from Shot 2 .......... Facsimileof Chromatcgrm Taken from the Eaterlirm-Angua Detemined by Lead Abeorption .............l Mass Distributionof Elmnenteof Interestin Liquid and Sunmary of Resxlts for State of Iodine .......... Spectrophotometric Analysisaf Minor Conetituents ....

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ConcentrationAnalysisof Solid Fractionsfrom Fallout SpecificGravityof Active hterial cettlingon Decks of Gamma Energy basurements from Sample 4-Y39,Shot 4..,.. Energiesand Gross Mstribution of Gamma Rays from Gross Average Bard Gamma Energyfor Each Shot ........... lmounts of Neutron Indwed BadionuclidesProduced& Nmber of Atcmc of @37 and U239 Relativet0 bber of

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crreatedebllitatlag effects far beyoui the xwge of its blast dsmago. its physical, Weal and radiochexkal pmpsrties l ra premquirite u developlent of mundoxmeasuree agakmt its radiatibn fieUs, At opsratlon CASTLEthe transport and distribution of fallmt vaa primaim~ the concern of Projects 2.58 a& 6.41 Projwt 2.5b rtudiad the mlout OPIislax&~ near the rhot point; lnvostlgrtion of fa:Lluut propartdee was the concern of Pmjectr 2.69 and 2.6b. The purpose of Project 2.k war to invesfigate the &ml&al, physical, and radloahemical properties of tha fallout fort a. Deducing the mechanianl whereby oantarinant is formd. marfar oounte 78 for ahipu. 1.1.1 Mechanism of Contsalination Forratieg The aontamination folaed frcm rurfaoe or sub-surface detonation detonations. Eech of these operations represented a unique uond%tion of detonation, but prorided insuff%oient data to establish bases for pmdictlng radiological effects for a ride range of probabxe cordiflona of detonation. An tierstanding of the mschaniumwhereby c?ontamlnation ir produced is necesw in makIng such predictions. Data obtained in CASTLEare applicable In answering such queatione on the mechanics of the event as: To what extent is wet contcuninant fomed by condensatlolr phenomena? With what type of particles do the primav partialas of

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radioactivedebris associate? What is the rate aud extentof Kattliq out and mildng of falloutdepositedon the water surface? Owing to the incompleteneesof the data taken at Shot Baker, cROSSRoADs,essentiallynothing was knaan prior to cdsTu concemling the mechanism of formationof wet contaminationfrom this typs of burst. The relativecontributionsof base surge and falloutwere uncertain; the roles of condensation,evaporationarxlmixing with sea water in the productionof eitherbase surge or falloutwere unknown. Particlesize and individualparticleattiiesundertakenat JABCLEand IVY have yielded considerableinformationon the mechanismof formatica d$s reactionsof dry contaminantsfrom these operaticns..-%-1, been undertakento solve presumedfield radiologicalproblems'butin many cases lack of full-scaleteat data has made it impossibleto define them clearly. For example,before CASTLE it had not been determined whether an internalcontaminationhazard would be producedon ships by tion from falloutin the water with that on contaminatedships could not be calculatedbecausethe rate of eettliag or mixing of the oontaminant in the water was unknown. Insolubleparticleswill c?ettledepending on size ariddensitywhiledissolved(ionio)contaminantswill mix; ment of such radiologicalsituationsand the developwot of counteneesurea require a knowledge of many physical and chemical pmpertles of the LixLteddata eldst with regard to the contaminanta which may be produced by surface and uz-zergroti detonationsbecame of the atypical nature of the soils at IVY and JANGLE. No direct lnforaration has been obtained on the natureof contsminmtsfromurrderwaterdetonations.For this reason,there Is specialinterestin surfacewater shots which should pxwduaea contamimmt most similarin natureto that flm an 1.1.3 Snecificatlonsof Simulantsfor Radio&&al Contamia are to be obtalned,it is essential that the artiiicialoonferd.nsnts used must sinulaterealones In chemicalaxI radlochemicalomposltion and In importantahgical and physicalcharaateri8tics.In the part, It Is importantto know the extent of dlfferenoein ftision yields for nuclear processesother than slow flsslonaxx!whetherinducedactltities contributeappreciablyto the contamination. Mwlly, It is necessaq to evaluatethe relativecantributioncfarch radioelmt to ocmtaxdnation fields on the basis of its yield and the mmber aad energy of the gammarqys emittedby the variousradionuclidesof that element.

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Fiastan fldd curves have been determined for oafiow fisafa e the important radionuclldea produced by tie detonation of m type5 The presence of activities induoed in elemerts foti i.5sea +ar was reported for Shot baker at CR~,CFdADS. An analysis for i&uoed ,+&vsties was also lpadeat ,TANGLE,l9r~/'It wa8 shown that the single m, However, scm unoonfimmd data indicated an activity pmssnt in B@I yield at early tinee,~ Detonation of certain of the CASTLE devioes mr mater posed the qtmstion of the extent to which importmt l.uiltumj ~loulstfons for eetiratlng the conttibutioa of different chmi- (H3. alsmsnts to the rota of gama radiation have been mado. 'Piold from slow neutron fission we28 used. Data regarding the numberead energy of the gamma rays emitted by various redionuclld68 were incomplete. To Lpmve the validity of these impmtant calculation5 better radlonuclide field data were x'e@r%d. Also it ms important to measure the gamma mrgiea of a few r5dionuclFde5, for which the energies had n.otbeen It has been shown that contamination-decoataminat~onbehavior is a fknction of the phpsical and chemical pqnsrtlae of the contamirmbrt. rpstsm. TM5 15 Illustrated by the ease with which gross particulate contaminants are remved,32by the relation of particle siz6 to decontandnation efficiency,ls/ati by the influence which comosltion and tiveness.22,23,24,10/Definition of the real cor&.minant system was therefore an tiportant prerequisite for apecificaticn of COntamiriaIh Def3nltion of any chemical system reqtires a knowletdgaof the identity ark!amounts of Its various coaponents. The contaminatirq!fnllout from each shot consist5 largely oi nouradioaative materials. The pxwduction of realistic laboratory contaminants for more basic infomation about radiological decontamination has, in the past, 8uffsmd severely from the absence of elementerg information about the actual oontemin5tion-decontamination system in question. Since real contanination had not bemaallablc, many investigations were conducted using high‘_y questionable contmlnation praceduras with no available mean5 of relating the data to real events. Knowledge of the concentration5 of WCM constituenta along with radiochetical anal*icel data provide all the information needed to ptspa1-6laboratory contaminants wh:icbwould conaiatently have the same cereral decontem~nation characteristics. isoconcentration plats from them data, laboratory experiments 011tb6 effect of level on deccntamj.mtlan can he investigated -2Ua'bly. The themodgrulmic statea of imctive or bulk materials usually am of greater importance than those of the radioactive ConatitumtsIt is iaconceiveble, for any radiological contamination Gf interest,

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of the total fallout. Henoe, mo8t of the properties of the contaminant aoept the radiation characterietics will be essentially determined by the inactive elements. Therefore, =*aais was plaoed on detezmining the states of the Inactive constituent8 apd the states of a few important gsmmaemitting elementa. 1.1.4 Proof Testing Atomia Warfare Countermeasures for Shim_ There has been extensive laboratory and field scale development work on atomic warfare (AR) countermeaaurea for rhipa.i/ Project 6.4 teated the washdownsystem at CASTLEand cor.ducted decontamination operations on the ships used in the operation. Since the contamination found from certain of the shots of CASTLZdiffered fnnn either real or simulated contaminants previously strrdied, detailed knowledge of the pmperties of the oontaminant wa8 needed for interpreting these re8ult8. Information on the rate of radloaative deoay, gross gammaenergy rpeotrum, ard the ratio of bete. to gammaradiation wa8 Miehed by

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Chemical, physloal, aad radiochrmicel masurement8 mre made oa the fallout samples collected at lagoon, island, and ma 8iations. Short lived radioactive species uere analyzed In the fomard am; the remainderof the analyses we- made et U.S. Naval Radiological Defense frborstory. Owing to many unforeseen difficulties early samples for the radiochemical analyses were not obtained, although early deoay dats were obtained fmn several shots. The nmber of sarllple8 colleoted m8 6uch smaller than planned. Huwcver, it wad possibl8to g8t considerable fnformation concerning all planned phasea 8xcept those involting very short lived radioisotopes. b. Concentration of maor0 conetittmnte, primarily the elmate which occur naturally in coral ard 88a water, but also the elements present in large amountr 5.n the weapon assemblyalldaesociatedequip co Ozddation state of certain mdlonuclides whose flnal state under the corrditione of the detonation could not be predicted, and whoscr contuainatlon-decontaminationbeharloris believedto depend upon their d. Slse distributions of fallout drop8 and particles, alrd the rarlatfon of these distributions throughout the Sampling amy, e. Specific radioactititles and salt content of various particle end drop size fraction8in fallout. …

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