GAMMA‘RAY $PECTROM£YRIC SYSTEMS OF RADIOACTIVE FALLQUT ANALYSIS Thesis {or ”10 Degree 0‘ M. S. MICHIGAN STRTE UNVERSETY Ronaid L. Hangen 1963 THESIS This is to certify that the thesis entitled GAMMA-RAY SPECTROMETRIC SYSTEMS OF RADIOACTIVE FALLOUT ANALYSIS presented bg Ronald L. Haugen has been accepted towards fulfillment of the requirements for Masters degree in Mechanical Engineering _/J Major professor Date z/z/(lm'b/V/ /@ 0-169 LIBRARY Michigan State University 3.1—3.1. :72.- A- .» ‘ w Th. nochmfim of tho fallout radionuclide trench: rm tho a‘lmccphcrc “E1111! nudicdbyucinga gums-ray spectrometric cyctcmcruulysic. Tho Misti" ncccurcmnt of scrotal long-lived "fallout radicicctcpoc' inbothaircndnincamphcmdctcmd. Tho syltmctcmlycic tor tum-Worth“. icotcpccm devised usage octet simul- tamcnc equations for making tho necessary mutual comment. A computer program for than solution is included. rho game-cw spectra of the samples (colloctcd at daily marvels) arc wanted. The Winn mum-nu. method of isotopc and 11mm calibration. and tho calculation of thc isotope mutations from flu Mn an discussed. ThomflydsofcbothBSdaflyaircamplumdhsmsamplcafrom tthuisingmampnscntcd. Grccsbctamlymotthcurmdrain samples m described and their sciatica to tho WW analysis is gmptdcally presented. Finally. a prcthccic on the transfer mechanics of tho radicmclidcc is propane! based upon thc cremation of tho field study. GAIQWRAY SPECTROI'E‘I‘MC SYSTWS OF RADIOACTIVE FWD? W By Ronald L. Hanger; A THESIS Buhuittcd to ' Pacifigan State University in partial Want of the rcqvircnents for the degrcc of imam OF SCIENCE . Deparmmt cf mohanical mgmeemng 1963 '.‘ ;) ABLE CON ‘13‘1‘3 Abstract‘...’OOOOOOiOOOOICO..0. matafFimcccccccccccccccccc‘ccc Chapters IIntrodmtim23é..........ac... HHWtWStWoccccccccclcccccc- 9 III Atmocpha'ic Radioactivity and It: transfer to Rain. IV The Gama-ray Scintillation'Spmmctcr. . . . V Quantitative Analysis of Gama Spectrographa. . VILaboratmInstmmtationmdPrcccdurc.... m Collecticm mum-icy a: filtering Walt. . ‘Eiimmsisandnicmcian......i..... IIGoncluaims.................. fierce-mans....'......-..u.......... Appmdiccs F A Gama-ray Spectra at thc Fallout Radioisotopca. BeanpntwrProms............... GAnaJyucchMplu.............. DWtUacd..-................. ..i 00‘ .03 ..7 ..!0 [.19 ”34 ..36 ..’10 ”to '..52 ..72 3 OF GUREB Figure Page 1.0rosaSectimVicwcttthdntillationW611Mcctors..u c c c" LWdAbcorbtimofawmad-aywaumbymm DW...¢..-.ou...o.......2.3.......13 3.mflclntillztm3pmm....s..g..........15 a. We 3pm at we.“ a. Obtained on a acmmmm spec-mm. 11 5c wwmflloccoccccceases-cocccccccfa 6 Mamaavmmsmmwmwmm Fallout...........o..u....a....¢.....20 LWWMMctatimSmnplccmminingwmm moutcccccccoccoccubclccccccccccccczt 8. Gama-m Spoon-m 03' chctcticn Smplcd M Hacks after Fresh fallen-ticsccucccccc-cccccccccicccccoczz 9.6cnmw5pcatnmofthcranontfiadicisctcpccchovingthcmerw mwmtmmpmmmrwmmmdm 1391301).chcocciccoccccccccccccccconn02“ 10. Mental Values for the Caspian and Photopak Gorrcctimc .Sampnngmmmtm. 12.6cmtingi‘quipnmi................... 13.3mIch’occaMEquipnmtsooaa....s.. £6.2295ih95mm1m1mWWWH :7. ca‘373a‘37 mmmnm WSW . 18.1‘3‘Wy8pwm.............. 19. «mam Wrim Wm 032M spam-m . 20.M’°3Wy8pm.............. 2t. Baflfu‘“ Equllihrim mm. W spam . 22.0:t0mm-mr5pm..u.n.u..u 23. 213°6sz “when Mixbm Wy spectrum . 21-h mwmgmffiraghtthc c o o -'.OOI»C‘II-§.’.U..‘ . ,V C . O M. ..26 ..31 ..32 ..33 ”M ”155 ”#6 ”#7 ”as ”he ..50 005' ..53 25. 26. 2'7. 28. 29. 30. 31. 32. 33. 311-. 35. 35. 3?. Ccsnputm‘ Program for Four Component Systen . DailyCa‘oscBetafidxActiirity. c .5 . . . . my m1103.406 and Gamma-n Mr Activity . Daily arr-Q5 and as”? Air Activity. . . . . em Versus 2m- Aotivity (Gross Berta). . . . c‘ 0 Pain Versus Air Activity (Individual Isotopes) . . . Gross Beta M: Activity Versus mm” and Ru‘°3“°5 m Activity 0 O 0 Gross Beta Mr Activity Versus as”? and oem‘w‘ An- Activity. Fain/Mr Activity Versus wind Velocity . . . Rain/Air Activity Versus Rain Depth. . .w . . Rain/Mr Activity Vm‘sua Cloud Height. . . . C Predicted Verena Measured Aulzlain Activities. DEL-13130110” Percentages. . c 3‘. c c b a c O 38.Listo£M.randRamDatA........... D O O O O 0 0 0 iv .55 .58 .60 .61 .62 .63 .a .65 .66 .67 .68 .69 .70 .71 W Th- proscncc of fission product radioactivity has been rcpor'bcd in sitcoms and watcrways. foodstuffs. and mags ”comm. plants. This world uido distribution of radioactivity docs m tapas-st an imam. healthhazczd. butitwrcsultinlongtcminjmytohwmhcalthm income). deposition. Prosoutly. tho cmaphcxio radioactivity M018 arc but a fraction oi‘ tho lml. labeled 'cafs' by tho U. 3. We However. the "safe" level ismsrclyotompomswflardandtcndingtobcndwdbymrthsr understanding of tho macs]. effects of radiation. Also. with expected incmscs in tho us. of radioisotope. in industry. mm. and research institutions; mixing and chemical prccccsing of uranium on; mclsar reactors for power pmductlon and march: clinical processing of spent roommate! formflmofmclcarm: and falloutductoths use oi.‘ nuclear toatihg devices: the presence of fission product radio- activity in our cnvimrmzt will. We. It may possibly increase into the dam levels of concentrations. Evan tho prcssnt “low” low]. of anvizormcutal radiation w present a curious probm. who has tons imam-y possible through ecu-tic effects may be tho most mm of ps'oblcmc to Mun Mons. Radiation is known to In tho camp of mutations. Sons of thou mutations on for tho goodbutthcmjoritymmrttwworsc. Inflicpast, mtmmowcdcnly the mo: survivc axdthuswcdcdoutthcunwamumtstions. However. today at}: tho advanced stats of tho medical. profession. the weaker. un- WWWM‘VIe mummummmmmum majority. tho long tom “toot m In dmlutionszv. For thcsc roams. studios such as that pmsontod in this thesis arc desirable. The idmtification of tho radioactivc matcrisls prooont in the fallout 1:! noocssary hr 3 marinara]. comm of the potential. health hazard of the continuation prosont. m morn difficult and yet important problem concorxmig tho radioactivo pollution of our cnviromsnt is to understand. quantitatiwly. transfer noclmdms of the who mclidcs in the environ- mentalmcdia, inparticiflar. mum-tam mmmnummgaummmmmumdimmdotmrer mm tho stmsphorc to tho rain. Gama swims: 53ch is applied as a possiblc moons of analyzing the transfer merchant's: of in- dividual radiomolidoc. .It is attomptod first to dmlcp smothod forths quantitative analysis of names containing mfimn amounts of gonna-ray mitting radioisotopom sodomy.“ Marian of tho fallout Momma transforfromthcmicsphmtotmrainio studied. Intholshutow.bothmssbctacountardmnascdrtillation spectrompha of air and an miss an analyzed. in amm- carnation is found batman ruin commit-stun of a cortsin radimmclidc and atmo- sphcrio constitution of tho cams mclids 1hr all tho radionuclidcs analyzed in this study. In addition to tho direct air to min activity uhtionship. addi. tionsl pas-motors of important innocuous haw hm invcstigatod. such as wind ”loony. slow height. climtobacal auditions and others. this studyisbasodosdailyavorago samples. observed mm 1962 to July 1963 on tho mctdgan Stats Mir-nit? comm. Also. the opacicc orthorodlmlidosamlysodmlhmodtcthcfwrlonghalfuh new products; Comm“. cssa “37 NOW“. and 2m”. 2m M1957. Gmnflem (13) made a th'ccmtical analysis of the rain scan waging of radioactim particulate matter nun the aimcSphcrc. A two step pmsa m imalvoiin the mm rcr- m «mm of partials: by water-cloud droplets and subsequent dcpcdtisn by rainfall. It was can- cidcred that (a) a certain percentage of particles would be captured by tater-cw drcpltts. and (b) a certain montage of ths droplots would be Subsequently captured by falling rairximps. It was concluded that. as a result of tho collision of falling rain-- crops with particles. particles uith dimtora less than tm‘Mcmns muld be retrieved in only nimb- mncmrta. depending an the amount of rainfall. Also. the pmbabmw was very mu that cater-mom droplots would pick up significant quantities of partial“ with cimnctcrs greater than 0.08 microns. and tho'mcchanism of 6:013th capturo by Wraps would occur in a mm: mm tel the direct captun a: radicactiw particles. Assuming a mean partials dimer 391‘ We mimns, Greenfiold showed thcaroticauythaterpemntcttMt radicactivity is mngodby direct interaction with mining». For all practical purposes. the rem ~ naval is by direct inquingment cf falling mirth-cps with particulate nutter. Itagaki and Roma (11$) intcrprcted the Greenfield analysis to mean that tho prodmdnant transfer mechanism was collisions batman mirrlrcps and radibactivo particles during tho mecca of rahadrcp descent. They mea— sursd tho radioactivity of seven mine at five diffomxt auctions and found that the specific activity amend with altitude. W. at. «1.. (15) mm the mum at tar-90 1a pmpi- taticnrocultdmgmlargoacalsuplmmmctiw stem. my 3 interpreted Greenfield's analysis as mezming that the predommnt deposi- tion mechanism was by cloud-droplet capture and subsequent raincoat. This 1: in apparent. contradiction to the mrk of Itagaki and Room. By mimng three rains thy found evidence of oomlation between cloud ceiling and the concentration of 81590 in the rainwater. The cloud ceiling was interpreted to be a measure of the concentration of the radioactivity _ resulting mm the. evaporation'er the rainirop 1n the unsaturated layer of air war the MN , ‘ Conn: (16) eaqalaine this pheromomn on the basit of certain meteoro- logical hmootheaos: briefly, that precipit‘ion‘that origmatea from air nth lees miaturo eon produce higher concentrations than air with greater hoisting since more air is needed to make the some depth of rainfall. The mmmpfim is mm. that arid regions obtain rain from drier air and that raindrops falling in. arid regions madame more evaporation than in hmid' moo. thus onrlomng the Sr-90 in the ramming liquid water. l-fiyake. at. a3... (17) have proposed an equation for the deposition of radioaotivity in items of the concentration in the air and the amount of pmdpit'a’oiono Their data are Wisely represented by the equation When Mapherio ao‘hifitgr is taken as a constant om an extended period of time. Homer; in MI by mm: (18) large fluctuations in the con-- centrations of radioactive Aduste are observed. Fluctuations 91‘ $11.21* activity may be due to these fluctuations in the oonoentrations of radioactive dust in the air: Norris monoludoo that in the case of armor rains. Groenflold'o model does not apply. No rain was extensive to the demo that tho penning. of particles removed mm a.~ vertical cylinler was equal to the percentage of Mules W from the entire radio- active cloud. The speoii‘lo activity of rain did not appear to be related to either cloud height or rain intensity. This tends to support Gmfiold's proposition that the fraction scavenged w be oonaidered to be indepament of rainfall intensity. Norrie proposes a relationship, between specific min activity and the specific activity of air at. the time of the rain. oftho rm (33:22: CA . M the WWW a: mohigan. Dangle (19). has undertaken to model the rain process in Mt more detail, accounting for the size spectra er cloud droplets. or rename. and of mm particle: in integrating the Wmn and :1an We”: layer by me:- though a Wool atmsphm. unfortunately. the ”ligation of data is not 811111de at this time to make oompnhm'vo omiyses. Dingle claims hisdflflholdsamotdoalofprmisomdplmstomm further details and mm: in the m M. Kruger save that in general. the fallout radioactivity oonoontration in precipitation which reaches the ground is 111:on to be deponionh upon the paramtoro noted below. (15) 1. The height of the precipitation generating level. 2. The precipitation mutton and growth mohanime in the aloud. 3. The mum: 0d radioactivity mum in the air masses participating in the precipitation moose. V 5. The previous precipitation madame of the air at the generating lml. 6. The descent modem. or the predpitation 15mm the cloud. in which precipitation originates, to the wand the data out Kruger (is). show that in each ease the grown 1m]. 31590 concentration follows cleanly the trends in the height or the cloud ceiling. A poorer correlation is noted for the average precipitation rate . and very little comlation is noted for the influence of previous prea- cipitation more. at the generating level. Variations are seen in the individual showers. The largest Bra-90 concentrations are in the rain which falls after the cloud has acMevcd its greatest vertical dmlcmnt. Showers which occur mm fmm frontal atom systems cm lover concen- trationsbut stillvith venetian: dmtothe mm height atthe predpditation generating level. ' In all the works performed to date: San-90 or gross beta analyses are used. With the vast mm of debris deposited in the atmosphere by 'nucleartcsts. motherisotopcsmpnscnt. Alscbecanse cfnatural decay the relative amounts are constantly changing. It is thus possible thatasnflycfthcixflividuaiieotopcswfllbemremealingthanthe was me analyses. 08.111113 scintillation spectrmtry offers a possible means of analyzing the transfer alcoholism of air activity to the rain. Beginning with the work of Greenfield. s sexier of authors have pm pared plausible accruing mother-sec on the transport of the radicnuclides in air to rain. However. nearly all authors have restricted their view.- point to one basic parameter: Itegaki, with transfer via direct collisions between reimnops and radioactive particles: Kruger, with chm-droplet capture and subscqmnh raincut; Me. with the correction for the wind velocity- _ In mmining Greenfield's work. the author feels that the emphasis is placed on the direct collision appmoh as furtheni by Itagaki and Koemma. Itagaki and Kcemma's proof is dependent upon the observation that. the specific radioactivity of rain was icon! to decrease with altitude. How.- e'vcr. as described by Collins. the observation does mt automatically impr such a generalization. Raindrops may begin their descent with an initial common. The change in concentration ehsemd by Itegski and Koemzma maybednetcthemmmtormpcraticnaraindmpwerimdmdngits fall. Thus. the specific activity or the rain would decrease with in. cream sampling altitude. I: the direct. collision of raindrops with radioactive particles is an important Wm. the spedfic activity ctreinsrmuldbedepementupcnthe specific activitycttheeires WetthetMecrthel-ain. mammmmwupmm later which tends to W this proposition. Itagaki. Kama. and Kruger all observed an influence of cloud height upon the final specific rain activity . Their observations are unfortunately only qualitative . Although their resume are och used for proving opposite viewpoints. it is hrrportarrt to establish or disprove aw relationship. Further study on this mechardsm is presented in this report. It nger and Collins are correct. e eermlstion batsmen specific rain actiflty and specific hmrlidity 5mm exist. is judge such e son's- lation it would be necessary to know the specific activity of the rain at the cased height. Mth only ground level observations available. this mild be impossible. However. the relative hlmidity idea may be of assistm in qualitatirely whining extme points round in the angler}.- mental s‘tudics. ' ' milerthesssmptibnthatthebasde mhaflmfltransportisvia dimt collisions. Norris prcpoeed a actuation for diifereneee in gmund lwsluimspeeds. However. themmbercfreimm small. MoreSlnPor-r tantly. the velocities used were daily averages measured fire miles distant fans the rail! smapling location. It is quite probable that air turbulence increases the possibility of e ranch-op a pal-timetafmatter collision andthatwilflvalocitiesmsybeussdasanindicatienefthis effect. flow- ever. the data and meats presented by mm: were insufficient and 3. else:- leek at us; mechanisms justified. The amount of proclamation is listed by myske as an impsrtant pm. Altlwugh this mid not be ac asserdlm to Gmeni‘ield, its effect may actually met. For this reams. the amount of pnsipitation and its effect upon the specific activity or rain water is seam and will be discussed later. ‘ I . * m'previeue experiences! the air at the generating level was pre- amtedbyxrugsrasapeesiblyimpex‘tantparameter. itpresemt. itis only possible to look at us; emu: qualitatively. W. it my be of some impertame and theretere its effect will. be detemined. In the process of evaluating the possible parameters. both gross beta and mvidual isotope analyses will be used. Gross beta. comts are made 6: all beta emitting isotopes. mum 1mm rm bo more re. veaJng since the mount and propérhions a: each radioisotOpo changes because of the addition of new radioactive debris and natural decay of the old. The! gamma scintillatian spectrometer is used to analyze the spectra otgmmtung radimmclides. Thoma annalnthnaedfortho detaotion 9! radiation in a gain: Miniman spectrum“: is 3 Wm activated sodimn iodide cmstal. In being absorbed in such a crystal. gmphotonstransfaralloraportionoffiheir awtoarbital aleabmm of the mlmles managing the metal. These mm lose their mom by exciting and Wing the minerals: mung tha crystal. The wary received by the mleoules is. in turn. am of! in the form of pulses at light, .part of which are 00.1le On the photomflmdo or a multiplier tube which is optically aouplod tn the metal. The can» binatian or crystal. phmmupnar tube. and ampnmr act as a scin- tillation cantor. (5) A diagrmn at. the datum! and aomrpaming phato— mnltipliar tube is sham in Figure 1. WWI: is absorbed in the metal by £11m. principle processes: (a) Human“ (b) Compton flattening. and (0) Pair production. These moses m scheaucalk diam in Flam-e 2. Absorption of gm photons in the metal by the photoahahrio pm. Mssmfltsmwmesossmifllyflpflmtingmmafm mam pMans. In th. pm: effect. mat. of the W at the gm 18' am to an m:- shdll atomic alsotmmhiah W m the pm when. This atomic Wu mm the pawn: atom with an mhnmmmrwcfthegamaphotm (lassbyanamtmtoqual to the hitting W at the 315011110 shell mm which it escaped). The .pmwnwgummwmmncalpulsobytm adnmntian «mm. pmmnu- m. m parent atom. being lam-~11: an mm 10 REMOVABLE PL UG HANDLE CO UNTERBALANCED 212. / CRYSTAL SCINTiLLATION 25.9612 FBURE¥I CROSS-SECTION VIEW OF THE SCINTILATION wELL DETECTOR 12 state. soon gives off the moining emery when an electron falls into the shell from which the photo-electron come. In Conmton scattering. some of the energy of the incident gamma photon is transfered to enozbital electron, the remainier of the energy being carried away by the scattered photon. The scattered photon may or may not be further absowed in the crystal. Again. because of the relatively long resolving time of the detection oquipnent. any series of Camber: Mutations follms'ed by a final photoelectric capture within the crystal v1.11 produce the signal proportional to the anew of the incident photon. The photmvmltiplier tube can not distinguish between two separate light flashoe if they are Simultaneous. 3rd in the“ in. stances a current pulse representing their sum results. (1) Thus. Compton scattering ecmasfied by phytoelectrio absoxiation of the scattered photon may yield a pulse representing the energy of the original game mdiatian. In general, however; absorptions involving Compton scattering yield a spectral}: of pulses with a madman emery less than the emery of the incident 33mm photon. Inpairproduetion, ameitmamanohetmmmatd.‘ This creation mm: 1.022 New my. the remixing at the inddant gamna plntonappearlngeekimtiaomrwehandbetmenthepeadtmnufithe .-' elem. The poeitmamtho Whacthdrkinetio Wmugh. com with molecules composing the crystal. After it is brought to rest. thopesitmnnmnhnateewithaneerbyelwtmziflng meetom photons. not: possessing 0.511%" m. It the M amihilation photons ”capotmmam. mmflngpfilnmflaom the emgyotthe Wmmmiwzzm. Ifhthmabaexbodvdthintho a(0'1PMO'I’OEL.E¢'I’RO N) I / / INCIDENT PHOTON CATO“ PHOTOE LECTRIC EFFFCT ATONIIC , ’CONPTON ELECTRON ://\0 ELECTRON COMPTON CONPTON SCATTEREO PHOTON EFFECT 'MO ,/’ POSITRON ‘\\ ELECTRON \\ PAIR PRODUCTION .\ o .5IMOV\ Y \/_ o ORBITAL ELECTRON FIGURE - 2 PROCESSES OF ABSORPTION OF GAMMA RADIATION BY THE CRYSTAL DETECTOR 1h motel. flmpuleowillropnuntthowgyotthoinddmtgmphotomw) Through use of suitable electronic oirmfite and discriminators. it is poedbloto oomrtomypflueuthinamvenonorgymngo. Suehan instrmmtel sot-up constitutes 3 gm scintillation spectrometer. Its baeio oompormrta are shown schematically in Figure 3. The Olootxical 31ml output of the photomzltiplier tube is directly proportioml to tho mnt which caused the scintillation. Bovevor. mrtlnr anplinoation is meow because the pulse is of the order of minivans. and the pulses are in the order or volts when used for the munting prams. (9). is described here. the spectnm is a curve showing themnbeofpuloeo Orwam onerw asai‘unotionofenerg. mammal- yzer contains two diocxiMnatoz-e. Unless the voltage pulse is higher than the setting on the lower discriminator. the pulse is rejected. The second discrhuinator is set to reject voltage pileee above its setting. The circuits are arranged so that the second disorhflnator setting is a voltage slightly higher than the first discriminator setting. The second setting is rat-ems: to as the ”Charmel width". The output of the pulse analyzer is oomectm to a scalar to record the mortar of when observed in a specified time. To calibrate the curve in terms or raw eorresponding to am given pulse height setting. a redioaetivo sample with a lawn anew epeotrum is used. Ost- 137 flth its angle peak at 0.661 Nev is a very oomon source material. The Na «zit Spectrm is an excellent illustration of the priviously mentioned prindplee. A study of the Ha-Zh epoctnm reveals that there are peaks at W W Of “ut- 0051. $002. i073. 2023.. 8:11 2.75 M". awkmiomhomam ZO_._.<..:__._.Z_om (2.240 m . mmDOE vmmoZzEEUma "NEE—.524 mdwzfi 4m o j] 52.55% _ _ \ _ momnom >4Qn5m mo<._.n_0> 10.x 16. Thefsotthatthorempesksattheseenergiudoeemtneoesssulyirdioste that “3“ emits game photons with all. these Woo. It does indicate that the sdnfillstisn mpment observed a considerable umber of events having these various Wes; To explain the various peeks it is mpmhmsh Ra-Zhdoes mt mphomhavmgmuo: 1.36 and 2.75 Move. The peaks at these margin indisste the likelihood that sonsiderable numbers of M game-rays are completely absorbed in s Compton phtoelectrio series of events. The 0.51 Mev peak is produced asth otpairproduotionend subsequent amdhilstism butwhere one of the photons escapes the orystsl. The 1502 Nov peak scours nth gig/he woman of both 0.51 Kev photons. The 1.73 MW pus is the kinetic wary of the pair production from s 2.75 Mev gems-my (2.75 «1.02 - 1.73). The 2:7.23 M'ev peak is evidently the observation of s 0.51 event and a 1.73 * event where both events assured in less than the resolution time of the equipment and thus were observed as s singls event of my. 2.23 Mev. This is called a m peak. (9) ’ The broadness of the peaks is attributed to a certain extent to Wenoestteringwhemonlyspartoftheensryms givenuptethe crystal while the reminder escaped and was not observed. Because of the Wm of its operation. the gm sdutfllafion spectmeter affords an excellent means for the study of the basis processes by such gamma radiation interacts with matter; (1) More importantly. the spectnanoter makes possible on analysis winch does not denand distruo. tionortho maple: Also. ornament ofthepeak ores ( etlesst tor ample spectra) gives a direct imtioation of the isotope sonoentmtion. The sizing of s ma of isotopes greatly oomliestes the analysis and unhediswsaed htsrintrds report. —._.. a--__—o.-———.A—- --.—.. - - RELATIVE GAMMA ACTIVITY, cpM lll'lTl I I 3 N g, 01 O ‘- N N U1 I fl rnl 3 ." I I IIIIIII l I : l l l J O 20 4O 6O 80 IOO PULSE HEIGHT (VOLTS) FIGURE-4 GAMMA SPECTRUM OF Na-24 coum’me an: WINDOW —-n~— || GATE ;; GATE II I! new ,, SCATTERING“ . u COMPTON 0 IO 20 so 40 50 'l 60 PHOTOPEAK \\\\\\\V\\\\\\\m\ \\\\\\§ V O O O 0 O PULSE HEIGHT (vane) FIGURE' 5 GAMMA- RAY SPECTROGRAPH We resulting from the decay of maioiatopes are emitted in Wmmmmmcnlymghtetminm with m ewe more. These properties have panned qmutitstive spectrometric analysis of certain We e: radioisotope: in Bengals: oftiseueembone WWW. invasions Mutts-isle. and else is lame». (5.6) m sinist- Mined: or analysis it is possible to quantitatively m radioisotopee roaming from fallout oat-other sacrum. Thepmblenotneuuringrsdioutintalloutis summed bythefestthetthemotintopesiemrmynetnstedtc I rather donut. compositions. mama-monstrous: 'msh tallest“ ndiodootopes. wanton ngehtiomthreeto burden sites-fission (usflgure 6) istherosult otaoomploxmcommsM‘rt lived radioisotopse. Aquam. itative game-m We: mm of the individual SM mtmmmmupuinmhendxtmwfldbemdirfloult. About on week after fission. new or the short lived radioisotope handmade sndslessccmplugm-rcyspectmiscbeened.(sse Figure?) morethnstsmurmkdessypsricd, the elm-blind radioisotope have decayed is insignificant concentrations and the gums- ray spectrum possesses five characteristic phctopeaks (see Figure 8). due to com. con-m. m‘°3"°5. um”. and Baum. rm this time mmimsmamodbmnddemumit is possibleto mflmwith assemble seem-sq mathegarmna-rayspectrmorm V owls. ammuwmmmgammtrmummmmte 19 COUNTS PER MINUTE‘ PER 0.03l MOI! CHANNEL 0 Te I32 / //R0Ios 'I32 / . so I40 Bc-Ls W— A 17'1“, I 3 4O 50 6O CHANNEL NUMBER FIGURE- 6 GAMMA-RAY OF A VEGETATION ' SAMPLE CONTAINING 3-4 DAY- OLD FALLOUT 23 asinNevada.thcreisecontimslslowfallcutofradiciootcpesmm atmic detonation at more wan/to locations on the globe. The material from these tests consists largely of the longer 11m isotopes: 63311137 . 091M. Ce‘m. 311103,"!!nm6. and ZrNb95; and does not usually contain sigxiilcant amunts or sm‘m or 1131. ('7) The general method employed for measuring the concentrations of the musiootoposis graphicallyimstrctedinfimeh. Thocounting rate at the Baum protepeak is direct): pmpcrtionsl to the mum. of this isotope present. The test counting saw at the new” photo- poak requires a correction for the contrlh‘xtbn iron Edema as well as for some of the other isotopes. Similar corrections are required for the maidngiootopes. After these “Compton Corrections" have been made. the not ccmrting rate of each characteristic photOpeak is proportional to the mum at imp. present. A discussion or the specific conditions for making the game-ray spectrograph and the methods used in calibrating the equipnont are Unified in the mammal section. rho graphical method is not sufficient since it produces many additional errors. Another 3.1mm methOd might be to algebraically handle the 'Compton Motions.“ InacasewhcreedghtisotOpesmtcbeneasuMMmsgm-w spectnnn and each Offers 3 contribution t0 the counting rate. the calculation o: the net phOtOpcak coming sates or ths'individual has. tapes rcqiflres tho sOlutiOn of eight eimltsneoue equations 1°: the fight We i amoral solution for the cyst-m m be calculated as follows: COUNTS PER MINUTE PER 0.03l Mcv CHANNEL IOO — I4l-l44 CO IISI / l03-l06 Ru 95 I40 ’ZrNb Bch l l 1 20 3O 4O CHANNEL NUMBER FIGURE-'7 GAMMA-RAY SPECTRUM OF A VEGETATION SAMPLE CONTAINING WEEK-OLD FALLOUT 25 Lee A,B,¢,D.E.I.G, and a reta- to tho activaty in micro micro curios for ouch of tho tight radioisotope: proaom. respoctivoly. P1"1 I111 rotor to tho ratio of the count rate in channel ”1" with the total activity of isotope “1", mg. PM =- Count rat. in channel one as caused by ieotopo A Activity (one) of isotope A Thomtoro eight simultaneous equations may be written and their aolutione yielding A,B,C,D,E.F.G,and H. Lot K1. K2, K3, K4, K5, K6. K7. and K8 reproaont the total count in channolo 1.2.3.b.5.6,7,8 rcepocttivoly. 'I‘haz‘otoroa K11" P18A+P1bB+P1¢C+P1dDiP103+P11F+P13G+P1hH XZ'PZEA +P2hB+PZOC+P2dD+P203+P2fF+PZgG+P2hB K3” W1+P3b3+P3°G+P3dD*P303+P3!F+PBEG+P3hH Klu- Noe+m8+moc+mb+mn+mfr+mgo+fimn x5:- Psai+rsb3+pjec+MD+P503+P5£F+p5go+p5hn x6:- PoaA+P6bB+P6ec+P6dn+P6ex+Pérr+P6gG+P6hH l7. Wai+m8+floo+mn+nofl+fitf+P7gG+P7hH 18!- P83A+P8bB+P8oC+P8dO+P8¢l+PBtF+PBgG+P8h3 mammotPunuetbocbtaimdupmtam. Fortbospcotroe graph as um for that-port. tho Value to! P13 am given in Figure 10. Sincoalltbommumaayudtorthicnportmtainodwmur www.mmommmaimpmidbyudngmlytm mltanmoqum. :1:- .5559A + 359$ + $561! + .086th .Rfi.0083A+-.26h60+.3fl31+.02503 :6.- .008“ + .fi69b+.66&sr+.zih93 W'.M+.12750+.8703P*9W For can in canputation. a Fortran columnar program was used in solving those equationu. mo program for both eight and tour cmponmt We is am in the appendix. FIGURE ‘0 WWW VALUE FOR THE COW! AND HiOTOPEAK commons Itotopo P1 r2 P3 In P5 P6 PI P8 a cam .55589 .oflm .00916 .oosso .007» .008» .00596 .0055!) B sen-“M .36270 .ormo .0321: .0275: .0255: .03050 .0203 .01872 a 1m .16891 .1521 .69832 .oms-z .03036 .02119 0.0000 0.0000 12 mm .115“ .mm .ohoza .25800 .1’4063 .01370 .0107: .00881 R we“ .25979 .192»: M913 .26‘69 .02154 .01h68 .0127: .01096 r we” $5610 .58592 .uzsav .3112? .1373! we: .87030 .018st 9 seem .mse .2036b .2133? .35052 .20153 .mos .16515 .07982 a case”? .08639 .09369 .0590? .0250? .omm .zmaa .00018 .00032 LiBOIUe T mmmmm on MID - ~ Folloum are descriptions of the air sampling, rain sampling. and counting arrangsnmte and procedures. The apparatus is shown in Figm‘ce 11, 12. and 1,3. We Two techniques of air sampling were unplflyed. One method was used for gross beta Wee uhilc amther for the W spoon-metric anajyeee. Forthegroeebetaonalyeie. aWemnm-tywbiem ofadr were sampled every twmtynfouv hours through a mnipore filter. This small volume results in a slightly reduced reliability due to cmmting statistics when. empared to the ”stormed” high volume fibrous filter method. The fibrous filter introduces an error as the result of parti- mfla’co matter which pmctratce and in stored within the filter matrix. i’hese particles are nevee counted who: the gross beta method at analysis is used, and according to Cotton (10)t1d.s ' tide'effcct camot be accurately compensated by calculations. " {the P3131130?! filter has the characteristic erratainingontboeurfacemparticlcewhicharclargerthauthe specified pore size. men-crotch.- there in negligible absorption of ’ radioactivity by the filter matrix. Air samples for beta counting were tale: on a twenty-forn- hour basis at a flow rate or 25 libero perminutc. meme rate was then corrected for pressure drop. into filters were mounted and stored in a deesicator until counted. for gamma-ray eointflletim ommting a large counted-ate is necessary. For this reason a larger volume of air nae used than that. produced by the Hilliporc filter system. Instead a. model (MS-It Atcmio Products Corp.) 28 high volume air sempler with a (one 2133) felt filter was used. , Air samples for gem co‘mting were taken on a totality-four hour basis at a flow rate of 35 cubic foot per nflznzte. The filters were then placed in one ounce bottles for commuting. Under the asmmption that a Immoledge of the distribution of radio- activity in rain would be ramming, a. collection basin was eitneted on the roof of the mgineoring Building. the basin one designed of 16 gauge sheet metal with an area of 36 square feet. Rain samples were 1151mm about thirty liters in values. one liter of the rain sample was evaporated emd its residue placed on a oomting pinnchet for beta ommting. The procedure wed was in all essentials the same as that described by Setter. Hagoe. and Straub. (1‘!) Toolmiquee for preparing radioactive emupleo on planchete is described by the finoloar Chicago Corporation. (12) The retaining rain was mad for gamma oomting. mie large volume of rain we evaporated in shallow pane, one meter square and heated by Si: 250 watt infra-red heating 1.8311339. ‘Ihe residue was then washed into a mall glass bottle for emmting. enema All bate cmmmng wan performed with a. gas-flow preportional cmmter with a 2.5 minivan sensitivity. A blanket (:01th efficiency of flit‘y percent was named for all samples. Ineffitvaomtmasemedsothat that-emits couldbeoon- pared. at the same order of magnitude. with other data. If "absolute Women rates " were needed, eeperate efficiencies would have to be determined for each sample. However, fifty percent closely amend.- 29 rmtes the efi oimc'y of gas flow counters or this type as well as aga‘eoing with aizpezinmtal values for hidividual isotOpes. me £011me procedure was used. 1. A background coma’c. of 500 counts was taken before each. 001111th 86331011. 1315.3 was mlbtracted from the total coating rate for each sample. 2. the thousand counts were taken on each ammo 14-7 days tor sawing. Two or throe additioml counts were taken at 1+4? day batman. 3. The sample ooxmting rat-es Hero extrapolated back to the tins of 53221313 collootion. The axtmpolated ommting rates were converted to micro micro curios per liter according to: e in A I-hmleau‘ Ohicago ems channel War with a 2m ('11) deteo'tor was used for the gmmxaway Spectrmetria measuraaents. A plwtogmph of the analyzer. detoctor, associgted lead. .shield, and sealer is sham in Fig-giro 12.. The general Operations of the analyzer is included in the fastmtion normal. m detaotor is a three inch by times inch 1m ('11) well crystal (flax-shat: menial Gmpamr) mounted on a Dtfiizmt rmlti. plior phototube. The sample oontainar, a one ounce glass bottle, is placed directly within the mom moose. A high voltage of about 2000 volts was: used on the multiplier phototube and was adjusted to center the 0.661 Hexr as"? photome with a. alumni width of 0.060 New... Known mtg, or each muted isotope, were ommted with the Spectmneter so as to deteming the counting affidmcy of: each. The rosulto of this analysis are shown in Figxn‘e 5. The procedure used 30 was essentially the same as used for beta. counting. mm 1000 counts were taken in each of the Bixtem .060 Mm.” channels. A180. the gm counting was performed only once. this bong filmeflata‘iy after each sampling period ended. 3! 32 33 5—- _—————_—. _ .» fii... 7—.--H_ _ gym—«h--- _.A w“ . mgoaainSmpleaforOMAnaJms The efficiency of 3.1V partimalar smupler. eSpocisJJy one used to detect radioactive matter, is ultimately determined by the type of filter material used. The detection of high charge, law penetration ytrticulate matter such as alpha particles requires the use of a tight weave, fine grads filter while beta particles and germs radiation are best counted from more porous filters pcmitting greater air flow. Despite the availability of more efficient air sampling filters. felt filters were used for air sampling for gamma counting. Because of its cacpcrativehr low resistance to flow. it was selected over the cellulose papers. However. for a mearfingful analysis to coast, the efficiency of the filtering system mt be Imam. this chapter describes work performed to dctcminc the collection Efficiency of 'I'FA 2352153 felt filters. The AA Pfilhpcre filter was chosen as the standard of measurement because of its near perfect efficiency; However, allomncos were necessary since the bullpen filter operates in the velocity range of 200 rpm wlflla' the felt filters in thawv’olocity range of £300 fpn. A. Boots (10) used Cobalt Oxide fume particles of size 0.01 to 6.02 . microns at the rate of ten liters per mimte. With this he dmmstmtcd that one particle in 500,000 passed the filter mmbrane. Merrill Esa'fout (11) measured the officimcy o! the IflJJiporc filter as 100 percent dam to 0.1 micrm. firms for partimflato mattm‘ greatsr than OJ micron. one may use I'Iilliporo filters with confidence that its efficiency is $00 pcrcmt. However. for atmospheric fission products, the particle size distribution 35 smears to contain a percentage of matter which is moller than the 0.1 micron lbzit. filese particles may not be efficiently trapped by the I-fillipore filter matting Crude, qualitative meammeuts of these parti. cles show that their effect is neglfilfible. This is due, probably since the ' fine particles have ins7 ficieat inertia to pmetrate the falling rail“:- drop, and are instead merely pushed aside. ”fimoughout this report the effect of these fine .sxfmicron particles is assumed neflig'iblc. Further and more emet work will be neeesswy to completely establish the true extent of the subsicron particle's Mumce. At erg rate, when com. pared to the I-fillipore filter's high efficienqr; that detemined for the felt filters should be meemimmfl. O": - merits“ it? us 0 The felt filter was placed in an Atomic Products Corporation model ELM high volme 8111131631“ and run at 3 5 cfm. in AA- I=flllipore filter W118 placed in a filter holder, witch was then placed directly in the high volume sampler' s ordnaust sud mm at 2 511m. Simfltaneoashr, another rallilmre filtering systeu was placed rec eiving fresh air frcm outside the mgiueering Building. Each filter was then run for tz-renty-four hours. The two I-Iillipore filters were mounted and beta counted with a gas flow proportional counter. Doria-m1 g the filter efficiency as : For the mug aent used here. this efficiency was n = 87.675. Using the method of aimlysis as described in chapter five it. ms possibio to quantitatively meamxro radioisotm resulting rm mutant in both air and rain samples. The laboratory setup meets all criteria of mmpucity and adaptability. me data produced is both quantitatively and statistically reliable» __ when young fission products are mooted {such as in Ms 6), quantitative annoys“ booms quite mics-om since approadmatol: sight 11:31am mt. Baum. amen amines arc mods at wig-dived radioamya fallout. only four mm are needed to deems tho aamplo. mu: only in: mama” the resulting simultaneous equations may be solved directly using detmmmts. This results in Native]: m Wm: M m the tour Wm activitioo after 41 1133111111311 of «madam. However, for we W. calculations would approach the impossible and oonputor prom pron to be Mimiblu. In dflieu‘ case. tho umputor serves meantimoandmuadmgimtthisrw. Ibohookthoaacuraayofflxflmethod. Wmmtaofaovm isotopes 17mm mo amplom the: treats-clan anmlmonn and thoactivity or each isotope calculated. Tho rosultdng mm am all within or near ten percent which is quite good Mulder—lag the difficuty of preparing seawater samples. min method is mom than adequate for the quantitative Wis of mixtma calming whim mm of gammy matting radioisotopes. 36 37 Activity Activi Isowpe (calculatod) (actual Error ($0 com 214,791+ 22,600 9.? Gen-m 18.010 18.200 4.0 1131 2.534 2.300 10.2 2111121905 , 9.989 10.120 4.3 ZrNb95 2mm 25,200 4.3 Baum 9.090 9.760 .5.6 Gena”? 27.100 28,600 -5.3 Itagaid, tom, and We each claim an Monaco of cloud height. upon tho final Specific rain activity. Itagald. and Koemma measured the radioactivity of mm min: at five different elevations and. found that the specific activity deorosood with altitudo. On the other hand, . the author has undo“ ground level obsmations: the spodfio antivitjsr~ of which is plotted versus cloud height. (mm. 35) 1121: data show no relationship between the specialities rain activity and the cloud height. Tins appamt contradiction may be winked by archer of two possible causes; first. the author 1180:! only aloud cooling measuremmm, and since” this makes no allmnoo for the cloud Mimosa,‘ the possible error in moments may cause the Apparmt discrepmoy. Secondly. as mqalainod by was. at. 91.; the distanoo a mindmp tans may b. 1mm to be a measure of tho oonosntratim of Monetiviw resulting tron rain- drop evaporation through tho @321th layer of air nom- tho grow-1d. Fm precise cloud height ammonia or. needed to clear this point. Norris' interpretation mggosts that. tor Sumner precipitatim, an equation of the form OR :- Km + kf‘cA mam. be more descriptive. In this equation . Km is a constant for the spocfiio suscepheric activit , and V is the wind Speed, CR and CA are reapootively the specific: rain and air activities. and. k and n are adrhtional constemts. Figure 33 00:1st mat some relationship exists bets-roan rain activity and wind Speed. Ibr-xevm', the relationship is linear in natwto. In addition. the specific activity of rain did not appear to be related to the W of rainfall. This tends to support Greenfield’s proposition that the fraction scavenged may be considered to be indopsidmt of rowan intmwity. V Figures 29 and 30 show a direct correlation Esteem air activity and rain activity. The gross bots analysis shows two curves, one for early spwxg rains and anothsr for tho armor rains. The curtarwoo is probably due to the additional upper atmospheric Wanna; as typified ‘ ‘ during the early spring monthS. Since only Spring rains were Wed for the individual isotoyes, may do not eafiiiblt the two curve characteristic, see Figures 29 and 30. Howsvar. in each moo the relationship between air and rain activity appears to be linear. This it appears that. rain activity depends basically upon two parmetors, air activity and wind speed. Using the data of figures 29 and 30, it appears this relationship is at the torn ‘Rain/Am ' (G1 + ‘32”- If metalocityismmodinmiluperhour. this equatimbeomos ARIAA '- 190 + 15.1w. Unfortunately. the only wind speeds available were averagedaflyvaluast thomewind speedmayvary grostlyuith time. More closely measured velocities may show a better correlation 39 Using the average daily values, a bettm- fit to the data. is found if the equation is used as 133/31 2 321; + 10v (see Figure 36). sing the field stucbr as described above, it is possible to hypo- thesize about the ~ ansi‘er mechanim of fallout radionuclidos flora the atmosphere to the rain. Since the amount of radioactivity captured by the rain was found to be proportional to the mom’s of radioactive particles preseated to the falling raindrop. it is 5113* ”5.31316 to assume tint the mechanism of wanszaort is basically thromgh direct collision. However. a. certain percentage of particles may be captured by mter cloud droplets. It does appear that this percentage is mall. A more complete Wants-.1 prom will be necessary to establish the acts-a amount. Also. the usage of daily averages has reduced the some}; of the EtUdy. It is recommended that averages of mailer time duration be used in any firther studies. me rollmdng general conclusions are drawn from this atmiy. (1) The Sammy Spectrme’crio systen of anaflysia and the laboratory setup meets an criteria of simplicity and are both quantitatively useful and statistically reliable. (2) The relauonship batman rain activity and air activity at the time ofminappearsmsmablywlldescribdbyflr'33hc‘. ' (3) son. mum betwem rain ammo and. was speed at the one ofmdnappeas-I mm. W. mmmmuuaom seam madam. Possibly. wind wane.“ amen! during the mm would be more descriptive. its data is described. quite; accurately. by the relatioMp, Gr :- 33b Ca + 10 V. (It) no specific activity of rain did not. appear to b: ralatd to either cloud height or rain intensity. (5) In: mm of fallout mammda transfer tron: the amosphm taminilbasioanytmghdirmwmsimsbmtmgraindmps and the mom” particulate matter. ‘ (6) may averages of air activity. rain activity. wind W. cloud taught. mflfiinintmitymoftoomaunodmetim. Further studies should use $313116? time average: of the above W. (7) WWW of Wm radioactive particle are presmt in the amaphm. However. filsyaromtacavmgadbythorainaxflmsythersforu be neglected in consida‘atima an the mechanisms of radionuclide transfer. R. E. Comm, Instrmnental Methods of Gama—ray Spectmnetry, Anal. Chm. 28. 1&7‘539 “956). . P. 1”. Wm, Argonne National Laboratory. L. B. Inckhart, Jr. R. A. Bans. R. L. Peterson. and A. W, Saunders, 31%. m 130. $61. (1959). , '1‘. Wm B. vadmg. A. mnegraven, and 3. Small. W185. 805. (19605. G. L. Bromell and W. H. Sweet. Smflng of Positron-Mum IsotOpes in Diagnosis of Interorazfial and other lesions . Proceedings of the Intemtional Conference on the Peaceful Usae of Atomic Energy. Geneva, 1955, 2/181. Velma 10. page 249. United muons, New York (1956). R. W. Patina and J. D. McComack, Ihe Determination of 01164 in Reactor Effluent Water by Coincidmce Gomting of the Positron Atmflfiletion Radiatim, Iii-M5636, (12 Gotcha, 1956). 1. Kaplan, "finale” mica, " Addison wesley Publishing Cmnpany, , Cambridge he, Mass. pages ans-.349. (1955). '9. 10. 11. '13. 1.5 9 '3. A. Reynoldsk'imalg‘rtlcal Radioohenietryz' Record of Chanical Pro- , Number 2, pages 99-119. 1955). B. Xahn and W. s. 1am, “Use of a Scintillation Spectrane‘bm' in fidégcihmioal finely sis.“ unclean » cs, Volume III, Number 11, pages 61.62, 9 ¢ R. A. Gotten, Research Director. Ellipore Filter Comoration, in a letter to the author. 15 October 1962. L. R. Setter, G. R. Hagee. and C. P. Streub, ”Analysis of Radio» activity 1:: Surface Waters an Practical Laboratm Methods,“ Marleen Society for Testing Material: mnetin Emba- 227, January 1958. Melee:- Gdoago Comparation, *Hew to Prepare Radioactive Samples for counting en Plandxetefl Techfical Bulletin Weber 7 and 7B. 1960. S. M. Greenfield, ”Rain Scamewlg Of Radioactive Partimflate butter from the Ahmaphere,” * I»? .. 11+: 1957. P. Krugw, L. Salter, and 0. Easier, ”Meteorological Influmees of Sta-90 Fallout Concmtmtion in Precipitation . ” WW gross, Velma .. War. “1962. 1.4. I. Itagald. and 3.. Emma. “Altitude metribution of Fallout Gen. tained in Ram or m..' 391mm]. 01‘ Geophyaical Rees-rah, 67310, 1962. 41 11-2. 16. w. R. Collins, "rimmed and Predicted Contributions Fm Fallout to Want}. Radiation Levels,” TED-7532, Novenber 1961. 17. I. lfiymce. X. Hanmaohi. I. Katmu'agi, and T. Kamzm, "Radioactive Fallout in Japan and Its Bearing on Meteorological Commons, " ‘ a 432‘ 7 Eat r f 3.; 33607130 XI. ‘. ‘9500 18. w. E. Norris, "en Investigation of Relationships Beteem Meteorology and Radioactivity Levels 111 Rain. " Unpublished masters Thesis. mobigan State University. East Lmsing, 1963. i9. A. Dingle. ”Run Scaveugmg Studies,” QED-7632, Novauber, 196.1. 4" LRAY SPECTRA OF ' V W its way Spectra of saw. Cam-”‘1‘. 113‘, Rum. mm105, we” and Memo are presented as Fig'tn‘ea 16 thrwgh 23. 43 I4l-l44 0 c 'F _ H 15225.8 30.0 _ _ -_ _ cum 9.52.! cum mhzaoo 30 4O 5 CHANNEL NUMBER 20 IO F FIGURE- 8 CHANNEL ‘0’ 3 O O 8 q coum's PER MINUTE PER 0.03: Mev on 8: § ' T (“Ml-I‘M / F r R IO3-I06 95 n\ /ZrNb l3! 1 I ' l IO 20 3- 4. " .. :- CHANNEL NUMBER FIGURE - 9 GAMMA‘RAY SPECTRUM OF THE FALLOUT RADIOISOTOPES SHOWING THE ENERGY INCREMENT AND COMPTON CORRECTION FOR THE MEASUREMENT OF EACH ISOTOPE COUNTS PER MINUTE PER BO KW CHANNEL g, 'm in i. ’on 'a 53%» AQU “H __ __h ‘11— IB 0 42 54 66 78 90 CHANNEL VOLTAGE. o-I Nov FIGURE- I6 5 E UILIB TRIUM MIXTURE -RAY TIUM I? US SOLU , luuc r- 95 COUNTS PER MINUTE PER 60 Kev CHANNEL 0.3 0.2 .. O.I {TH—1* —L l J J 6 l8 304254667890 CHANNEL VOLTAGE FIGURE- l7 CS‘I37 GAMMA-RAY SPECTRUM loz. BOTTLE AQUEOUS SOLUTION luuc. 0.4 03‘ 0.2 4 PER MINUTE PER 60 Kev CHANNEL OJ .4 o T m... 6 IS 30 42 54 66 CHANNEL VO LTAGE COUNTS FIGURE - I8 I-l3l GAMMA-RAY SPECTRUM loz. BOTTLE AQUEOUS SOLUTION, luuc. COU‘NTS PER MINUTE PER 60 Kev CHANNEL, 0.25 _. 0.20 _ 0.I5 - ' I 0.|0 0.05 — o “l—I—I—III III 6 I8 30 42 54 66 78 SO CHANNEL VOLTAGE FIGURE- l9 CePr' I44 EQUILIBRIUM MIXTURE GAMMA-RAY SPECTRUM, IOUNCE AQUEOUS SOLUTION, luuc Ce'l44 COUNTS PER MINUTE PER 60 Kev CHANNEL .25 __ .20 _. .ue E .l0 E .05 'l _IT I 0 11111 e I8304254667890 CHANNEL VOLTAGE FIGURE-20 RU'I03 GAMMA'RAY SPECTRUM loz. BOTTLE AQUEOUS SOLUTIOI I we .1 Ill 2 2 < I 0 ’ O X 0 0 ._, g 0.3 .. III 0. Ill .— g 0.2 +- x C u — —. — a DJ _ g T'“ r— 2 3 ° “H- T ° 0 0 :0 304254007090 CHANNEL VOLTAGE FIGURE '- 2' BaLa'I4O EQUILIBRIUM MIXTURE GAMMA-RAY SPECTRUM loz. AQUEOUS SOLUTION,quc Ba-I4O COUNTS PER MINUTE PER 60 Kev CHANNEL 0.4 0.3 0.2 0.I __...Xl0 0 I8 30 42 e4 00 70 '90 CHANNEL v0LTA0E FIGURE- 22 C0-I4l GAMMA-RAY SPECTRUM I02. BOTTLE AQUEOUS luuc SOLUTION. COUNTS PER MINUTE PER GOKov CHANNEL 0.2 0.I5 _ 6 IB 304254 6678 90 CHANNEL VOLTAGE FIGURE '23 RuRh-IOG EQUILIBRIUM MIXTURE GAMMA-RAY SPECTRUM loz. BOTTLE AQUEOUS SOLUTION loz. Ru-IOG .0231on B For «sci-meme sysmzs PWNSOLWBXBWWWEM mm WANSMIWBZBWLWNEOIB mm mm 1(8 i9):“ 0 “.8 M935; 3 mflm .Im. én0.4.no.e.m. 4mm) m 3. INS??? am mm III-'M. BIN-11.3)}, mmg mus mama-2.x murmg 3" “1 ”3‘5 ’ 30 AQIWIBII) fig; WW mom) 7 2012122 m 13.61.me22.1'10.ammogxmmfixmmm. If m mu." m n 4. 1. 2222234 IIIIIII" ’m' " "m" 00 £54! 1'39 o o '0‘ j 8 We» 2(09) Ir ’ mgotmrienm 2 I! m m 23.23 23 man-0 140-2244 00 1' mm me me as étnznmm) gufi‘fi’fi‘” *’ 2: H mm 0W 3.“ 0mm: “mm-1. 00 N 20 19 “2:33-20:20 "Om-NR) 5.5.5 5 130 “NW. ACE RSI-40mm 53 7 A(I-2«£,III=T GO TO 21 6 PAUSE 0‘! P3111225 20 no 1 2:21.22 8 Do 9 IT=IEJ,NC A(I~I,IT)=2(II,IT)*A(II,M) IF Accmmmma 0mm! 6,9 9 COIII'IIHJE A(II,I1)==0. 1 COEETIEI mm: mm W: In lines 14-, 7, and. 11: Replace letter 'N' with the amber of days of data to be analyzed. PM '10 ”HIE ll- ! 1‘ WW -mnms BADGE! WATOSQLVEIFXII'BMW ENE-TIDE mm w: m, a); 3 m?3% h.}§g.mo ”1' m3? au‘fi:.5.a.~s.x-: mm: (m lawman.“ PRINT 7on5.“ W138 mu 1:13.33 Z 51935.13: ' 113.5” . : m 8W sum 8%“ mm mm A DEMON A(‘P.5).B(‘h5) IF mm mm 2§m If mm m 23.23 21 DO 18 m :8 uninvmm) Hugh: (Mn/A: d1:) 22 I? Ammaovhm gamma: mm. 33319 131.110 19 MMJTPWJT) 5):“ 1:15“: ;P1.0.3 «3‘ @111 :1 55 56 6 m SE 0: 5mm: 20 D0 1 21:43.13}; IF (3 3-1) 8.1.8 8 D0 9 mszmgzc MN,I‘I‘)r-AC-IJTLAO-iJTMME—l,Ivz) IF mommy-230:: 0112mm; 6,9 9 conmm A(I-I,I£)==0. 1' cozmzwm 5mm; 31.33 3* RT“; 37 In lines £5, 7, and 11; Replace letter 'N' with the mmber of days of data to be mama. £23209... . 3.254 m2. 2:3 383 5:3 mm - ”.532“. 52:25. cwmzuouo cumxu>oz munchoo zumzmbawm 9 no Sui/9"" ' ALIAILOV HIV 0 N on hm393< >433 0N .. mmDGK .mzas >42 .i¢a< 10¢<2 9 2 (2w Iona) ALIMLOV aw ON on mm! M 3 Co-MIJ 44 ACTIVITY, I1 I! u! l H h ATMOSPHERIC R |03 I06 O - N u g 0 - l0 1” & a a I u I“ I .1! III I MARCH APRIL MAY JUNE FIGURE- 27 DAILY AIR ACTIVITY Ce-l4l,l44 8: Ru-IO3,|06 ATMOSPHERIC ACTIVITY. mm! M 3 Ifii_ LO ZrNb-95 in I I“! I] I“ I Il L5 L0 I37 Cs- 0 ”III I, MARCH APRIL I MAY JUNE FIGURE ' 28 DAILY AIR ACTIVITY Cs-l37 BI ZrNb-95 RAIN ACTIVITY flue/l. so " EMh‘émJ aoooL 400:;— o _ O 300 ° ‘3' cR- 223 CA - suuusn RAINS zooo — _. .0 O .000 _ , o H AU as N 56/ . 0 mm 02468I0l2I4I6l80 ATMOSPHERIC ACTIVITY uuc/M FIGURE ' 29 RAIN VERSUS AIR ACTIVITY GROSS BETA RAIN ACTIVITY uuc/I. so P IEASHEIHMN aoodL 4004 O _ O 300d. 0 cR-zzacA — suuusn quus 2000— O -— O O IOOO— , o HAUOEN / . - some 024SSIOI2I4ISISO ATMOSPHERIC ACTIVITY uuc/M FIGURE " 29 RAIN VERSUS AIR ACTIVITY GROSS BETA RAIN ACTIVITY . uuc II. 2200 _ ZOOO_ I600_ I200 BOO O l I I I I l I J I o I 2 3 4 5 s 7 a 9 AIR ACTIVITY. cue/M3 FIGURE“ 30 ' RAIN VERSUS AIR ACTIVITY (INDIVIDUAL ISOTOPES) IO GROSS BETA AIR ACTIVITY. uuc/M 3 20 IB I6 I4 I2 IO - Zr-95 ° 0 o r- o R“"03 - o o o P 0 0° 0 . C O 0:: o . Io +—O Co . C o o '0 °. C O 0 Mo 0. %‘ I— O . . 3”, cut 00 O o - . . l . L' o I 4 l J _ O I 2 3 4 5 AIR ACTIVITY, one! :13 FIGURE‘3I GROSS BETA AIR ACTIVITY VERSUS ZT-95 B Ru-I03 AIR ACTIVITY- GROSS BET» Mia ACTIVITY. CI-I37 20- O 0 I3 _ , o . O 0 I6 _ o ‘ . O O o o o '4... . O 0 g 0 CO-I4I,I44 I2_ ° . . o 0. 1'0- .. . . .0 . . .- .00 8— .. . . O .. O . o 0 0° 6 I— . .00 o O 4 — . o o O 2.. o o O J I I I I I I L I O I 2 3 4 AIRACTIVITY , uuc/ M3 FIGURE-32 GROSS BETA AIR ACTIVITY VERSUS Cs-l37 BI Ce-I4I,l44 AIR ACTIVITY. RAIN ACTIVITY AIR ACTIVITY CI I000- A 900... D 300 _ . 0 700; 0° O 600_ .5 500_ w 400_ D E d3 - p 300 .9 :& O BETA b o of 0 Ru-IO3.IOG zooI. '. A Cs-Ia'r . u ZrNb-95 I00 _ U I CC-I4I.I44 O I I I I 0 IO 20 so 40 so WIN D VELOCITY, MPH. FIGURE- 33 RAIN/ AIR ACTIVITY VERSUS WIND SPEED uuc/l uuc/ M3 RAIN IAIR ACTIVITY l000- a a I 800. I - 0 ° . CI 600..“ A 84 ° ’ I. d ' 8 4on0 8303. Q’ a I 2 ' A A 3 0A 0 A0 on. o‘ o . .8 o I I ’ o zm-A .-A. . ° I war A“ O I I L l I I I I l O I .2 .3 .4 .5 .6 .7 .8 .9 I.O RAIN DEPTH .In. FIGURE'34 RAIN/AIR ACTIVITY VERSUS ' RAIN DEPTH RAIN/AIR ACTIVITY I000 a U ' . BETA 0 Ru-l03,I06 800 .. ' CI-IAI.I44 0 U ZrNb-95 3 ° ° A CI-I37 300 -A A A A 0 go. 2 15' I 0 (J 400 ."z go .0 g g u A 0 a A A A U A 0 g 5° 2 zoo—3‘. 9' . . A O . o I I I I I I I I 0 I 2 3 4 5 6 7 8 9 CLOUD HEIGHT. I000 PI. FIGURE'35 RAIN/ACTIVITY / AIR ACTIVITY VERSUS CLOUD HEIGHT §§ N MEASURED ACTIVITY 5 o I l l l I l J I 1 I00 200 400 600 800 PREDICTED ACTIVITY AR — - 324* Iov AA FIGURE '36 MEASURED VERSUS PREDICTED RAIN/AIR ACTIVITIES mm0430 Fm I wmaoi >3. _ 4.52 :22: RAENE .. .. ”MU“, H 578 2? 3.52-3. .. >5? v3.3.7.0 ‘..Qa L 0. ON on O? AlIAILDV 'IVLOJ. :IO lNBOUHd .03 3.. in ”am 93 in 2m m3 3 «3. 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TF1; 232133 ”mgh Volume" felt filters 3. Rome’cer, 30 liters per minute capacity 13-. nanometer 5. Building Vacmnn systan 6. M high Velma” air mpler 7. min Collection Basin 8. Rain evaporation pants 9. 250mm infra-red lamps Counting 1. Iiuclear Chicago single channel analyzer model #1810 2. tholear (fracaga Model 186 scalar, (3-1 1013 automatic: sample changer and c.1313 panting timer. 3.- 69.8 flow mportional commuter with preamplifier and normal W, N. 0. model aMED 4. Sample mounts, copper scrapie pans. and one ounce bottles or glass 72 51W UUE? .4 4 z 535 GfiLY STATE UNIVERSITY LIBRARIES MICHIGAN 3 1293 O3 0 15 0196