 J. Hot Spring Sci. 0* --+ῌ-.- ,*+*

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A Method for Determination of Radium
Concentration in Hot Spring Water
Application to the Field Works
Takashi SAITO+

Abstract
The concentration of Ra and Ra in the environmental water can be determinedfrom the amount of radium isotopes recovered in the two successive batch operations
using cation exchange resin. The radium isotopes are collected on the cation exchange
resin by a successive collection procedures : the second collection procedure is applied tothe same sample water after the removal of the resin in the ﬁrst procedure. The concentration of radium isotopes in the sample water can be estimated from the amount ofradium isotopes recovered in the two operations by calculation. The amount of ,,0Ra and,,2
Ra on the resin are obtained by a g-ray spectrometry for the -/, keV g-ray from ,+.Pb
and for the 3++ keV g-ray form ,,2Ac, both in radioactive equilibrium, respectively. The
present analytical method is applicable to +* L of sample water having ,,0Ra concentration of larger than +* mBq/L and is also applicable to the ordinary underground water ofless than + mBq/L by use of /* L of sample water.
,,0

,,2

Key words : radium, radioactivity, radium isotopes, gamma-ray spectrometry, cationexchange resin !"#$%&'()*+,-./012345678*9:23;<*=><5? @ABCDEFG*H6 IJK8"LMNOPQ*RS;<-TU VWXYZ[\]PQ1"^_!`a#$%&*+,-./5 NObc?#$%&"d*efghijU kClmnopqrsqtu-TU ,,0Ra  ,+.Pb " -/, keV "kClm ,,2 Ra ,,2Ac " 3++ keV "kClm*vcwcx05 yac?#$%&1`az{#$%&|}*~023456.78*9:5? 78*H6c ,,0Ra |}<5 +* L "^_+

/0/ῌ*21+  +ῌ+. + Department for the Administration
of safety and Hygiene, Osaka University, +ῌ+ Yamadaoka, Suita, Osaka /0/ῌ*21+, Japan.

331

 



 +* mBqῌL  /* L   + mBqῌL 
!"#"$ : 
78%   &' ()*+,-./01/2" 34)56+ῌ ῏ ῍ ῐ ῎
9:;<= &'>)?@ABC= ,,0Ra DE : +,0**   /2?
@ABC= ,,2Ra DE : /.1/   ,,.Ra DE : -.00  FGH I.JK?@ABC= ,,-Ra DE : ++..   . @A:;<= LM &'>DENOPC= Q  RS T &' DEUV ,,2Raῌ,,0Ra WX<=LYGZ [\]^_M= `C= aLB B>RS T &'bc<=de fM ^_=ghiRYeje  &'Wk<=LYYe
LlB RS T m ,,0Ra ῌ>nopqfj=
ῌ  Trst2 s]*)() rsuvwxYyzf{ |z }sB!~e LpMejIv+,-./01/2"GZk<=  +303
῍  }]t2 !Y"sI)K ! j="st2Yyzf{ e z  EDTAῌ.Na! j!pe # +  ejYapM $)Y %$<= | $)'w)J"w)u)GZk<= M +33*
῎  }s% ejs`e |&'BO=t2(pMeBa, Y)*"sI)K

 !T"st2Yyzf{|# + e z TY+@A Pb Y %$ejpM z ()*+,,+.

-./01/2"GZk<= M +33.
῏  f{ ,-()*+,-./01/2"GZk<= M+31/
ῐ   1+* ./ e | $)'w)J"w)u.v!0 e'w)J"w)u)GZk¡¢ kf $)£e   e ¤¥¦v$I§¨ejn=$)pM©<= 12M +313ῑ.0sª/2j T ,,0Ra-free t2Yyzf{ az
}sB!~e «34)56Gj.0s34)¬­<= 3®f{
CyDTA B!~e |34)5678Gjt2¬­<=L.

w)pM4¯GZ+°±²e Iv+,-./01/2"GZk<= Yamamoto et al., +323
ῒ N³*2´2¦"u" ./e  µ¶()*+,-./01/2"GZk<= Salih et al., ,***
ΐ  t·2)¸ej$)¬­e | + ¹./<= a|¦v$I§¨e $)t·2)¸ej$)(,K"Bk<= Sapan et al., ,**+
῔"st2Byzf{ ºs!e Radium Rad DiskTM j»¼®¡ Radium Rad DiskTM (,5½./e |()*+,-./01/2"GZk<

332

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  Rihs and Condomines, ,**,

   !" # $%&῍  ῌ)*+,-.+/01234567897:&;<%'( ) ,**3 ;Tomita et al., ,*+*

=+ >?@A BCDEFGH ,**, &I#J >ῌ
J 

,,0Ra, $$K&%'( LM&.+ Rn $N,,,OP QR1ST:RU14567897:&;V#WX'*# .Y.) Z*)%[&.\.\)*   &J   ]1^_`:RU1a  Yamamoto et al. +323 J   &=* .#I< +< *.+*.. Bqῌg !bc.# $"d.#  #e %

+g

[&J f +** mg   )*#I< Z*)]1^_`:RU1J#e$gh  + mBqῌL igj%
 ')& j%



k&e&'lmn$

op ' ()qa< r1s1t u

vw$q Z*)xy*[ uvZ$Jz+qa +{& f +*f +** L  |}~&)*\)
NZq ,1   S , -.[ uvZ$&;< /0&1[q' Y)

2&3. '*+  |}~&< 01234567897:&;< OPqa
keV 0123 N**

W
4

?

,+.

Pb  -/, keV, ,,2Ac  3++

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9. 

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333

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-ῌ ῐ

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-ῌ+ ῎ῑΐ῕῍ῒ῔ !"#$"% &'() *+$ ,- .()/012 345%6#$" 789%:;<=>?@-9 ABCDDE,F/GH%IJ<KL,MN OP$
MN

--* ppmQRS / /* L  *.+ M TUVW2%XY Z[\]/^ -* g _`abcdefg Dowex /*W-X2 ,* /* meshOP@() *+

$ ()hE0MijE%kl@ m%n"$%odpq/rsW2 tuv%wxy
z#.{%=9MN %|}yz$ ~{%rsW2 J]W
2 9 *.+ M TU/J]YABCDD%@IJY$
$MN %|}y$MN] Y  !"$ MN{W2]-=hE0 Table + 9/# $ $
Fig. + %6

Figure + =9 rsW2< / L /MijE//=>MN /#< /* L %,#{MijE0 {,#.{<8+$ YY pq OP$wxE
OP#.{%=9 /* L rs/¡ -* ¢/ /*ῌ /#.{<£¤y$
rs< +* L {¥,P¦§0MijE /* L

OP$wxE/Y$h<«/#.{<8+$
Table + Barium concentration, sample volume and collection methods
used in the experiments.
Barium conc. (ppm)/Volume (L)Collection method-*//4*-4*//*-4*//*

Batch method
Batch method
Circulation method (0 L/min.)Fig. +

334.=9¨l#=©,ª]rs OP#¦§0pq

Collection curve of barium ion onto cation exchange resin.

0*  ,*+* 

-, 

 

!

 "#$%&'($)

 *+,-./0

12(34 5 !$)%&'657 89:%&';<=

%&'(>?,+@AB<

 C  DEFG
H I, +331 <6 Ca, ;<= Fe- ( /** ppm J!
KL 32῍ " M+

N>5

7 #$%&'($)OPQR
S ,TU

Fig. , Concentration of coexisting ions and ratio of Cc to C*.
 : Ca, ;  : Fe-(./V+

EWVXY7Z[\]
^_`
TU
89:

ab *.+ M S / L 89:%&' -* ppm%&' c`%&' d?

%&'( ,/* /** 1/* +,,/* ppm 6"<e c`%&'( -**

0/* 3/* +,0** ppm 6"<e*+f+g5` %&'hijk Dowex /*W-X2

5 +/ l +* m

5 !no"v_`!nw=x5Y%&'hijk5` C+ 6 C,

pq4rs5`!C+ jk-. + 6# {|-TU

C, 6 ^Y jk}./ C+῎6 C,῎ ~t CC 6 C* 6 ^_` 

Fig. ,   Figure , <46 CCῌC* 6 5`6M 89:

%&' 0/* ppm %$)57Y7!&'"TU%&' +,,/* ppm(~tV+M6(()5`
#L ,,0Ra ;<= ,,2Ra  *+-3

7Y

q4t5`u-* g d?7# yz ^Y pq_`!n5` C+῎6 C,῎ ,~57$,+`TU---* g ';<=U-+,

'+ῌU

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Fig. -  - ,.tV+' M6<4 5 5 ,,0Ra --3 ,+.Pb  ,+.Bi ,,0Ra 6M+,-/2L-3 ' ,,,Rn ; 0 : -.2,  ($)57Y` !5 'o"(S1 ,2 6 ,,0Ra-,+.Pb-,+.Bi -.¡3¢ £¤3¢ (H45"Y M` 
1 , '(2 5"Y<e56¥ ¦78(3*M- - 91 :Y

S; §<V¨`%&'hijk 1©=5*+f+1XY756 ?7 ,,0Ra +20 keV 6 ,+.Pb -/, keV 6 ,+.Bi 0*3 keV.¡ª 5 .¡ ,+.Pbῌ,,0Ra ,+.Biῌ,,0Ra « .¡3¢(H457Y ¬e \]>? ^_`:Y`/­@657(ac+A®¯ , °"123

'6U

 ±%&'hijk :Y7²³5`! ´:5`%&'hijk Doewx /*W-X2 aµV¨ jk66!1©=5` *u1 565 ,,0Ra
6 ,,,Rn (.¡3¢Bc- -* J¶m 5`!

HPGe '·¸¹º»¼½7

 ^_`
335

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

Fig. - Decay chains of uranium series (a) and thorium series (b).
(numerical data in parenthesis is half life)
ῌ !"#$%&' () : 0/ mm, *+ : +/ mm, ,+ : +.* mm -./!0123

45 Aralditeῌ 1"6'789:;<=
῍ >?@1AB& () : 1* mm, *+ : +0 mm, ,+ : ,.* mm CD.1"6'EF78G

H;:;<=
῎ I"0 () : 01 mm, *+ : +/./ mm, ,+ : *.,/ mm -CD. Aralditeῌ 34;;<=
JK Table , 8 !"#$%&'LM ,+.Biῌ,,0Ra *.2 >?@1AB&LM
 ,+.Biῌ,,0Ra*.- ,+.

Bi  0*3 keV >'NO +,+,* keV >'NOPQRKS

T.UV;:=WXYZ7[;:\]\ ^_ !"#$%&'`ab.;: \>?@1AB&>?@1"6'c7de]\CD]fgh?i'jkl;<mUeh_n_7o; I"0LM,+.

Pbῌ,,0Ra, ,+.Biῌ,,0Ra =pqrs + ]9:t

WXYZ7[;:\ ^juv+_< ^_8 7I"0.wxy ^
;<;g; z{h ,**3 |}~"Q;<?Q.!"/ &'77
;<LM ?i'_j]g9<^.;:\^_ Mj|}~"Q +h7 0** ;: <m |}~"QJgh?i'jl7;7
]9:\ ^jUeh_` 'EF7?Q'j4;<\ <m ?i'lj ¡]\=7]9:\ =Ueh_336

 0*  ,*+*
Table , 

Concentration of ,,0Ra, ,+.Pb and ,+.Bi (in cps), and activity ratios of ,+.Pb/,,0Ra and ,+.Bi/,,0Ra.

Container

Ra (+20 keV)

,,0

,+.

Pb (-/, keV),+.

Bi (0*3 keV),+.

Pb/,,0Ra,+.

Bi/,,0Ra

Polypropylene,4,2*4,*,4+,*4+3+4,,*4-,4+,*4--






+4/1*4*+40-*4**423*4*.
+40-*4--

*403*4*0*411*4*1*41-*4,**411*4+,

Glass culture dish+4-3*4+,*413*4+**4/,*4*,*4*0*4*,*4-1*4*.
*4*2*4*,

Steel (Tin can)*423*4-+/4,+*4/.
-40**4/*421*4,3*432*4*//4***4+*-4*-*4*2+4***4*/*422*4*/.4-2*4+*,41,*4*3*43-*4*/+4+**4-3*430*4+**42.*4++4+/*4-3*433*4-/*42.*4*3*410*4+++4*1*4-0-. 


 1 +, !"#$" + !%&'()*+,- "%&'( /+* L %./(012
(345

'+6

'+ 789:;$<=>?

ῌ @ABA"%CD῍' $"%&'( /* L %./E/ *.+ M CD F%,GH%IJ/+

IJ/+"%KLM > -* g  NO4PQRS Dowex /*W-X2+* UV/RS W=X/+ YRSRS ^/ +/ T

C+ resin #/+ Z+ "[ /* L \] -* g

/2 mmf2 cm %_`/ab345> 0 Lῌmin c> -* d" F

6ef+
῎ g*+ F%hij/' NO4PQRS Ek +/ T +* UV/ RS W=X/+ YRSC, resin #/+ "[ /* L \]lj/' NO4PQRSEk+m ῍#% -* d" F 6ef+n/+RSKef+m -.- >o /+pqrst%uv Aralditeῌ῏> /+w ,,,Rn [xy%zZ> + {|;}UV/(~/+
ῐ UVm" 3q24%A HPGe 4 > ,,0Ra : +20 keV,,+.

Pb : -/, keV, ,+.Bi : 0*3 keV -Gi ,,2Ac : 3++ keV 4 /+  ++. 

d)' A+ X# >/"x! v+
ῑ A+ C+ C, resin x! a # C*

%G=v+ ,- C, x!

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">/+  21+v% F424'(" x! )*+ F424> X[¡'Y#¢£ #¤>¥$%&l¦'[ §¨©ª![G«,'+v '§¨© (/+='!x X"> )¬!x */(Y#­+>? %

,®¯%lx°¬![±ZA(-= @>l)%²³%´A¬! .*K ,µ¶ : +.,-+*3 - >? // ·¸^qº>?+v ^q

%±ZA .*K ~¹ A» .*K x! ¼½lY#[>¥

789:;$<=>?
337

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¼½

ῌ

  !"/**+,*** mL

῍ #$% & '( +** mL )*+,-.,/-0)1234 &56/* mL 7("῎ 123489,-.: INSTA-GEL PLUS

B7C !

'*7,-.: DE !" F" &/* mL 56"1GHIJ-K0)
῏ 1234/* mL 56 ;<=(">?@A/* mL  INSTA-GEL PLUS

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level discriminator : o# ab( +, Ncdb ef"ῐ gh"ijh1GHIJ-K k(lm channel number 7nop7hqroE

stuv OP( * channel wx("p ynop7( z{|} dbNc~(y g"
ῑ h +322 )

  0"Y X u]^@  )WJ)b e   .*K ) {(". 
.+ ῌ

db(" 1 ) +, W)  @ + ) )IJ ¡7IJ
¢ ,,2Raῌ,,0Ra )ij

Table - £¤ Table - @ ,,0Ra

0§ +* mBqῌL ¨¡ +* L )¡7(¥ ¦0§ + mBqῌL R

¦ /* L ))IJ)b©ª«¬­7©®h«f" F" ¯°) ±h¬IJ ¡7¦²`³4¦´µE¶(¥  0¥L·¸)«­7©¹mh«f"
Table -

Concentration and activity ratios of radium and the progenies in environmental waters.
Concentration (unit : mBq/L)

Volume(unit : L)

SampleActivity ratio

Ra-,,0(+20 keV)

Pb-,+.
(-/, keV)

Bi-,+.
(0*3 keV)

Ac-,,2(3++ keV),,2
Ra/,,0Ra(,,2Ac/,+.Pb)

Reported Conc.
(unit : mBq/L)
Ra-,,0

References

Tamagawa+*+-.1-

0/3.33++3*.*+2-//ῒ,1* Yokoyama (+3//)

Sarugajo+*+**./

.+-

.-.





0ῒ++* Sato et al. (+31/)

Masutomi +

+*



+3-

+*,





Masutomi ,

+*



/*0



/3++

+4,*4,et al4+0*ῒ-** Horiuchi(+312)
et al4-1/ Yamamoto(+33.)

Masutomi -+*+12*++/*+*1*3*+*3*+-*,,1*+.*,4+*4,

Arima +
Arima ,

+*
+*




,*-+.
03+*+02+,
1*++

0.,0
.3+.

*4--*4+.
*41+*4,,

Onogawa +Onogawa ,+*1,3/+-2.0.+.0-/+-0-..,/-*.-.
,32,//,/0.
/0/.,+4/*4,+40*4,

Misasa +Misasa ,

+*
+*

.0+/
+.0-1

.2+
/,3

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..+,

++,/
+*++0,4-*4++43*4.

3



+.,

++,

-,-

,4,*4.

/*

*40.*4+/Hijiori

Kasawaki** Well water338-1ῒ11/* Yokoyama (+3//)
Ikeda (+3//)-1ῒ//* Yokoyama (+3//) 0*  ,*+*





  !"  #$! %& '( 
*+ -1* mBqῌL ,- ) ,,0Ra./)0123&, + 45"6789: ,< $=>! ?,@"#& !"A;,)B,

CD<#EF $!"#G, +20 keV HIJKL! ,,0Ra M$!"H

IJK<#N $!O = ,,0Ra A P# QR< ,+.Pb # ,+.Bi A P
#S,TGDUVW!"X"YZ[\ = 0 ) ]^I_*`a,) ,,0Ra
b,c Ide< ,-/ U f,gh& =<#EF 
i I, *.1,*ῌ '9 !j3 a k$! +2/.1 keV HIJK
ῌ,,0 [M& HIJK) +20.+ keV <3 

HIJKnopqrstu)0 ,=

Iῌ,-/ )l /1.,ῌ Mm  , keV < HPGeHIJK nopq8v 0#)GD" 0

IT ,gh& =X) ,,0Ra w[xvTGYy+& c#EF 

9= ,,0Ra  +20 keV HIJK l) -.0ῌ <3 ,+.Pb # ,+.Bi [M&  -/, keV# 0*3 keV HIJK l23z&Y [Z5{|8}t<= nopq8v)~IqIp I,tp!$90#$$\ = 0= 

 O ,,0Ra  +20 keV HIJKtp "0#)C)DY QR<2" ,+.Pb  ,+.Bi HIJK., 




 gh a ,) -*3*ῌ #[D3ZG\ = 0 )X]^I @"=, a z&YD>!$9>=c#EF  ,)gh a ) C+ # C, #),'9

]^I =W)D" -., c a

)? #\D$!D"0#& !" 0 .X,j"!c+,D"0# [= ]^I_*`a  mesh #X

y
F a

!,&=#G,y+&  >=./)]^I_*`a 
Onogawa +,*/* mesh [ +**,** mesh , X Masutomi -,/ L ,$ -. . #" " C+ # C, [ a # +M$= 

Table . ,¡ Table . 23 gh a  -*ῌ <>!c 3*ῌ <>!c y+& )¢U#£$?¤$!"0#%[,D>= 0 23 & = ) a ,¥¦
G0#& =.-  §¨'!?Z#$! (©ª«f,# ¯ $

\ X[ $¬­®30 $!" 0 .°±,!(©ª«, $=

[O

=# WX Onogawa ,, Hijiori
./ >=./²,)³$´  >=c

Table / ,¡ Table / 23 (©ª«f#§¨²$µ­>=./ c¢U#£$?¤$!j3 0(©ª«,*&0#,C<0#+%$=
..  !"#$%&'"%()*+ ,-./,j"! ¶e)·¸,¹#TGYº¦0#& !" b,»$!D"$=A P#prn¼½p "
339

῎ 


Table .

Radium concentration obtained in di#erent experimental conditions.

Volume(L)

Resin size
(mesh)

Masutomi -ῌ+Masutomi -ῌ,+*/

Onogawa +ῌ+Onogawa +ῌ,+*/SampleTable /

Collection e$ciency (a)Concentration (unit : mBq/L)
Ra ( Pb)

,,0

,*ῌ/*
+**ῌ,**+*1*3*++,*-*+*3*+-*+*-*-*,,1*+.*,01*0**4--*4*,*43,*4*+*4,1*4**423*4*+*4-2*4*,*423*4*+,*ῌ/*+**ῌ,**-/+-0,3+3-*.-.
,2.3/,/0.
.31+2*4-,*4**43+*4*,*4-2*4*.
*43+*4*,*4.+*4*.
*43-*4*,

,,0

,+.

Ra ( Bi)

Ra ( Ac)

,+.

,,2

Pb

,,2

Bi

,+.

Ac

,+.

,,2

Radium concentrations obtained during the ﬁeld work and in the laboratory work.

SampleRa (,+.Pb)

Ra (,+.Bi)

,,0

,,0

,,2

Ra (,,2Ac),,2Ra/,,0Ra (,+.Pb)

Onogawa , (lab.)
Onogawa , (ﬁeld),2*+/-..,/,3++/,32,//-1,//0/.,+43*4++40*4,

Hijiori (lab4)
Hijiori (ﬁeld)

++,
+.,

++,
++,

-..
-,-

-4+*41,4,*4.

 -. /   /**  +,*** mL  !"ῌ#$%&'()*%+ ,-./01(2% Masutomi -  Onogawa , 3$%
-. / 45#6!789:;<=9>:?@:A

B+CDE-./01

LSC

FG῍H3I$JKL X M XRF B+C?N@OP1QR .*K -./01(B+C'E-./01 .*K S3TUV'#6!

D,-2 U, ,-, Th

WXYZE-./013B+&'([/*&\]C&  ^N@O_`8,-,

Th, ,-* Th, ,-. Th pH ( - ab*%c!defghij,-2U, ,-. U *fkWlmnopghJ%Jk qRcrab*& W+ sB+C&-.tY
Z Fig. - 6! ,,0Ra|}J&,+.

Bi u6v ,,2Ra,,2

Ac wYZ&\]C& xyz{~NA:#@O( &3&+#*.+ M 7#J&+ onw|}J%&D Ra  Th lmn : +.3+  (
,,2

,,2

J%& WCXYZkE-./#QpC&j&W' :M^^N=C@OWXYZE-./01
Ra -./013 0 

,,0

Ac

,,2

,,2

,+.

Pb

Ra -./013 , JB+ ^N@Oῌ,,2 -.

/01XYZ& ,+,Pb  ,-3 keV :M3 1 &'#6!B+C&j&# Masutomi - # %J,**+  0 ¡# ,**,  . ¡#3¢3 Table 0 #£ Table 0 6! ,**,  . ¡# ,,2Th (¤ +*#Ju! 789:;<=9>:#6!B+CE-./# ,,2Th kQpCJ%&'(¥¦ Masutomi - # %J  ,+,Pb ,,2Th (§QpC( Onogawa , # %J(¨©J%+#3&'()*¬

W'ῌ3²JQ!

,+,

Pb ª«S

Ac -./01­®¯°±¯w

,,2'C³´3 +¢3 Table 1 #£

Th

,,2

Table 1 6

E-./01 .*K S3TU%S:M^^N=#6!B+CE-./01(dµ_¶S#*! :M^^N=#6!B+CE-./01
§QpCP1·%k&'(¸¹pC



E-./01 .*K S3T

U%S( :M^^N=#6!B+CE-./016!º»¼%6½#k340

0*  ,*+*


Table 0 

Build up concentration of ,,2Th in stored hot spring waters.

SampleDate ofmeasurement,,2
Th (,+,Pb)
C+ (cps+*-),,2Th (,+,Pb)
C, (cps+*-)

Concentration(Bq/L)

Masutomi -῏+
Masutomi -῏,Jun. ,0῏,3, ,**+
Apr. ,῏., ,**,

040*41.34,*43.4+*4.
-142*43*4++*4,+4*3*4++

Table 1 Concentration of Ra and the progenies in hot spring waters by
di#erent method (in Bq/L).
SampleRadaughters.*K(LSC)

Radaughters(LSC-XRF)

Radaughters(HPGe)

Masutomi Onoawa ,,04,*4,
14-**4*3+141+4+.40.*4,*,*4.+4+.4+/*4+,   ! Masutomi -" #! - $%&' ()

#*+,,#*-./0/1 2345 6%789::;<=./ ῌ



>?4@A: B  CD#CE ,,0Ra F#94J#I #*)
 Table - *)

GH4I ,,2Ra

6 ,,2Raῌ,,0Ra K;%4J

GH

6 Raῌ Ra ! *.- L +2 MNO%A

GH

,,2

,,0

LP:
L  QR!SO:F ῌGH4I)  %T#C
4I!UEN V4WXY Z[\]^_# ,**-  1 `L ,**. 
+ a` +, `'4

Ra, ,,2Ra (*b ,,2 Th,,0#:QR Fig. . #e Figure . *)



6 ,,2Raῌ,,0Ra cd

!fgg4! + hiN %I) LD 6 ,,2Raῌ,,0Ra 9!J7 %ALP: V#^ ,,2Ra
k4I

,,2

Th

!lmn ELP:  op4  qrst !lmnu (v wx ,**3
N   ! y%!J7 !#T#z${|}<=~ % &%'I) V  D

%(# N&%~)%D7% ,,2Th

L#"j

%C4IC*EN !9+4I%  ,%#= oῌcdE%@A#*) ,4 

JEn,u#-E

./%4J9 <=/   ῌ 

0+F#1# )WX¡# P ¢/£¤¥¦-§¨©§ª «NB:῍ ! ¬­/®¯°± ²³0Y 2@´9 4I) "  3% +* L 4 µ¶!²³0 5d24 /* L ·¸!3 " %^_#Eµ¶!¹/ºN:»4¼6*72%½4IP:
῎"

3% +* Lµ¶! +* mBqῌL 4 /* Lµ¶! + mBqῌL ·

,,0

Ra

3%½
341

 



Fig. . Concentration of radium isotopes and the progenies, andactivity ratios of ,,2Ra/ ,,0Ra in Tamagawa hot spring water.
 : ,,0Ra ;  : ,,2Ra ;  : ,,2Th ;  : ,,2Ra/,,0Raῌ    !" ,,2Raῌ,,0Ra #$%&'()*+,-./#012) 34/"+567./2&' %89 :);<#=0>7?!@#ABC>
῏῎D+EFG72'HIJ KLMN+OJPQRHISTUVS ῌWXYZ[\)0]2^_`ab cde2fghIXiHG H jk+lm2' noc
pq+r'HIsSt u[\ v wxy2fgPIHG jk+lm2

'zc{ +|RHI }~S  xy ~S 
VVxy)0]2 LSI N2hIXiHG
ῌῑῐ῍
"

¡¢l £ ¤¥ ¦ +331 : §%¨%©¨9 ª« %¬5^­® No. ,/1.
¯°V ±W ² ³X´ +313 : µ¶·¸¹º » ¼½2PJ 342-*

2.῍23.

0*  ,*+*

   +312 :    !





"#$ %&   ' ()    *+, -. ,3 02ῌ1/.
/ +3// : 0."# 

1  1 0.23 4 / !"0.56

10 +*13ῌ+*2,.

7879 +303 : 

,,0Ra #$:;%<&/3=> 4 . ?.@6 1 +0ῌ,..
AB ' CD E(FG +33* : H)I*J+K () +Lῌ+,
M-NO ,,,U, ,-.U, ,,0Ra, ,,,Rn P. +Q-. ,. +,-ῌ+-,.
RSTUV/WX ,**, : #YZ[ \0 pp. +2ῌ+3 RSTUV/WX *]
 12 ^_3` 48a` b5 c +322 : 678def X g#Y h ijk ῌlmno ῌpqrs ῌ9tῌuvῌwk ῌwqo ῌlx(hy: ?.@6 ,, + +ῌ1.
Rihs, S. and Condomines, M. (,**,) : An improved method for Ra isotopes (,,0Ra, ,,2Ra, ,,.Ra)
measurements by gamma spectrometry in natural waters : application to CO,-rich thermal waters from the French Massif Central. Chem. Geol., +2,, .*3ῌ.,+.
Salih, I., Pettersson, H. and Lund, E. (,***) : Determination of ,,,Rn and ,,0Ra in water using alarge volume ionisation chamber. J. Environ. Radioactivity, .2, ,-/ῌ,./.
Sapan, A., S., Kullab, K., M. and Ismail, M., A. (,**+) : Radionuclides in hot mineral springwaters in Jordan. J. Environ. Radioactivity, /,, 33ῌ+*1.

b5 c z;{< =5|> +31/ : }~?I(hy4%<@AB 
?.@6 +* .1ῌ0*.
Tomita, J., Satake, H., Fukuyama, T., Sasaki, K., Aya Sakaguchi, A. and Yamamoto, M. (,*+*) :Radium geochemistry in Na-Cl type groundwater in Niigata Prefecture, Japan. J. Environ. Radioactivity, +*+, ,*+ῌ,+*.

cC bD E bF  C  BGH ?IJ " ,**3 : K
BL Na-Cl 

Ra M_I+K -.

/2 ,.+ῌ,//.

NI =5   !EJ B/
M¢£

8aO ,**3 : ¡_ Be ++ ¤ AMS o¥  P¦§K.

Yamamoto, M., Komura, K. and Ueno, K. (+323) : Determination of low-level ,,0 Ra in environmental water samples by alpha-ray spectrometry. Radiochim. Acta, .0, +-1ῌ+.,.

" Q ¨ ZBR< © Rª S « ¬­| +33. : ®T¯B°y  ,+*Pb : ,+*Po 4 ,  ,+*Pb : ,+*Po ±  -. .. +2ῌ,1.
zUO +3// : %<&g"# +-  !"0.56 10 //+ῌ/0,.

"VW² SAITO, T., UEDA, H., OHTA, T. and SATO, J (,**,) : Determination of radium concentration in hot-spring waters with cation exchange resin. J. Balneol. Soc. Jpn., /,, -ῌ++.

(+,X,³,+ ´ µY ¶·¸¹­Z µº´»¼  ,*+* [ 3 ½ +. ! !"-.@

0- ¤K@ ,,

343