J. Mass Spectrom. Soc. Jpn.

Vol. 59, No. 2, 2011

REVIEW 
 10  
Fundamentals of Mass SpectrometryῌIsotope Ratio Mass SpectrometryῌKeisuke N6<6D  Geochemical Research Center, Graduate School of

Science, University of Tokyo, Bunkyo-ku, TOKYO, JAPANThe basic physical aspects of atoms and isotopes, as well as the physical and chemical processes responsible
for variations in isotopic ratios are overviewed. The major techniques in current use for isotope ratio measurements are stable isotope mass spectrometry (MS), noble gas MS, thermal ionization MS, inductively coupledplasma MS, secondary ion MS, and accelerator MS. The types of ion sources suitable for use in isotope ratio MS
are electron ionization for gases, thermal ionization for non-volatile elements, inductively coupled plasma
ionization for the majority of elements, and sputtering ionization by means of a high energy positive or negative
ion beam for solid target elements. A variety of ion detection methods using a Faraday cup, a Daly collector
system, and an ion counting system with a secondary electron multiplier are capable of covering a wide dynamic
range of ion beam intensity, from 10ῌ8 to 10ῌ19 A. Methods used for data processing and for evaluating thereliability of data for the isotope ratios that are obtained using MS are described
(Received September 9, 2010; Accepted January 14, 2011)1.  

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ff1)   .gDJ6& hi $ #j3,k:lLmJ !"2&2), 4)6)n*"#qr%#s&

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31*+¬­# "#®¯; °e& v:"Correspondence to: Keisuke N6<6D, Geochemical ResearchCenter, Graduate School of Science, University of Tokyo, 7῍
3῍1 Hongo, Bunkyo-ku, Tokyo 113῍0033, JAPAN, e-mail:nagao@eqchem.s.u-tokyo.ac.jp
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5O10191.6O1021(1.0¶1.5)O1019
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Se
82
Kr
96
Mo
100
Ru
110
Cd
124
Te
130
Xe
136
Ba
130
Xe
150
Sm

8O1020 b)
2O1021
7O101848

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Ge
82
Se
96
Zr
100
Mo
110
Pd
124
Sn
130
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136
Xe
130
Bac)
150
Nd

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76

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Table 3.
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F¢a)
c)

Th
U
238 c)
U
244
Pu
252
Cf
235
U
235

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Table 4.

. a1?%DNFu

L»1-

L»
3

H
Be
14
C
26
Al
36
Cl
39
Ar
40
K
53
Mn
87
Rb
129
I
138
La
146
Sm
147
Sm
176
Lu
187
Re
232
Th
235
U
238
U
244
Pu
10

M N¼U+",F¢

M
3

He
B
14
N
26
Mg
36
Ar, 36S
39
K
40
Ar, 40Ca
53
Cr
87
Sr
129
Xe
138
Ce
142
Nd
143
Nd
176
Hf
187
Os
208
Pb
207
Pb
206
Pb
131῍136
Xe etc.
10§OI (2005)6) ½
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12.32
1.50106
5,715
7.10105
3.010105269
1.270109
3.70106
4.8801010
1.570107
1.0501011
1.0301081.0601011
3.7801010
4.301010
1.4001010
7.0401084.4701098.00107b῍b῍b῍bῌ, ECb῍, ECb῍EC, b῍
EC
b῍
b῍
b῍
a
a
b῍
b῍
a
a
a, sf
sf, a

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C[\" |;S3,jz !+ 01ALE Tv '( )*+ " 

C5++"{5# | }}Gu O< !",-  

01AL,H

 ./012 149Sm, 157Gd 3# keV  4u# VW"#ZW~5Y"L+01[5+6 , 7 56 !+m2rH,rAb9|;S5- %85%9 !

k+5H !+AL`+ ~VW!+aO\j`+ }G+*# :;3$5< # =+, ZW5 ,`9O [m2rH5B

,>!5" ?@A# B*#,$,c! "{ M+"Zo5+,+C$D+ ?@A*8(%,EHe

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10

14

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41

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K. Nagao

Fig. 7.

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Table 5.

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86  86Sr/88Sr«

>?¯F­TQIJKQf

1 * 2 *?

t¥&4A.


&

23)

? kl¨{

 V®JKx& df

ICP-MS 8 Ba  138

8u¦m§

CO2  40Ar  2 *

Arf ]?c CO2f #$%-A= hB ! N138>?=&' WF£%¤JK @ )lY s@! ! ab XVW #$%-A' de'8q

Z #$%YTZ8 

J&  ]^RA.w]A.

`];^8[_Jp"r !

8[ A.$] 20Ne ]?c 22Ne "%-mok¢] A.=

"#$%& ,- >#$ ;?@ A./0%-hi+jkg#$%zX$|n¡@ 4()  ! #$ ;8%:#$%#$#$ ; 6"8 !

&<'

ICP-MS ODPQW8

 a#$%o8 bcBCDE%F=

4 ! Table 5  5404  mODPQ_= `)! "#,&-./0123 ,#$%40

'#$>?>?$hB !

  R4?& 8b ! #$ ;Z"8  ]^RA.



!

pTuK! #$ ;] #$ (mass discrim-: ½M/DM½

! ~Y #$%oVyW

{

6" #$%

o&U8-8 VyWzX{ ?

8 Rtrue ]?c Rmeas ' V
epow, eexp, eli ' 1 #$¡J[ Dm '%: }#$F8 !
῍ 46 ῍#$  


Table 6.
L


2

1

H
Li
B
C

H/ H
Li/6Li
11
B/10B
13
C/12C

N

15

O

18

7

Mg
Si
S
Cl
Ca
Cr
Fe
Cu
Sr
Pb

N/14N
O/16O

26

Mg/24Mg
Si/28Si
34
S/32S
37
Cl/35Cl
44
Ca/40Ca53
Cr/52Cr56
Fe/54Fe65
Cu/63Cu86
Sr/88Sr
206, 207, 208
Pb/204Pb
30

yz

T¢

yz£5 (Standard Mean Ocean Water)
4 Li2CO3
B(OH)3 ¤X¥ NIST, ~¡yz^¦~¡§ J¨% ©ª PeeDee  Belemnite
f (Belemnitella americana)Fuyz£5 (Standard Mean Ocean Water)~¡§ J¨% ©ª PeeDee  Belemnite
f (Belemnitella americana)
« Mg
f¬­
Canyon Diablo sfJ® J® (FeS)yz£5¯4 CaCO3
4 Cr(NO3)3FeCu
4 SrCO3
4 PbCO3

V-SMOW, SLAP
L-SVEC (NIST SRM8545)
NIST SRM 951
PDB, NBS18(CaCO3)°± (2007)3)% k² (2002)8), ³
IAEA¶ ¡'·¸27¹
NIST¶ ~¡yz^º»q
IRMM¶ ¼n½myz|:º»q¡'yz|}N2(atm.)V-SMOWVPDBNIST SRM980
NIST NBS-28
VCDT
SMOC, NIST SRM975
NIST SRM915
NIST SRM979
IRMM-014
NIST SRM976
NIST SRM987
NIST SRM081´&dk (2010)17) µ0

 !" (mass
discrimination)  # $ % & '  ( Fractionation )mass bias *+,-./*0 1(% 2.2.2 2
34+ fractionation (&  5
6*78% mass discrimination (% 92 %  : ;<=>*0 <?/@% fractionation 4 
 ( MS 2 <3A&BC*2D
% mass discrimination (E!"?F<3AG?  2D0

 2(% 10ῌ7 Pa z{Iw|}N yt<C.OP~2DS% IwQRm<0 S ?`2(% i?5
TUDM\ mo2(VW
X?Y"56 \0 C4+?599?ZB<IJK ABC&d ?\% [\Ck* P++2IJK0](r\]/2DS&d^_`C2-D0
4.3 

4.2 

 :25   moC ( HIJK(% L !"

 a bc#CQFd% LJa#$M 92N%&O '?&O<  e ;(*?*0 fg 

?*()2PA% Q*R"5 gh< K-Ar gh4+% fJa< 2DS% */TUVKWJXY2D0 IJK

ML

 

<-[D0  jk(% Ck  y>kM+M    3,Z2

A?*-[(% IJK <C./2DCk(% Mjk2 l   mnC%L !"3^2(% 4H4_5?`67a9 56h=>D0 -[4(% C4'ol   mnC % EC Mol 

L % 5M(8b9c)&de:+;M-M5
L % M!"L f[g< EiC e  ./

F 2A0\% IJK0]<12(DMT  2P/
*0(Ar)  e\jk2DS% mKk (peakheight comparison method) #C-D0 C

jkpq(% olg< 

a< rjjC-D

2AC2DS% <3  599?/0 C4+?!"#$3^Hi?A\

4  aCMsfJyt 

% BCk*4)5&de25M#$.D<?`tD*M*0 uq(%+?i? Mj@5L  CC)% &deE-Klmnmo pq y>k 3`C2DS% v&5

Mi?r2AsE*0 t  (wxC)yzolZHH*(FuE-G/?i?v?-[*?`M0 yt He 

H*2% IwJJ2KLP+0 MxF

 ( 510 ZC{-M*0

ῌ 47 ῌ

K. Nagao4), 21) 
   

1KZQ[ACj (TIMS) \> N{  j (ICP-MS)  VW'y&G! !

  !"  #$



%&

'(

 E(Mj !"VW῍()#*+   ,-./0  !
+  12 3(45"

" ]^ + $$ Ri, R 
y&G! !"'wf(( 6-7 

!*& (!6/ (((((6/(9$%  # "+ rx, rs,:' 

[S 0] ῍' 

'1%;( “0” (&#  

D TVW'_1" !": ( 'TF((`

# “1” (  [X0]!'( “0”ῌ(RmFRmi)2
nF1

Q# B^ + Rmi, Rm wf(TF<!"=>(%<?-*+(TF n TF(wE*+

rm@([X0]rxA[S0]rs)/([X0]A[S0])[X0] =BC  D E #  'G  -@('( 2/G6/G

 I/G([X0]@F{(rmFrs)/(rmFrx)}[S0]!5$ !c*+ WR VW'$(H/GI/%  rm JKLMN
O( ( JK"'(

(()*  !P ' Wdy&G! ! 'G  F
VW'(efF (1%;y&G! (
g!"6/G!EF !"Q#+

9Q+E-R, + -. !"  S

M8 i *g

D  TSU/Gj % E+ $(9'V/(

'V/( 

X!-YI $ -*+ 1KZ [2( K-Ar $%  1" [2 K /G\3!"40

6]^_ 40Ar (-)**+ $(9

[2( Ar/ Ar 
40

36



5.1 

 D(N)*-*9

0' SD  ( -I/G9(( 2/Gabop#$ !

c*+ !-" #E(



¡(¢

%"%.<5G VW' #$%& £( N ,#qrsW0i0¤¥#$Ar `a 100bD!21)+
5. 

F-@(F/G

'h:!"ij#k( lE ,#+   #jm nG  0W((#9 38

'(@(

`ab-7 F*--'G +45(TFn  ' (wE*  n100+(!6/ 8#" -#+ rm 

ῌ(RFRi)2
n(nF1)-9t*+ D O¦§M-¨K©ªO u!" «I¬q­^$#c



,#(

 ®¯¡]VW'Wv(' ( JK" °¦±(§²³#$ - ab(7  #78DcD*- 9:# °¦±I´#Kw**+ $!"' (% (&d9" KL(c ¢(µc¶X !F ef(*g3h! (3hd9"(abQ#+ ·D. x F M8-*+ i ("  j %;kT*+ j <= >?

¸y ! /0y&G!7©ªOuz!"(*+ -lMh  @mA"no"

5.2  pB#q ( -C + $ GD

E( r#stuOv !" q(wE *x)#+ $(% F¨j  1%;%" "1&(  #    KL(c  Y   y&G! z {M|} HI#~J  K

 lM¹ 8#+ Table 7  $ G(%

L;k ^g!"@F/GM8 i -NO#

Q81D 9(*+ ®º *d 9 (9EP!"EF !"Q!

!

 &(6/#74 !"#25)+
 WR 

F 02G ( 78 %" + Table 7 I/
%  {8(7(Q[ACj (TIMS) *& 10ῌ5 => o"

N {       j (ICP-MS)   10ῌ5, j >? 'y&G! !"\>

'G #ES( /Gd9TF UVWX

McKinney 4j 10ῌ4 |»lM : (YZ U!6 ' #j 10ῌ3 J}¼j 14 C/12 C @{M(5(*+10ῌ12 `  
ῌ 48 ῌ

!"0.5 ½ 10ῌ2 `  (     # 


Table 7.






()

®






87

Sr/86Sr
W/183W
18
O/16O
18
O/16O

0.7
1.85
0.002
0.002

TIMS
¯!´ ICPMS
McKinney ´ MS
SIMS

µ

3

He/4He10ῌ5¶10ῌ9±²D´ MS

³J

14

10ῌ12¶10ῌ16

AMS

182

C/12C

14C  50  
ICP-MS  

 





TIMS,
1)

ICP-MS  !



2)


3)

 3He/4He *)+ 14C/12C

*,#!" #   $%-%#4)5)&'#./
6. ῍ ῌ ῎

()

6)
7)

 0123 
8)9) #4) *+56 7,*)+"-8./
9:';)0 <#=>12?@8A#BC 345D8EFG@8EH68E78#92:
=10)> 7,"#7,"O?#-@PA.

11)

,;I./JJK L5<6MMN

= BC*   ?DQ R  
12)13)

#EM FG  HI SJ K#TL (23MBU(5V5N(4)(  OPQK 
(#ST



MJ#R 




W#

XYZ[*)+XYZ$ #7STU\OP#

* VWKJ 

#Y] KZ[\^J17)  #X
]

18)

5#_^

`abcdeZfJ #_g#hi`a

14)
15)
16)

 

19)

bcLdMjklk#  mE# %efn#gh`a oi-%H jp i-%#qk'6,01 

 rnls(

' #)%W# tmn  uoJ
MpvEpEq*)+qLjklkwkxk#stJ #4)u

Mr

22)



ῑ ῐ # vwyzx{|( 5y8}z#{~|}~ =v5 %{EwZ M # r |5v5

20)
21)

23)
24)
25)



¸ SIMS῏¹ºXYZ῎

±10ῌ5
ῌ10ῌ4
10ῌ4
10ῌ3

Faraday cup
Faraday cup
Faraday cup
16
O: Faraday cup
18
O: SEM
4
He: Faraday cup
3
He: SEM
14
C: ´XYZ$®
12
C: Faraday cupῒ   

"#$% #&'( #)%    TIMS

 

$®

Z¯e°²Zc³Z°J°JTIMS῏Rµ¶´ ¸ ICP-MS῏·¸r"d¹® ¸ SEM῏¹º¶,¼½»¸¼½ -%/®

#10ῌ2

῍5·10ῌ3¸ AMS῏º»῏J. S. Becker, “Inorganic Mass Spectrometry,” John Wiley& Sons, Ltd. (2007).
p~    2?8A#B bw
k   w (1983), p. 143
J.    2?8#0 n, ZkEZ (2007).
~   8z (1998).
“Radiogenic Isotope Geology,” ed. by A. P. Dickin, Cambridge Univ. Press (1997).
7  8 8  (2005).
      2?8  3  8z (2003).
4p   ¡ ¢£¤ No. 1, 2 (2002).
F. W. Aston, “Mass-Spectra and Isotopes,” New York
Longmans, Green & C. London Edward Arnold & Co.
(1933).
p~  O¥8 10῏>12?8 =¦ῌ §¨ z¡ (1976) p. 444.
“Nuclides and Isotopes (5th ed.),” General Electric Co. &KAPL, Inc. (1996).
p~  J. Mass Spectrom. Soc. Jpn., 52, 159 (2004).
M. Ozima and F. A. Podosek, “Noble Gas Geochemistry(2nd ed.),” Cambridge Univ. Press, Cambridge (2002).
=¦ῌ SJ |¢£ (1977).
bwk   w (1983).
2?8O¥( ¤ ¥E©¦§ª 4=2?
8z/«¨ ©ª¬ (2010).
M. Kusakabe, S. Maruyama, T. Nakamura, and T. Yada,
J. Mass Spectrom. Soc. Jpn., 52, 205 (2004).
J. D. Gilmour, I. C. Lyon, W. A. Johnston, and G. Turner,Rev. Sci. Instrum., 65, 617 (1994).
S. A. Crowther, R. K. Mohapatra, G. Turner, D. J.
Blagburn, K. Kehm, and J. D. Gilmour, J. Anal. At.
Spectrom., 23, 938 (2008).
{­« 2?8 31, 35 (1997).
K. Nagao, A. Ogata, Y. N. Miura, and K. Yamaguchi, J.
Mass Spectrom. Soc. Jpn., 44, 39 (1996).
N. Ebisawa, H. Sumino, R. Okazaki, Y. Takigami, N.
Hirano, K. Nagao, and I. Kaneoka, J. Mass Spectrom. Soc.
Jpn., 52, 219 (2004).
T. Hirata, J. Mass Spectrom. Soc. Jpn., 52, 171 (2004).
R. H. Steiger and E. Jäger, Earth Planet Sci. Lett., 36, 359(1977).
¬­ \ ¢£¤ No. 2, 56 (2002)

Keywords: Mass spectrometry, Isotope ratio, Ion source, Ion
collector, Data evaluation

῏ 49 ῏