Stable isotope anomalies and

early Solar System chronology

Stable isotope anomalies and

early Solar System chronology

F. Albarède, M. Arnould, R. Carlson, N. Dauphas,

T. Fujii, S.Jacobsen, Q. Yin, E. Young

F. Albarède, M. Arnould, R. Carlson, N. Dauphas,

T. Fujii, S.Jacobsen, Q. Yin, E. Young

Chronometry must also separate radiogenic ingrowth from isotopic anomalies:

• Nucleosynthetic anomalies• Spallation

• Mass-independent fractionation

Assumption of mass-dependent fractionation of stable isotopes

Consistent with Urey-Bigeleisen-Mayer (1947) equilibrium fractionation theory and kinetic effects.

Additional distillation (Rayleigh) effects permitted.

Interpreting isotopic anomalies:evidence of mixing

Interpreting isotopic anomalies:evidence of mixing

Trinquier et al. (2006) Luck et al. (2003)

Internally normalized Stable isotopes

Interpreting isotopic anomaliesInterpreting isotopic anomalies

Zanda et al. (2006)

I Nucleosynthetic anomaliesI Nucleosynthetic anomalies

neutron closed-shell N = 50

neutron closed-shell N = 82

Predominance domains of the different nucleosynthetic processes

Predominance domains of the different nucleosynthetic processes

Arnould and Gariely (2003)

Detecting s- and r-process anomalies on Ba Detecting s- and r-process anomalies on Ba

11σσ iiii NN

1

10

100

1000

10000

130B

a(p)

132B

a(p)

134B

a(s)

135B

a(s,r

)

136B

a(s)

137B

a(r,s

)

138B

a(r,s

)

5

10

15

20

25

30

40

50

60

80

100

Tσ

temp (keV)

neutron cross-section in mb (Bao et al., 2000), temperature T in keV

s-process at steady-state: N mirrors

Dip of neutron cross-sections forclosed-shells (magic numbers)

Dip of neutron cross-sections forclosed-shells (magic numbers)

138Ba142Nd90Zr

88Sr

208Pb

Ba nucleosynthetic anomaliesBa nucleosynthetic anomaliesAndreasen and Sharma (2007)

Ranen and Jacobsen (2007) Carlson et al. (2007)

Mass balance equation for nucleosynthetic componentsMass balance equation for

nucleosynthetic components

f: weight fraction of each component: deviation from terrestrial abundances

Linearity also holds for isotopic ratios of a same element not for different elements

Binary (s,r) mixing in Ba from carbonaceous chondrites

Binary (s,r) mixing in Ba from carbonaceous chondrites

Andreasen and Sharma (2007)Andreasen and Sharma (2007)

Saint Severin

Murchison

Allende

Juvinas

-8

-6

-4

-2

0

2

4

6

8

10

12

14

0 5 10 15 20 25 30 35

137Ba (ppm)

13

8B

a (p

pm

)

More than two components in Ba from carbonaceous chondrites (p,s,r)

More than two components in Ba from carbonaceous chondrites (p,s,r)

Andreasen and Sharma (2007)Andreasen and Sharma (2007)

Saint Severin

Murchison

Allende Juvinas

-100

-80

-60

-40

-20

0

20

40

60

80

100

-40 -20 0 20 40 60 80

130Ba (ppm)

13

2B

a (p

pm

)

Binary mixing in Sm …

Binary mixing in Sm …

Mokoia

Grosnaja

Allende

Murray

Mighei

Orgueil

Indarch

Ucera

Peace

Homestead

Gladstone

15555

GRZ-1

-200

0

200

400

600

800

1000

1200

-600 -500 -400 -300 -200 -100 0 100

e149Sm

e 150

Sm

100

1000

10000

100000

144S

m(p

)

147S

m(r,

s)

148S

m(s

)

149S

m(r,

s)

150S

m(s

)

152S

m(r,

s)

154S

m(r)

T1/

2

5

10

15

20

25

30

40

50

60

80

100

Carlson et al. (2007)

… or not?… or not?

Mokoia

GrosnajaAllende

Murray

Mighei

Orgueil

Indarch

Ucera

PeaceHomestead

Gladstone

15555

GRZ-1

-200

0

200

400

600

800

1000

1200

-30 -25 -20 -15 -10 -5 0 5

e154Sm

e 150

Sm

Binary mixing of Mo-Ru nucleosynthetic components

Binary mixing of Mo-Ru nucleosynthetic components

Dauphas (2004)

Binary mixing of s- and r-process Os componentsBinary mixing of s- and r-process Os components

Yokoyama et al. (2007) Humayun and Brandon (2007)

Pre-solar grains and predictionsPre-solar grains and predictions

Lugaro et al. (2003) Loss of consistency for different elements

There is more than binary mixing

Issues: Issues:

•Do nucleosynthetic components have discrete isotopic properties?

•How many components are needed to account observations (deconvolution)?

•Which mineral or organic phases are the carriers?

II Field shiftII Field shift

Nuclear field shiftNuclear field shifta.k.a.

Nuclear field shifteffect of nuclear charge radius

Nuclear field shifteffect of nuclear charge radius

Point-chargeapproximation

Breit (1958)

Nuclear field shift:effect of nuclear shape

Nuclear field shift:effect of nuclear shape

4.80

4.85

4.90

4.95

5.00

5.05

5.10

142Nd 144Nd 146Nd 148Nd 150Nd

nu

clea

r ch

arg

e ra

diu

s (f

m)

0.00

0.05

0.10

0.15

0.20

0.25

0.30

qu

adrip

olar d

eform

ation

b2

Bigeleisen’s (1996) formulation of mass fractionation

is the difference in nuclear charge radii between nuclei of mass m and m’, A and B are constants

2δ r

mass independent 1/T mass dependent 1/T2

Temperature dependence of isotope fractionation between U(IV) and U(VI)Temperature dependence of isotope

fractionation between U(IV) and U(VI)

Bigeleisen (1998)

Mass-independent fractionation remains after

internal normalization!

Sites: gas-dust interaction

Evidence of non-mass dependent fractionation experiment between crown-ether and acid solution

Evidence of non-mass dependent fractionation experiment between crown-ether and acid solution

Fujii et al. (2006)

Further evidence from elution on ion-exchange resins

Levins et al.(1999)

Hfnuclear charge radii increase

smoothly

Campbell et al. (1997)

Zr: deformation of nucleus increases past the neutron closed-shell (N=50)

N=50

Odd-even staggering of Sn nuclear properties

Suggests using even-even or odd-odd for normalization!

1

10

100

1000

112Sn 113Sn 114Sn 115Sn 116Sn 117Sn 118Sn 119Sn 120Sn 121Sn 122Sn 124Sn 125Sn

neu

tro

n c

ross

-sec

tio

n (

fm)

4.58

4.6

4.62

4.64

4.66

4.68

4.7

nu

clear charg

e radiu

s (fm)

Odd-even staggering of nuclear massesOdd-even staggering of nuclear masses

-40

-30

-20

-10

0

10

20

30

58 59 60 61 62 63 64

Mi/(

Mi-

1 -

Mi+

1) -

1 (

pp

m)

Ni

Begs the question of which process control mass fractionation

Test for an effect of nuclear field shiftTest for an effect of nuclear field shift

ar

mmm

mmmr mm

i

immm ii

e211 ,

2

12

12,

2

1m

mi1

2

m

minternally normalized to

Fujii et al. (2006)

3.62

3.63

3.64

3.65

3.66

3.67

3.68

3.69

50Cr 52Cr 53Cr 54Crnu

clea

r ch

arge

rad

ius

(fm

)

Mo isotopes in carbonaceous chondrites

Mo isotopes in carbonaceous chondrites

Fujii et al. (2006)

The origin of the 54Cr anomaly

The origin of the 54Cr anomaly

1.0

10.0

100.0

1000.0

50Cr 52Cr 53Cr 54Cr

3.62

3.63

3.64

3.65

3.66

3.67

3.68

3.69

nu

clear charg

e radiu

s (fm)

10

15

20

25

30

40

50

60

80

100

Trinquier et al. (2006)T

σ

Neutron cross-sections do not separate 54Cr from 52Cr, nuclear field shift does

Extraction experiments(Fujii et al, 2002)

50

52

53

54

III Analytical issues(or the limits of mass-dependent fractionation)

III Analytical issues(or the limits of mass-dependent fractionation)

Chen et al. (2003)

Correction for analytical and instrumental mass bias assumes constant isotopic abundances

Anomalous behavior of 125TeAnomalous behavior of 125Te

Moynier et al. (2006) Fehr et al.’ (2006) data renormalization

100

1000

10000

180W 182W 183W 184W 186W

T1/

2

5.30

5.31

5.32

5.33

5.34

5.35

5.36

5.37

5.38

nu

clear charg

e radiu

s (fm)

100

1000

10000

T1/

2

5.33

5.34

5.35

5.36

5.37

5.38

5.39

5.4

5.41

5.42

nu

clear chag

e radiu

s

Risky normalisation (odd/even ratio)

Also 61Ni

Pb: the double closed shell at mass 208(Z=82, N=126)

Pb: the double closed shell at mass 208(Z=82, N=126)

0.1

1

10

100

1000

204Pb 206Pb 207Pb 208Pb

T1/

2

5.465

5.470

5.475

5.480

5.485

5.490

5.495

5.500

5.505

nu

clear ch

arge rad

ius (fm

)

10

15

20

25

30

40

50

60

80

100

5.460

5.465

5.470

5.475

5.480

5.485

5.490

5.495

5.500

5.505

202 204 205 206 207 208

nu

cle

ar

ch

arg

e r

ad

ius

(fm

)Odd-even staggering of Pb isotopes

(extended spectrum)Odd-even staggering of Pb isotopes

(extended spectrum)

Sakakihara et al. (2001)

Analytical mass fractionation Odd-even staggering and

instrumental bias

Analytical mass fractionation Odd-even staggering and

instrumental bias

Blichert-Toft et al. (2003) Doucelance et al. (2001)

PbPb

ConclusionsConclusions

• The number of nucleosynthetic components needs to be more rigorously evaluated

• The strength of the nuclear field shift effect w.r.t. nucleosynthetic anomalies still unclear

• Odd-even staggering of nuclear properties is ubiquitous and its cause is multiple: neutron cross-sections, nuclear field radii, and masses

MoMo

SmSm

100

1000

10000

100000

T1

/2

4.85

4.90

4.95

5.00

5.05

5.10

5.15

nu

clear charg

e radiu

s (fm)

5

10

15

20

25

30

40

50

60

80

100

SmSm

-800

-600

-400

-200

0

200

400

600

800

1000

1200

e Sm

i

GRZ-1

15555

Gladstone

Homestead

Peace

Ucera

Indarch

Orgueil

Mighei

Murray

Allende

Grosnaja

Mokoia

Carlson et al. (2007)

r-process nuclide abundancesr-process nuclide abundances

Arnould et al. (2007)

MoMo

100

1000

10000

92Mo(p) 94Mo(p) 95Mo(s,r) 96Mo(s) 97Mo(s,r) 98Mo(s,r) 100Mo(r)

T1

/2

4.25

4.30

4.35

4.40

4.45

4.50

nu

clear charg

e radiu

s (fm)

10

15

20

25

30

40

50

60

80

100

Series11

Mo isotopic anomalies in carbonaceous chondritesMo isotopic anomalies in carbonaceous chondrites

Orgueil

Allende

Dauphas et al. (2002)

Yin et al. (2002)

Meteorites vs pre-solar grainsMeteorites vs pre-solar grains

Dauphas et al. (2004)

Nicolussi et al. (1998)

MoMo

100

1000

10000

92Mo(p) 94Mo(p) 95Mo(s,r) 96Mo(s) 97Mo(s,r) 98Mo(s,r) 100Mo(r)

T1

/2

4.25

4.30

4.35

4.40

4.45

4.50

nu

clear ch

arge rad

ius (fm

)

10

15

20

25

30

40

50

60

80

100

Series11

SiC: Pellin et al. (1999)

Os: normalization to 189 is risky too

100

1000

10000

184Os(p) 186Os(s) 187Os(s,p) 188Os(r,s) 189Os(r) 190Os(r,s) 192Os(r)

T1/

2

5.33

5.34

5.35

5.36

5.37

5.38

5.39

5.4

5.41

5.42

nu

clear chag

e radiu

s

10

15

20

25

30

40

50

60

80

100

SmSm

100

1000

10000

100000

T1

/2

4.85

4.90

4.95

5.00

5.05

5.10

5.15

nu

clear charg

e radiu

s (fm

)

5

10

15

20

25

30

40

50

60

80

100

Nd may help telling NFS from (s,r) mixingNd may help telling NFS from (s,r) mixing

10

100

1000

10000

142Nd(s) 143Nd(r,s) 144Nd(s,r) 145Nd(r,s) 146Nd(s,r) 148Nd(r,s) 150Nd(r)

T1

/2

4.80

4.85

4.90

4.95

5.00

5.05

5.10

nu

clear charg

e radiu

s (fm)

5

10

15

20

25

30

40

50

60

80

100

0.612

0.614

0.616

0.618

0.620

0.622

0.624

0.626

0.628

4.535 4.540 4.545 4.550 4.555 4.560 4.565 4.570 4.575

Age (Ga)

20

7P

b*/

20

6P

b*

The devil is in the details: precision is not the main issue of U-Pb

chronology but odd-even staggering

The devil is in the details: precision is not the main issue of U-Pb

chronology but odd-even staggering