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Pressure- and chemistry-dependent electron-capture-decay in crystalline solids. Kanani K. M. Lee 1,2 Gerd Steinle-Neumann 2 1 Department of Physics, New Mexico State University, Las Cruces, NM, USA. 2 Bayerisches Geoinstitut – Universität Bayreuth. Radioactive decay. Dating of rocks - PowerPoint PPT Presentation
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Kanani K. M. Lee1,2
Gerd Steinle-Neumann2 1Department of Physics, New Mexico State University, Las Cruces, NM, USA.2Bayerisches Geoinstitut – Universität Bayreuth.
Pressure- and chemistry-dependent
electron-capture-decay in crystalline solids
Radioactive decay
Dating of rocks (235U, 238U, 232Th, 40K, 87Rb)
Heat dynamics (235U, 238U, 232Th, 40K)
Mostly α decay (U, Th)
40K decays by β+ (89%) and electron capture (11%) (emission of γ ray)
Other electron capture isotopes: 7Be, 22Na, 26Al, 53Mn
β-, there is also β+
Radioactive decay
Radioactive decay nuclear process, hence independent on environment:
true for α and β processes (on fundamental grounds but also measured)
electron capture ~ charge density at nucleus
here 7Be (τ½=53 days)22Na (τ½=2.6 years, τ½,EC=27.7 years)40K (τ½=1.25 Gyr, τ½,EC =11.9 Gyr)
dependence on chemistry and pressure (decay constant λ~1/τ½)
refecrefe
eec ,
,
1
Energetics of a solid
Schrödinger's equation [-2+V]Ψ(r1,r2,...,rN)=EΨ(r1,r2,...,rN)
Density Functional Theory (Kohn et al., 1964 ff.):electronic charge density ρ is basic quantity[- 2+VKS[ρ]]ψi(ρ)= eiψi (ρ)
VKS[ρ]= Vne+Vee+Vxc
Static computations:
Thermal excitations (and zero point motion) neglected.Use full periodicity of the lattice.
7Be chemistry
Experiments: λ[Be(OH2)42+]>λ[Be]>λ[BeO]>λ[BeF2] [Johlige et al., 1970]
Our computations: λ[Be]>λ[BeO]>λ[BeCl2]
7Be pressure
1.0
0.8
0.6
0.4
0.2
0.0
perc
ent
diff
ere
nce
, ec
50403020100
Pressure (GPa)
Be, hcp BeO, hcp BeCl2, orth
Gogarty et al., 1963 Hensley et al., 1973 Liu & Huh, 2000
40K pressure
0.02
0.01
0.00
perc
en
t d
iffere
nce
, ec
50403020100
Pressure (GPa)
K, bcc K, fcc K2O, fcc
KCl, B1 KCl, B2
5395.0
5394.5
5394.0
5393.5
tota
l ele
ctro
n c
harg
e d
ensi
ty,
e80604020
Volume (Å3)
1.0
0.8
0.6
0.4
0.2
0.0
num
ber o
f d-o
rbita
l ele
ctrons
05102550Pressure (GPa)
22Na pressure
0.3
0.2
0.1
0.0
nu
mb
er o
f d-o
rbita
l ele
ctron
s
40302010
Volume (Å3)
893
892
891
890
889
888
tota
l ele
ctro
n c
harg
e d
en
sity
, e
010251001000
Na, fcc total electron density 4th-order polynomial fit d-orbital occupancy
Pressure (GPa)
0.14
0.12
0.10
0.08
0.06
0.04
0.02
0.00
perc
en
t d
iffere
nce
, ec
100806040200Pressure (GPa)
Na, bcc Na, fcc NaCl, B1 NaCl, B2 Na2O, fcc
Conclusions
Using first principles computations for the electronic charge density of electron capture isotopes we
reproduce the chemical dependence of λ for 7Be in various chemical forms can not confirm the strong P dependence of λ for 7Be find small P dependence of λ for 22Na and 40K see transition in electronic state (s d) for 22Na and 40K
Changes in λ for alkalines are small, are they measurable (γ rays)?
22Na: ~32 billion decays/day40K: ~40 decays/day
22Na available from ORNL as Na(OH) gel
1400
1200
1000
800
600
400
200
0
cou
nts
300025002000150010005000
Energy (keV)
Background measurementsEmpty DAC at GEANIE facility at LANL
1275 keV 22Na
611 keV 137Cs 1461 keV
40K
2615 keV 232Th 208Tl …