T. Kib è di , B.Q. Lee, A.E. Stuchbery , K.A. Robinson (ANU) F.G. Kondev (ANL)

Atomic radiations in nuclear decayDevelopment of a new code to

incorporate atomic data into ENSDF

T. Kibèdi, B.Q. Lee, A.E. Stuchbery, K.A. Robinson (ANU)F.G. Kondev (ANL)

Tibor Kibèdi, Dep. of Nuclear Physics, Australian National University 20th NSDD, Kuwait, 27 – 31 January 2013


Outline

Motivation Radiative and Non-radiative atomic transitions in nuclear

decay Nuclear and atomic data Existing programs to evaluate atomic radiations New model based on Monte Carlo approach Future directions

BackgroundKálmán Robertson (ANU) Honours project (2010)

Boon Quan Lee (ANU) Honours project (2012)2012Le09 Lee et al., “Atomic Radiations in the Decay of Medical Radioisotopes: A Physics Perspective”Comp. Math. Meth. in Medicine, v2012, Article ID 651475, doi:10.1155/2012/651475

2011 NSDD meeting (IAEA)


Medical applications - Auger electrons

Regaud and Lacassagne (1927)“The ideal agent for cancer therapy would consist of heavy elements capable of emitting radiations of molecular dimensions, which could be administered to the organism and selectively fixed in the protoplasm of cells one seeks to destroy.”

Antoine Lacassagne (1884-1971)

Claudius Regaud (1870-1940)



(Courtesy of Thomas Tunningley, ANU).

Targeted tumor therapy


Antoine Lacassagne (1884-1971)

Claudius Regaud (1870-1940)




electrons

Biological effect: Linear energy transfer LET,

keV/mm

Kassis, Int. J. of Rad. Biol, 80 (2004) 789





2011 August, INDC International Nuclear Data Committee

Technical Meeting on Intermediate-term Nuclear Data Needs for Medical Applications: Cross Sections and Decay DataEd. by A.L. Nichols, et al., NDC(NDS)-0596

Auger emitters: 67Ga , 71Ge, 77Br, 99mTc, 103Pd, 111In, 123I, 125I, 140Nd, 178Ta, 193Pt, 195mPt, 197Hg





Atomic radiations - Basic concept

1S

2S2P

3S3P

3D

K

L1

L2

L3

M1

M2

M3

M4

M5

Initial vacancy

X-ray emission

X-ray

photon

Ka2 X-ray1 secondary

vacancy

22 LKX EEEK

a



K

L1

L2

L3

M1

M2

M3

M4

M5

Auger-electron

Auger-

electron

23232

LLLKLLK EEEE

K L2 L3 Auger-electron2 new secondary

vacancies

1S

2S2P

3S3P

3D

K

L1

L2

L3

M1

M2

M3

M4

M5

Initial vacancy

X-ray emission

X-ray

photon

Initial vacancy

Ka2 X-ray1 secondary vacancy

22 LKX EEEK

a



K

L1

L2

L3

M1

M2

M3

M4

M5

Coster-Kronig electron

CK- electro

n

2121121

LMLLMLL EEEE

L1 L2 M1 Coster-Kronig transition

2 new secondary vacancies

1S

2S2P

3S3P

3D

K

L1

L2

L3

M1

M2

M3

M4

M5

Initial vacancy

X-ray emission

X-ray

photonInitial

vacancy

22 LKX EEEK

a

Ka2 X-ray1 secondary vacancy


Atomic relaxation and vacancy transfer

Vacancy cascade in Xe Full relaxation of an initial inner

shellvacancy creates vacancy cascade involving X-ray (Radiative) and Auger as well as Coster-Kronig (Non-Radiative) transitions

Many possible cascades for a single

initial vacancyTypical relaxation time ~10-15

secondsMany vacancy cascades

following a single ionisation event!

K

O1,2,3

L1

L2

L3

M1

M2

M3

M4,5

N1

N2,3

N4,5

X

AA

AAA

KC

AAAAAAAA

Initial vacancy

M.O. Krause, J. Phys. Colloques, 32 (1971) C4-67



Vacancies on the inner-shell can be produced by electron impact photo ionization ion-atom collision internal conversion electron capture secondary processes

accompanyingb-decay or electron capture

Vacancy cascade in Xe

K

O1,2,3

L1

L2

L3

M1

M2

M3

M4,5

N1

N2,3

N4,5

X

AA

AAA

KC

AAAAAAAA

M.O. Krause, J. Phys. Colloques, 32 (1971) C4-67


Motivation

X-ray and Auger electron spectrum is an integral part of the radiations emitted in nuclear decay

Atomic radiations are important for applications of radioisotopes (medical physics, nuclear astrophysics, nuclear engineering)

ENSDF: atomic radiations are not included


Atomic transition energies and rates

Basic formulas For a single initial vacancy on the K-shell following nuclear decay Number of primary vacancies T

KK Pn

aa

1Internal conversion

Electron captureKK PPn

X-ray emission

Energy YKX EEEKY

Intensity KKX nIKY

for L1 shell 111 LLX nIYL

Auger-electron

XYXKKXY EEEE

KKKXY anI 1 KK a

)( 312111 LLLLLKXYL ffanI

1312111 LLLLLL ffa

in an ion


Existing calculationsPhysical approach

RADAR DDEP Eckerman & Endo(2007)

Howell(1992)

Stepanek(2000)

Pomplun(2012)

Nuclear decay data

ENSDF DDEP ENSDF ENSDF ENSDF ICRP38

Conversion coefficients

HsIcc RpIcc/BrIcc RpIcc,1978 Band

RpIcc 2000 Stepanek HsIcc,1971 Dragoun,

1976 Band

Electron Capture Ratios

1971 Gove & Martin

1995 Schönfeld 1977 Bambynek 1971 Gove & Martin,

1970Martin

1971 Gove & Martin,

1970Martin

1971 Gove & Martin

Atomic transition rates

1972 Bambynek,RADLST

1974 Scofield,1995 Schönfeld

& Janßen,2006 Be et al.,

EMISSION

1991 Perkins,EDISTR04

1979 Chen,1972/1975 McGuire,

1983 Kassis, 1974 Scofield, 1974

Manson & Kenedy

1991 Perkins 1979 Chen,1972/1975

McGuire, 1970 Storm & Israel, 1979 Krause

Atomic transition energies

1970 Bearden & Burr, Neutral

atom

1977 Larkins,Semi-empirical

1991 Perkins, Neutral atom

Z/Z+1 (Auger),Neutral atom (X-

ray)

Dirack-Fock calculation

1991 Desclaux, Dirack-Fock calculation

Vacancy propagation

Deterministic Deterministic Deterministic(+++)

Monte Carlowith charge

neutralization

Monte Carlo Monte Carlo


Existing calculationsAuger electron yield per nuclear

decayRADAR DDEP Eckerman &

Endo(2007)

Howell(1992)

Stepanek(2000)

Pomplun(2012)

99mTc (6.007 h) 0.122 0.13 4.363 4.0 2.5

111In (2.805 d) 1.136 1.16 7.215 14.7 6.05

123I (13.22 h) 1.064 1.08 13.71 14.9 6.4

125I (59.4 d) 1.77 1.78 23.0 24.9 15.3 12.2

201Tl (3.04 d) 0.773 0.614 20.9 36.9

Vacancy propagation

Deterministic Deterministic Deterministic(+++)

Monte Carlowith charge

neutralization

Monte Carlo Monte Carlo


Existing programs

Common problems / limitations In some cases neutral atom binding energies are used for atoms with

vacancies; i.e. for ions

Single initial vacancy is considered. Secondary vacancies are ignored

Atomic radiations only from primary vacancies on the K and L shell

Limited information on sub-shell rates

Auger electrons below ~1 keV are often omitted


BrIccEmis – Monte Carlo approach for vacancy creation and

propagation Initial state: neutral isolated atom

Nuclear structure data: from ENSDF

Electron capture (EC) rates: Schönfeld (1998Sc28)

Internal conversion coefficients (ICC): BrIcc (2008Ki07)

Auger and X-ray transition rates: EADL (1991 Perkins)

Calculated for single vacancies!

Auger and X-ray transition energies: RAINE (2002Ba85)

Calculated for actual electronic configuration!

Vacancy creation and relaxation from EC and IC: treated independently

Ab initio treatment of the vacancy propagation: Transition energies and rates evaluated on the spot

Propagation terminated once the vacancy reached the valence shell


BrIccEmis

Reads the ENSDF file, evaluates absolute decay intensities of EC, GAMMA, CE and PAIR transitions

Simulates a large number events: 100k-10M radioactive decays followed by atomic relaxation

Electron configurations and binding energies stored in memory (and saved on disk). New configurations only calculated if needed!

(55Fe: 15 k, 201Tl: 1300k)

Emitted atomic radiations stored on disk (~Gb files)

Separate files for X-rays and Auger electrons

Smaller programs to sort/project energy spectra, produce detailed reports


111In EC – vacancy propagation


99mTc atomic radiations

below L-shell BE


99mTc atomic radiations – X-rays

DDEP BrIccEmisKa1 18.3672

4.21E-218.4214.05E-2

Ka2 18.2512.22E-2

18.3022.13E-2

Kb 20.6771.30E-2

20.7291.18E-2

L [2.134:3.002]4.82E-3

2.4664.72E-3

M 0.2637.83E-4

N 0.0478.73E-1


BrIccEmis: 10 M simulated decay events 455 type of Auger transitions 1981Ge05: measured Auger electrons

in 1500-2300 eV only

99mTc Auger electrons

2012Le09 Lee et al., Comp. Math. Meth. in Medicine, v2012, Art. ID 651475 B.Q. Lee, Honours Thesis, ANU 2012

Low energy Auger electrons


99mTc atomic radiations – Auger electrons

DDEP BrIccEmis

KLL [14.86:15.58]1.49E-2

15.371.48E-2

KLX [17.43:18.33]2.79E-3

17.855.58E-3

KXY [19.93:21.00]2.8E-4

20.275.07E-4

K-total2.15E-2

16.152.08E-2

CK LLM 2.08E-20.054

CK LLX 0.1449.48E-3

LMM 2.0169.02E-2

LMX 2.3281.41E-2

LXY 2.6546.07E-4

L-total [1.6:2.9]1.089E-1

1.7651.24E-1


99mTc atomic radiations – Auger electrons

DDEP BrIccEmis

CK MMX 0.1047.10E-1

MXY 0.1701.10E+0

Super CK NNN 0.0145.36E-1

CK NNX 0.0128.45E-1

Total yield Auger electron per nuclear decay 0.13 3.37

~95% below 500

eV


131mXe IT – charge state at the end of atomic relaxation

Only a handful of measurements exist for ionization by nuclear decay

131mXe: F. Pleasonton, A.H. Snell, Proc. Royal Soc. (London) 241 (1957) 141

37Ar: A.H. Snell, F. Pleasonton, Phys. Rev. 100 (1955) 1396

Good tool to asses the completeness of the vacancy propagation

BrIccEmis: mean value is lower by ~0.7-1.0 charge


111In – experiment vs calculation

E.A. Yakushev, et al., Applied Radiation and Isotopes 62 (2005) 451

• ESCA; FWHM = 4 eV• Calculations normalized to the strongest experimental line


111In – experiment vs calculation

A. Kovalik, et al., J. of Electron Spect. and Rel. Phen. 105 (1999) 219• ESCA; FWHM = 7 eV• Calculated energies are higher• KL2L3(1D2) energy (eV):

• Multiplet splitting could not be reproduced in JJ coupling scheme

• Similar discrepancies have been seen in other elements (Z=47, Kawakami, Phys. Lett A121 (1987) 414)

19319.2(14) Experiment Kovalik (1999)

19308.1 Semi-empirical Larkins (1979La19)

19381 RAINE (2002Ba85)

DE≈60 eV!


Breit and other QED contributions (2002Ga47)

Z=49 (In)~60 eV

Alternative solution:Semi empirical corrections, like Larkins (1977La19) or Carlson (1977Ca31) used

Gaston et al. Phys. Rev A66 (2002) 062505


Summary – Program developments

BrIccEmis: calculation intensive approach (hours to days) RelaxData (under development):

Nuclear decay event (EC or CE) produces a SINGLE INITIAL vacancy

Considering a single atomic vacancy the relaxation process independent what produced the vacancy

Compile a database of atomic radiation spectra for produced by a single initial vacancy on an atomic shell Carry out calculations of all elements and shells

Example: 55Fe EC, 7 shells for Z=25 and 26, calculated in couple of hours (1 M each shell)

Replace EADL fixed rates and binding energies from RAINE with GRASP2k/RATIP calculations

BrIccRelax (under development): Evaluate primary vacancy distribution and construct atomic spectra from the data base (20 seconds for 55Fe EC)


Inclusion of atomic relaxation data into ENSDF

Comment X-rays Auger electronsNotation: from IUPAC

• International Union of Pure and Applied Chemistry

• Based on initial and final atomic levels involved

K-L3 K-L1-L2

Group sub-shells to reduce number of transitions

• Summed decay rates• Use the mean transition energy for the group

L (for L1-M2, … L3-O4)

But not for KKa1 for K-L3

Ka2 for K-L2

Kb for K-M3&K-M2

KLL(for K-L1-L1, … K-L3-L3)

KLX (X=M1….,N1….)

KXY (X&Y=M1….,N1….)


Inclusion of atomic relaxation data into ENSDF

ENSDF coding: TRANSITION=ENERGY [INTENSITY] 99TC R XKA1=23.25 [0.451]$ XKA2=23.06 [0.239]$ XKB=26.26 [0.142]$ 99TC1 R XL=3.23 [6.90e-2]$ XM=0.424 [0.254]$XN=0.0477 [1.03]$ 99TC2 R AKLL=19.23 [0.107]$ AKLX=22.46 [4.39E-2]$ AKXY=25.64 [4.29E-3]$ 99TC3 R ALLM=0.032 [4.82E-2]$ ALLX=0.234 [0.132]$ ALMM=2.58 [0.816]$ 99TC4 R ALMX=3.06 [0.188]$ ALXY=3.54 [1.13E-2]$ AMMX=0.098 [0.859]$ 99TC5 R AMXY=0.308 [2.12]$ ANNN=0.020 [0.538]$ ANNX=0.017 [0.681]$ 99TC6 R ANXY=0.054 [0.206] 99TC L 0 9/2+ Before daughter GS level record

Intensity need to be normalised to GAMMA-rays; same normalisation is valid for both

Number of entries on the “R” (RELAXATION) records can automatically generated according to Z

Detailed spectra (list or figure) of the X-rays and Auger electrons can be generated and distributed for the user

X-rays

Auger electrons

Documents

T. Kib è di , B.Q. Lee, A.E. Stuchbery , K.A. Robinson (ANU) F.G. Kondev (ANL)