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Mossbauer Spectroscopy Applied to Inorganic Chemistry

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Principles and Applications

Philipp Gütlich

Institut für Anorganische Chemie und Analytische Chemie

Acknowledgement

collaboration. P.G.

Introduction

sciences. phenomenaandeffects.

numerous reviews. The purpose of the material shown here is to use schematic representations with the

reader to consult other material for the detail.

References

New York, 1975.

New York, 1968.

McGraw-Hill London-New York, 1973.

Verlag, Berlin-Heidelberg-New York, 1978.

Oxford, 1979

and subsequent volumes.

Rudolf L. MÖSSBAUER

discovers - and receives theNobel Prize in 1961 observation of recoilless nuclear resonant absorption in 191Ir!

Z. Physik, 1958, 151, 124.

Naturwissenschaften, 1958, 45, 538

and For pedagogical reasons the following presentations similar to

Acoustic resonance between two tuning forks with

same frequency fs= fr

Acoustic wave

Sender

Receiver

fSfE fs=fr Z,NEe Eg Ee EgZ,N

Ȗ-rays

Nucleus 1

Nucleus 2

Sender

Receiver

Transmitted Ȗ-rays

E0= EeEg

Excited state

Ground state

Z, NZ, N

Ȗ-rays

emitting atom absorber atom ERER

ER = EȖ2/2mc2

Important:

Elimination of recoil effect

upon emission and absorption of Ȗ-rays!

Recoilless Nuclear Resonance Absorption

and Fluorescence of-Radiation Z,N Z,N

Nucleus in

Ground

State

Nucleus in

Excited

StateEe

Eg

J-EmissionResonance

Absorption

Resonance

Fluorescence

e A nucleus with Z protons and N neutrons in an excited state of energy Eeundergoes transition to the ground state of energy Egby emitting a gamma quantum of energy Ee Eg. The gamma quantum may be absorbed by the nucleus of the same kind (same Z and N) in its ground state, whereby transition to the excited state of energy Eetakes place (resonance absorption). The subsequent transition to the ground state emits a conversion electron e-or a - quantum (resonance fluorescence).

Nuclear Decay Scheme for

57
27Co
EC

I = 5/2

1/2 3/2

136 keV

14,4 keV, ~ 100 ns

270 d
85 %
0

K ernzerfalls-Schem a für

57
27Co
EC 57
26Fe

I = 5/2

1/2 3/2

136 keV

14,4 keV,

~ 100 ns 270 d
85 %

05726Fe

Radioactive 57Co with 270 days halflife, which may be generated in a cyclotron and diffused into a noble metal like rhodium, serves as the electron capture (EC from K-shell, thereby reducing the proton number, from 27 to 26 corresponding to 57Fe) and initially populates the 136 keV nuclear level of 57Fe with nuclear spin quantum number I = 5/2. This excited state decays after ca. 10 ns and populates, with 85 % probability the 14.4 keV level by emitting 122 keV gamma quanta, with 15 % probability the 136 keV level decays directly to the ground state of 57Fe. The 14.4 keV nuclear state has a halflife of ca. 100 ns. Both the halflife and the emitted gamma quanta of 14.4 keV energy are ideally suited for I = 3/2 and I = 1/2 are the nuclear spin quantum numbers of the excited state (14.4 keV) and the ground state, respectively. The internal conversion coefficient (= the number of ejected K-shell electrons for each Ȗ-quantum interacting with the K-shell) is 9.7. PuAm H Li Na K Rb Cs Fr

CaScTiVCrMnFeCoNiCuZnGaGeAsSeBrKr

Be Mg Sr Ba Ra Y La Ac ZrNb HfTa Mo W Tc Re Ru Os RhPd IrPt Ag Au Cd Hg He Ne Ar Xe Rn BCNOF Al In Tl Si Sn Pb P Sb Bi S Te Po Cl I At

CePrNdPmSmEuGdTbDyHoErTmYbLu

ThPaUNpCmCfEsFmMdNoLwBk

IA IIA

IIIBIVBVBVIB VIIBVIIIB

IBIIB

IIIAIVAVAVIA

VIIIA VIIA PuAm

Experimental Resonance Conditions

If EȖ180 keV: Recoil energy ER = EȖ2/2mc2

becomes too large and destroys resonance

Transition energy: EȖ= EaEg

Suitablerange: 5 keV EȖ180 keV

If EȖ5 keV: Complete non-resonance absorption

IsotopeEȖ/keVȽr/(mm s-1)

= 2 ȽnatIgIeĮNatural abundance %Nuclear decay* 57Fe
61Ni
119Sn
121Sb
125Te
127I
129I
149Sm
151Eu
161Dy
193Ir
197Au
237Np
14.41 67.40
23.87
37.15
35.48
57.60
27.72
22.5
21.6
25.65
73.0
77.34
59.54
0.192 0.78 0.626 2.1 5.02 2.54 0.59 1.60 1.44 0.37 0.60 1.87 0.067 1/2 3/2 1/2+ 5/2+ 1/2+ 5/2+ 7/2+ 7/2 5/2+ 5/2+ 3/2+ 3/2+ 5/2+ 3/2 5/2 3/2+ 7/2+ 3/2+ 7/2+ 5/2+ 5/2 7/2+ 5/2 1/2+ 1/2+ 5/2 8.17 0.12 5.12 ~10 12.7 3.70 5.3 ~12 29
~2.5 ~6 4.0 1.06 2.17 1.25 8.58 57.25
6.99 100
nil 13.9 47.8
18.88 61.5
100
nil

57Co(EC 270 d)

61ȕ99 m)

119mSn(IT 50 d)

121mȕ76 y)

125I(EC 60d)

127mȕ109 d)

129mȕ33 d)

149Eu(EC 106 d)

151Gd(EC 120 d)

161Tb(ȕ6.9 d)

193ȕ31 h)

197ȕ18 h)

241Į

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