Influence of chemical bonds on the lifetime of the molecular-field-split 2p levels in H2S
Bueno, AM ; de Brito, AN ; Fink, RF ; Bassler, M LU ; Bjorneholm, O ; Burmeister, F ; Feifel, R ; Miron, C ; Ristinmaa Sörensen, Stacey LU
and Wang, HH
, et al.
(2003)
In Physical Review A (Atomic, Molecular and Optical Physics)
67(2).
- Abstract
- Different lifetime broadenings in molecular-field-split 2p core levels in H2S are predicted theoretically and are identified in an experimental investigation of the S 2p Auger electron spectrum. The measurements were performed for the transition to the vibrationally resolved X(1)A(1) ground state of H2S2+. The lifetimes of the 3e(1/2) and 5e(1/2) levels of the 2p ionized molecule are found to be 64 and 74 meV, respectively. This unambiguous determination of the lifetime difference of 10+/-1 meV is only possible as the 4e(1/2)-->X(1)A(1)(2b(1)(-2)) decay channel that overlaps the 5e(1/2)-->X(1)A(1)(2b(1)(-2)) channel is practically suppressed in Auger decay in H2S. The lifetime difference is confirmed by ab initio calculations. A... (More)
- Different lifetime broadenings in molecular-field-split 2p core levels in H2S are predicted theoretically and are identified in an experimental investigation of the S 2p Auger electron spectrum. The measurements were performed for the transition to the vibrationally resolved X(1)A(1) ground state of H2S2+. The lifetimes of the 3e(1/2) and 5e(1/2) levels of the 2p ionized molecule are found to be 64 and 74 meV, respectively. This unambiguous determination of the lifetime difference of 10+/-1 meV is only possible as the 4e(1/2)-->X(1)A(1)(2b(1)(-2)) decay channel that overlaps the 5e(1/2)-->X(1)A(1)(2b(1)(-2)) channel is practically suppressed in Auger decay in H2S. The lifetime difference is confirmed by ab initio calculations. A theoretical analysis shows that it results from the mutual orientation of the core hole in the intermediate states and the valence electron density in the sulfur 3p orbitals. Both are strongly influenced by the chemical bond. Thus the observed effect is the direct result of a fundamental property of molecular electronic structure. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/908848
- author
- Bueno, AM
; de Brito, AN
; Fink, RF
; Bassler, M
LU
; Bjorneholm, O
; Burmeister, F
; Feifel, R
; Miron, C
; Ristinmaa Sörensen, Stacey
LU
and Wang, HH
, et al. (More)
- Bueno, AM
; de Brito, AN
; Fink, RF
; Bassler, M
LU
; Bjorneholm, O
; Burmeister, F
; Feifel, R
; Miron, C
; Ristinmaa Sörensen, Stacey
LU
; Wang, HH
and Svensson, S
(Less)
- organization
- publishing date
- 2003
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Physical Review A (Atomic, Molecular and Optical Physics)
- volume
- 67
- issue
- 2
- article number
- 022714
- publisher
- American Physical Society
- external identifiers
-
- wos:000181361200071
- scopus:0038301321
- ISSN
- 1050-2947
- DOI
- 10.1103/PhysRevA.67.022714
- language
- English
- LU publication?
- yes
- id
- 4a715d6f-73fa-416a-841e-18af25e01763 (old id 908848)
- date added to LUP
- 2016-04-01 11:37:04
- date last changed
- 2024-01-07 14:06:58
@article{4a715d6f-73fa-416a-841e-18af25e01763,
abstract = {{Different lifetime broadenings in molecular-field-split 2p core levels in H2S are predicted theoretically and are identified in an experimental investigation of the S 2p Auger electron spectrum. The measurements were performed for the transition to the vibrationally resolved X(1)A(1) ground state of H2S2+. The lifetimes of the 3e(1/2) and 5e(1/2) levels of the 2p ionized molecule are found to be 64 and 74 meV, respectively. This unambiguous determination of the lifetime difference of 10+/-1 meV is only possible as the 4e(1/2)-->X(1)A(1)(2b(1)(-2)) decay channel that overlaps the 5e(1/2)-->X(1)A(1)(2b(1)(-2)) channel is practically suppressed in Auger decay in H2S. The lifetime difference is confirmed by ab initio calculations. A theoretical analysis shows that it results from the mutual orientation of the core hole in the intermediate states and the valence electron density in the sulfur 3p orbitals. Both are strongly influenced by the chemical bond. Thus the observed effect is the direct result of a fundamental property of molecular electronic structure.}},
author = {{Bueno, AM and de Brito, AN and Fink, RF and Bassler, M and Bjorneholm, O and Burmeister, F and Feifel, R and Miron, C and Ristinmaa Sörensen, Stacey and Wang, HH and Svensson, S}},
issn = {{1050-2947}},
language = {{eng}},
number = {{2}},
publisher = {{American Physical Society}},
series = {{Physical Review A (Atomic, Molecular and Optical Physics)}},
title = {{Influence of chemical bonds on the lifetime of the molecular-field-split 2p levels in H2S}},
url = {{http://dx.doi.org/10.1103/PhysRevA.67.022714}},
doi = {{10.1103/PhysRevA.67.022714}},
volume = {{67}},
year = {{2003}},
}