We investigate the dynamics of molecular core–hole decay using dispersed fluorescence from an ionic valence–hole state in N2. A core–hole excited state is created via the N2(1s→1 π*g) transition, and this state electronically autoionizes to the N+2(B 2Σ+u) state. The vibrational branching ratios for the N+2(B 2Σ+u) state are then determined from N+2(B 2Σ+u→X 2Σ+g) fluorescence. Fundamental aspects of core–hole state decay emerge clearly from these measurements. In particular, interference effects due to lifetime broadening of vibrational levels of the core–hole state can be investigated quantitatively using this method. As a result, dispersed fluorescence detection serves as a powerful tool for investigating R‐dependent aspects of molecular core–hole resonances. The experimental results do not agree with predictions based on previous theoretical developments, and possible causes for the discrepancy are discussed.
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1 October 1988
Research Article|
October 01 1988
Vibrationally resolved electronic autoionization of core–hole resonances
E. D. Poliakoff;
E. D. Poliakoff
Department of Chemistry, Boston University, Boston, Massachusetts 02215
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L. A. Kelly;
L. A. Kelly
Department of Chemistry, Boston University, Boston, Massachusetts 02215
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L. M. Duffy;
L. M. Duffy
Department of Chemistry, Boston University, Boston, Massachusetts 02215
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B. Space;
B. Space
Department of Chemistry, Boston University, Boston, Massachusetts 02215
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P. Roy;
P. Roy
Los Alamos National Laboratory, Los Alamos, New Mexico 87545
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S. H. Southworth;
S. H. Southworth
Los Alamos National Laboratory, Los Alamos, New Mexico 87545
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M. G. White
M. G. White
Department of Chemistry, Brookhaven National Laboratory, Upton, New York 11973
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J. Chem. Phys. 89, 4048–4053 (1988)
Article history
Received:
March 03 1988
Accepted:
June 23 1988
Citation
E. D. Poliakoff, L. A. Kelly, L. M. Duffy, B. Space, P. Roy, S. H. Southworth, M. G. White; Vibrationally resolved electronic autoionization of core–hole resonances. J. Chem. Phys. 1 October 1988; 89 (7): 4048–4053. https://doi.org/10.1063/1.454838
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