TY - JOUR
T1 - Unified description of sequential and coherent contributions to time-resolved spontaneous emission signals
T2 - generalized doorway-window approach
AU - Gelin, M.F.
AU - Egorova, D.
AU - Pisliakov, A.V.
AU - Domcke, W.
PY - 2004/6/21
Y1 - 2004/6/21
N2 - The doorway-window approach for the description of time- and frequency-gated spontaneous emission is extended to the case of overlapping pump and gate pulses, provided one can neglect the transient terms decaying with the characteristic time of the gate pulse. All the transient terms decaying with the characteristic time of the pump pulse, on the other hand, are taken into account. Both the sequential and the coherent contributions to the signal are considered. The comparison of the standard doorway-window approximation with the present more general formulation for a curve-crossing model system reveals that the former is valid for pump-pulse durations up to the order of the vibrational period and becomes qualitatively incorrect for longer pump pulses.
AB - The doorway-window approach for the description of time- and frequency-gated spontaneous emission is extended to the case of overlapping pump and gate pulses, provided one can neglect the transient terms decaying with the characteristic time of the gate pulse. All the transient terms decaying with the characteristic time of the pump pulse, on the other hand, are taken into account. Both the sequential and the coherent contributions to the signal are considered. The comparison of the standard doorway-window approximation with the present more general formulation for a curve-crossing model system reveals that the former is valid for pump-pulse durations up to the order of the vibrational period and becomes qualitatively incorrect for longer pump pulses.
UR - http://www.scopus.com/inward/record.url?scp=2942522994&partnerID=8YFLogxK
U2 - 10.1016/j.cplett.2004.05.018
DO - 10.1016/j.cplett.2004.05.018
M3 - Article
AN - SCOPUS:2942522994
SN - 0009-2614
VL - 391
SP - 234
EP - 242
JO - Chemical Physics Letters
JF - Chemical Physics Letters
IS - 4-6
ER -