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Pulse overlap ambiguities in multiple quantum coherence spectroscopy

Ulrich BangertLukas BruderFrank Stienkemeier
Jun 2022
摘要
Coherent two-dimensional electronic spectroscopy probes ultrafast dynamicsusing femtosecond pulses. In case the timescale of the studied dynamics becomecomparable to the pulse duration, pulse overlap effects may compromise theexperimental data. Here, we perform one-dimensional coherence scans and studypulse overlap effects in clean two-level systems. We find parasiticmultiple-quantum coherence signals as a consequence of the arbitrary timeordering during the temporal pulse overlap. Surprisingly, the signal lifetimesexceed the temporal pulse overlap by a factor of 1.8. These findings haveimportant implications for the interpretation of higher-order coherenttwo-dimensional and related spectroscopy experiments.
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