论文标题
脉冲重叠的歧义性多量子相干光谱法
Pulse overlap ambiguities in multiple quantum coherence spectroscopy
论文作者
论文摘要
相干的二维电子光谱法使用飞秒脉冲探测超快动力学。如果研究动力学的时间尺度与脉搏持续时间相当，则脉冲重叠效应可能会损害实验数据。在这里，我们执行一维相干扫描并研究清洁两级系统中的脉冲重叠效应。我们发现由于时间脉冲重叠期间的任意时间排序，寄生虫多量子相干信号。令人惊讶的是，信号寿命超过了时间脉冲重叠1.8倍。这些发现对解释高阶相干二维和相关光谱实验具有重要意义。
Coherent two-dimensional electronic spectroscopy probes ultrafast dynamics using femtosecond pulses. In case the timescale of the studied dynamics become comparable to the pulse duration, pulse overlap effects may compromise the experimental data. Here, we perform one-dimensional coherence scans and study pulse overlap effects in clean two-level systems. We find parasitic multiple-quantum coherence signals as a consequence of the arbitrary time ordering during the temporal pulse overlap. Surprisingly, the signal lifetimes exceed the temporal pulse overlap by a factor of 1.8. These findings have important implications for the interpretation of higher-order coherent two-dimensional and related spectroscopy experiments.
