Self-Analysis of Coherent Oscillations in Time-Resolved Optical Signals
Self-Analysis of Coherent Oscillations in Time-Resolved Optical Signals
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DOI：
10.1021/jp509657u
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发表时间：
2014-11-06
影响因子：
2.9
通讯作者：
Egorova, Dassia
中科院分区：
文献类型：
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作者：
Egorova, Dassia
时间分辨光信号中振荡的具体起源，特别是对于具有非平凡的态间耦合和不可分离的电子-核运动的复杂系统，通常很难确定。在这里，我们证明二维光子回波中的相干振荡能够进行自我分析；他们的跳动图提供了一种工具来区分基态漂白（GSB）、受激发射（SE）和激发态吸收（ESA）对振荡信号分量的贡献。由于 GSB 携带基态相干性信息，而 SE 和 ESA 反映激发态相干性，因此观察到的振荡可以明确地分配给基态或激发态相干运动。这些发现证明对于具有与每个电子状态相关的密集可检测状态流形的系统特别有利。简要讨论了频率分辨（色散）泵浦探针光谱的类似分析。
The specific origin of oscillations in time-resolved optical signals, in particular, for complex systems with nontrivial interstate couplings and nonseparable electron-nuclear motion, is often difficult to assign. Here, we show that coherent oscillations in two-dimensional photon-echo are capable of self-analysis; their beating maps provide a tool to tell apart ground-state bleach (GSB), stimulated emission (SE), and excited-state absorption (ESA) contributions to the oscillatory signal component. Because GSB carries information on ground-state coherence while SE and ESA reflect the excited-state coherence, the observed oscillations can be unambiguously assigned to ground-state or excited-state coherent motion. The findings prove especially advantageous for systems with dense detectable manifolds of states pertaining to each electronic state. An analogous analysis for frequency-resolved (dispersed) pump-probe spectroscopy is discussed briefly.