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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Transient phenomena in time- and frequency-gated spontaneous emission
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Transient phenomena in time- and frequency-gated spontaneous emission

机译：时间和频率门控自发辐射中的瞬态现象

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摘要

The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.
机译：探索了材料动力学模型中的泵浦和门脉冲重叠对时间和频率门控自发发射光谱的影响，该模型考虑了强非绝热和电子振动耦合效应，振动弛豫和光学相移，从而代表了气相或冷凝相中大分子的光致激发态动力学。分别研究了自发发射谱的顺序，相干和门窗贡献的行为。已证明，顺序和相干贡献之间的相互关系对泵浦和门脉冲的载波频率以及光移相速率敏感，从而为实验确定后者提供了可能性。在特定的发射频率下，相干贡献显示出支配频谱。

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