耦合欠阻尼振动的电荷转移系统的线性、三阶和五阶非线性光谱
Linear, third- and fifth-order nonlinear spectroscopy of a charge transfer system coupled to an underdamped vibration
摘要：
研究了欠阻尼振动条件下电荷转移系统中空穴、电子和激子的输运。我们分析了这些过程中的线性和第三和第五阶非线性电子光谱的签名。用数值精确的分层运动方程方法计算了欠阻尼布朗振子的谱密度。我们发现，与单独的激子耦合相比，电子、空穴和激子转移的结合可以产生具有更多结构的非平凡光谱。在二维光谱的等待时间期间所采取的迹线由振动运动主导，并且不直接反映电子、空穴和激子动力学。我们发现，五阶非线性响应是特别敏感的电荷转移过程。三阶2D光谱检测两个相干态之间的相关性，而五阶2D光谱（2D布居谱）在此被设计为检测两个不同时间段期间的激发态之间的相关性。
英文摘要：
We study hole, electron and exciton transport in a charge transfer system in the presence of underdamped vibrational motion. We analyze the signature of these processes in the linear and third-, and fifth-order nonlinear electronic spectra. Calculations are performed with a numerically exact hierarchical equations of motion method for an underdamped Brownian oscillator spectral density. We find that combining electron, hole and exciton transfer can lead to non-trivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a two-dimensional spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifth-order nonlinear response is particularly sensitive to the charge transfer process. While third-order 2D spectroscopy detects the correlation between two coherences, fifth-order 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states during two different time periods.
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