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Pulse-shaping assisted multidimensional coherent electronic spectroscopy

机译:脉冲整形辅助多维相干电子光谱

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摘要

Understanding nuclear and electronic dynamics of molecular systems has advanced considerably by probing their nonlinear responses with a suitable sequence of pulses. Moreover, the ability to control crucial parameters of the excitation pulses, such as duration, sequence, frequency, polarization, slowly varying envelope, or carrier phase, has led to a variety of advanced time-resolved spectroscopic methodologies. Recently, two-dimensional electronic spectroscopy with ultrashort pulses has become a more and more popular tool since it allows to obtain information on energy and coherence transfer phenomena, line broadening mechanisms, or the presence of quantum coherences in molecular complexes. Here, we present a high fidelity two-dimensional electronic spectroscopy setup designed for molecular systems in solution. It incorporates the versatility of pulse-shaping methods to achieve full control on the amplitude and phase of the individual exciting and probing pulses. Selective and precise amplitude- and phase-modulation is shown and applied to investigate electronic dynamics in several reference molecular systems.
机译:通过用合适的脉冲序列探测它们的非线性响应,对分子系统的核和电子动力学有了很大的了解。此外,控制激励脉冲的关键参数(例如持续时间,序列,频率,极化,缓慢变化的包络或载波相位)的能力导致了各种先进的时间分辨光谱方法。最近,具有超短脉冲的二维电子光谱学已成为越来越流行的工具,因为它可以获取有关能量和相干传递现象,谱线加宽机制或分子络合物中量子相干的信息。在这里,我们介绍一种专为溶液中的分子系统设计的高保真二维电子光谱仪。它结合了脉冲整形方法的多功能性,可以完全控制单个激励和探测脉冲的幅度和相位。显示了选择性和精确的振幅和相位调制,并将其应用于研究多个参考分子系统中的电子动力学。

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