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Delayed four-wave-mixing spectroscopy in molecular crystals: A nonperturbative approach

机译:分子晶体中的延迟四波混合光谱:一种非扰动方法

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摘要

The delayed or time-domain four-wave-mixing experiment is treated in the regime of intense near-resonant pulses. The interaction with the radiation during both pump and probe pulses is considered to all powers of the electric field amplitude. Analytical results are obtained for an effective four-level system. These include the dependence of the coherence amplitudes on the ratio of the pump-field intensities when there is a large vibrational discrepancy between ground and excited electronic states and a general solution for the unitary time development during the probe pulse. For the first time, delayed coherent anti-Stokes Raman scattering is detected from highly dilute (10-ppm) guest molecules. Illustrative examples are presented for the system of pentacene in benzoic acid at low temperature. Vibronic-free induction decay and the effect of field inhomogeneity across the beam profile are found to be essential for understanding the observed intensity and spectral distribution of the signal beam in the region of optimum pulse intensity.
机译:延迟或时域四波混频实验是在强烈的近共振脉冲条件下进行的。在泵浦脉冲和探针脉冲期间与辐射的相互作用被认为是电场幅度的所有功率。获得有效四级系统的分析结果。这些包括当基态和激发态电子状态之间存在较大振动差异时,相干振幅对泵浦场强度之比的依赖性,以及探测脉冲期间单位时间发展的一般解决方案。首次从高度稀释的(10-ppm)客体分子中检测到了延迟的相干抗斯托克斯拉曼散射。给出了并五苯在低温下在苯甲酸中的体系的示例性实例。发现无振动感应衰减和整个光束轮廓上的场不均匀性对于理解观察到的最佳脉冲强度区域内信号光束的强度和光谱分布至关重要。

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