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Wavelength-resolved stimulated photon echoes: Direct observation of ultrafast intramolecular vibrational contributions to electronic dephasing

机译:波长分辨的受激光子回波:超快分子内振动对电子相移的贡献的直接观察

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摘要

Novel wavelength-resolved stimulated photon echo measurements on a dye molecule in solution re presented. Data are simulated within the multimode Brownian oscillator model using the spectral density of de Boeij et al. [J. Phys. Chem. 100, 11806 (1996)] for the same solute-solvent system. For photon echo population times < 50 fs there are considerable differences between the measured and calculated data. Aided by further simulations, we conclude that these discrepancies result from dephasing dynamics of high frequency intramolecular vibrational modes not included in the previously derived spectral density.
机译:提出了对染料分子在溶液中的新型波长分辨激发光子回波测量方法。使用de Boeij等人的频谱密度在多模布朗振荡器模型中模拟数据。 [J.物理化学100,11806(1996)]。对于小于50 fs的光子回波填充时间,在测量数据和计算数据之间存在相当大的差异。借助进一步的模拟,我们得出结论,这些差异是由于移相了先前导出的频谱密度中未包括的高频分子内振动模式的动力学而导致的。

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