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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Line Broadening and Line Shifts in One-and Two-Photon Single-Molecule Spectra
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Line Broadening and Line Shifts in One-and Two-Photon Single-Molecule Spectra

机译：一和二光子单分子光谱中的线展宽和线位移

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摘要

The temperature and laser-power dependent SI -So spectra of single diphenyloctatetraene molecules in n-tetradecane are investigated using one-and two-photon excitation at cryogenic temperatures. Under one- photon excitation, the single-molecule transitions shift to lower frequencies and the line widths increase with increasing temperature while the line shapes are independent of the laser power up to spectral saturation. The experimental data are consistent with the model of thermal activation of a single localphonon. Under two- photon excitation, the transitions shift linearly to lower frequencies with increasing laser power while the lines broaden only weakly; These results are discussed in terms of laser-induced ac-Stark shifts and matrix dynamics. In particular, a bottleneck effect in the thermalization of nonequilibrium phonons is supposed to play an essential role in the observed broadening ~nd shifts. The comparison of one- and two-photonexcitation spectra provides information about the processes that govern the two-photon spectra:
机译：在低温下使用单光子和双光子激发，研究了正十四烷中单个二苯基辛酸八烯分子的温度和激光功率相关的SI -So光谱。在单光子激发下，单分子跃迁转移到较低的频率，并且线宽随着温度的升高而增加，而线的形状与激光功率无关，直至光谱饱和。实验数据与单个局部声子的热活化模型一致。在双光子激发下，随着激光功率的增加，跃迁线性地移至较低频率，而谱线仅微弱地变宽。这些结果将根据激光诱导的ac-Stark位移和矩阵动力学进行讨论。特别是，非平衡声子热化过程中的瓶颈效应在观察到的变宽移中起着至关重要的作用。一光子激发光谱和两光子激发光谱的比较提供了有关控制两光子光谱的过程的信息：

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