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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Fifth-Order Raman Spectroscopy of Excited-State Molecules
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Fifth-Order Raman Spectroscopy of Excited-State Molecules

机译：激发态分子的五阶拉曼光谱

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The fifth-order Raman spectroscopy of S_1 trans-stilbene in solution was demonstrated.A time domain observation of fifth-order Raman scattering was conducted by using ultrashort,tunable UV and visible pulses.A 22-fs UV pulse at 315 nm induced the first vibrational coherence state of the S_1 state.At the time delays of t_1 = 0.173,0.216,0.259,and 2.000 ps,a 17-fs visible pulse at 630 nm transferred the first coherence state to the second vibrational coherence state.The time-evolution of the second coherence state was probed by the other 17-fs visible pulse at 630 nm.Thirteen bands due to the fifth-order Raman scattering were identified in the Fourier transformation spectra of the second coherence in the range of 100-1300 cm~(-1).The intensities and shapes of two bands at 193 and 398 cm~(-1)showed significant t dependence,whereas those of the other 11 bands were insensitive to t_1.The 193-cm~(-1)band was assigned to the depletion of the UV-pump-induced first vibrational coherence(in-plane bending,V_(25)by the first visible pulse.Both stepwise creation of the vibrational coherence of the overtone of the v_(25)mode and the depletion of the first vibrational coherence may have contributed to the 398-cm~(-1)band.The 11 other bands are equivalents of time-resolved spontaneous Raman bands(third-order optical process)of S_1 trans-stilbene.
机译：证明了溶液中S_1反式二苯乙烯的五阶拉曼光谱。使用超短，可调谐的紫外和可见脉冲对时域观察五阶拉曼散射.315 nm的22-fs紫外脉冲诱导了第一振动相干态为S_1状态。在t_1 = 0.173、0.216、0.259和2.000 ps的时间延迟下，一个630 nm的17-fs可见脉冲将第一相干态转换为第二振动相干态。在630 nm处的其他17-fs可见光脉冲探测到第二相干态的峰。在第二相干的傅立叶变换光谱中，在100-1300 cm〜（范围）内识别出了由五次拉曼散射引起的13个谱带。 -1）。在193和398 cm〜（-1）处的两个谱带的强度和形状表现出显着的t 依赖性，而其他11个波段的强度和形状对t_1不敏感.193-cm〜（-1）谱带的强度和形状对t_1不敏感。归因于紫外线泵引起的第一振动相干性的降低由第一可见脉冲产生的弯曲，V_（25）.v_（25）模的泛音的振动相干的逐步创建和第一振动相干的耗尽都可能导致398-cm〜（-1）其他11个波段相当于S_1反二苯乙烯的时间分辨自发拉曼波段（三阶光学过程）。

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