首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ultrafast Vibrational Dynamics in a Quasi-One-Dimensional System: Femtosecond Impulsive Excitation of the PtBr(ethylenediamine) Mixed-Valence Linear Chain Complex
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Ultrafast Vibrational Dynamics in a Quasi-One-Dimensional System: Femtosecond Impulsive Excitation of the PtBr(ethylenediamine) Mixed-Valence Linear Chain Complex

机译:一维系统中的超快速振动动力学:飞秒脉冲激发的PtBr(乙二胺)混合价线性链配合物

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摘要

We have used femtosecond impulsive excitation to time-resolve the vibrational motions following the excitation of the optical intervalence charge transfer transition in a quasi-one-dimensional molecular solid, the mixed-valence metal-halide linear chain complex [Pt(en)_2][Pt(en)_2Br_2]·(PF_6)_4 (en = ethylenediamine, C_2H_8N_2). Wavelength-resolved measurements reveal an induced absorption signal assigned to the formation of the self-trapped exciton that is strongly modulated by vibrational wavepacket oscillations originating on both the ground and excited electronic states. The ground-state response, which includes the fundamental chain axis symmetric stretch frequency and its harmonics, is discussed in terms of resonantly enhanced impulsive stimulated Raman excitation of a strongly coupled electron-phonon system.
机译:我们使用飞秒脉冲激发来时间分辨准一维分子固体,混合价金属卤化物线性链络合物[Pt(en)_2]中的光学间隔电荷转移跃迁的激发之后的振动运动。 [Pt(en)_2Br_2]·(PF_6)_4(en =乙二胺,C_2H_8N_2)。波长分辨的测量揭示了归因于自陷激子形成的感应吸收信号,该信号被源于基态和激发态的振动波包振荡强烈调制。讨论了基态响应,其中包括基本链轴对称拉伸频率及其谐波,是根据强耦合电子-声子系统的共振增强型脉冲受激拉曼激发进行讨论的。

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