Egorova Dassia, Gelin Maxim F, Domcke Wolfgang
Department of Chemistry, Technical University of Munich, D-85747 Garching, Germany.
J Chem Phys. 2007 Feb 21;126(7):074314. doi: 10.1063/1.2435353.
The recently developed efficient method for the calculation of four-wave mixing signals [M. F. Gelin et al., J. Chem. Phys. 123, 164112 (2005)] is employed for the calculation of two-dimensional electronic photon-echo spectra. The effect of the explicit treatment of vibrations coupled to the electronic transitions is systematically analyzed. The impact of pulse durations, optical dephasing, and temperature on the spectra is investigated. The study aims at an understanding of the mechanisms which may give rise to cross peaks in the two-dimensional electronic spectra and at clarifying the conditions of their detection.
最近开发的用于计算四波混频信号的高效方法[M. F. 格林等人,《化学物理杂志》123, 164112 (2005)]被用于计算二维电子光子回波光谱。系统地分析了与电子跃迁耦合的振动的显式处理的影响。研究了脉冲持续时间、光学退相和温度对光谱的影响。该研究旨在理解可能导致二维电子光谱中出现交叉峰的机制,并阐明检测这些交叉峰的条件。