Efficient Approaches on Vibrationally-resolved Linear and Nonlinear Optical Spectroscopies

来源 :第十二届全国量子化学会议 | 被引量 : 0次 | 上传用户:w897156334
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  The general time-dependent expressions including the mode-mixing and vibronic coupling effects are formulated to calculate one/two-photon absorption,emission,circular dichroism and resonance Raman/hyper-Raman scattering spectroscopies.The developed time-dependent approaches successfully avoid summing over the large number of final vibrational states.With the further help by our recently-developed analytic energy-derivative approaches for the excited states within the framework of time-dependent density functional theory to calculate the electronic structure parameters such as,the excited-state geometries,harmonic vibrational frequencies and the geometrical derivatives of transition dipole moments,the computation bottlenecks on the vibrationally-resolved electronic and scattering spectroscopies are breakdown.The integrated approaches have been applied to calculate the one/two-photon absorption,emission,and resonance Raman/hyper-Raman scattering spectroscopies of a series of chromophores in gas phase and solution.The accuracy of the integrated approaches is demonstrated by the close comparison between the simulated results and the existed experimental results.
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