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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Photoinduced Cooling of Polyatomic Molecules in an Electronically Excited State in the Presence of Dushinskii Rotations
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Photoinduced Cooling of Polyatomic Molecules in an Electronically Excited State in the Presence of Dushinskii Rotations

机译：在Dushinskii旋转存在下电子激发态的多原子分子的光诱导冷却

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摘要

We present a theoretical study of the effect of Dushinskii rotations on the vibrational population created in an excited electronic state through photoexcitation.Special attention is given to the effect of Dushinskii rotations on the possibility of cooling the vibrational population in the excited state,relative to the thermal distribution in the ground state.The absorption spectrum and corresponding average energy in the excited state are calculated using a closed-form expression for the harmonic correlation function between the ground and excited electronic states,which includes the effects of Dushinskii rotations,equilibrium position shifts,and frequency shifts between the excited- and ground-electronic-state normal modes.We investigate numerically the separate and joint effects of rotation,position shifts,and frequency shifts on the absorption spectrum and average vibrational energy in the excited electronic state.We find that,although the Dushinskii rotations generally diminish the cooling effect,the effect does not disappear and,in some cases,may also increase slightly.
机译：我们对Dushinskii旋转对通过光激发在激发电子状态下产生的振动种群的影响进行理论研究。使用封闭形式的基态和激发电子态之间的谐波相关函数来计算激发态的吸收光谱和相应的平均能量，其中包括Dushinskii旋转，平衡位置偏移的影响，并研究了激发态和基态电子态之间的频移。我们通过数值研究了在激发态电子中，旋转，位置位移和频移对吸收谱和平均振动能的分离联合效应。尽管Dushinskii旋转通常会减小冷却效果不会消失，在某些情况下，效果可能还会略有增加。

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