量子溶剂中的飞秒光激发动力学
Femtosecond photoexcitation dynamics inside a quantum solvent
摘要：
利用脉冲长度不断缩短的激光，可以在电子和原子核运动的时间尺度上观察化学反应。超流氦是一种特殊溶剂，可以合成迄今为止尚未进行动力学研究的新型分子。然而，这种量子溶剂内的光激发触发了溶剂化壳层的明显响应，这还不是很清楚。在这里，我们提出了一个机械的溶剂响应于光激发的铟（In）掺杂剂原子内氦纳米液滴（He $_\mathrm{N}$），飞秒泵浦-探测光谱和时间相关的密度泛函理论模拟。对于In-He $_\mathrm{N}$体系，部分激发态电子能量导致溶剂化壳层在600 fs内膨胀，引发周期约为30 ps的集体壳层振荡。这些耦合的电子和核动力学将叠加在氦滴内分子系统的固有光诱导过程上。
英文摘要：
The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of novel classes of molecules that have eluded dynamical studies so far. However, photoexcitation inside this quantum solvent triggers a pronounced response of the solvation shell, which is not well understood. Here we present a mechanistic description of the solvent response to photoexcitation of indium (In) dopant atoms inside helium nanodroplets (He$_\mathrm{N}$), obtained from femtosecond pump-probe spectroscopy and time-dependent density functional theory simulations. For the In-He$_\mathrm{N}$ system, part of the excited state electronic energy leads to expansion of the solvation shell within 600 fs, initiating a collective shell oscillation with a period of about 30 ps. These coupled electronic and nuclear dynamics will be superimposed on intrinsic photoinduced processes of molecular systems inside helium droplets.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
