Femtosecond photoexcitation dynamics inside a quantum solvent.
Femtosecond photoexcitation dynamics inside a quantum solvent.
复制标题
DOI：
10.1038/s41467-018-06413-9
复制
发表时间：
2018-10-01
影响因子：
16.6
通讯作者：
Koch M
中科院分区：
文献类型：
--
作者：
Thaler B;Ranftl S;Heim P;Cesnik S;Treiber L;Meyer R;Hauser AW;Ernst WE;Koch M
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。超流氦是一种特殊的溶剂，它可以合成迄今为止还无法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描述的溶剂响应光激发的铟（In）掺杂剂原子内氦纳米液滴（HeN），从飞秒泵浦-探测光谱和含时密度泛函理论模拟。对于In-HeN系统，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。飞秒激光光谱学有助于我们理解物质的结构和功能。在这里，作者探索了超流氦纳米滴作为样品制备方法的适用性，该方法允许调查以前无法访问的定制或脆弱的分子系统。
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 (HeN), obtained from femtosecond pump–probe spectroscopy and time-dependent density functional theory simulations. For the In–HeN 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. Femtosecond laser spectroscopy has contributed to our understanding of structure and function of matter. Here, the authors explore the applicability of superfluid helium nanodroplets as a sample preparation method that allows investigation of previously inaccessible classes of tailor-made or fragile molecular systems.
登录
查看更多内容
影响因子：
56.9
作者：
Gutberlet, Anna;Schwaab, Gerhard;Marx, Dominik
通讯作者：
Marx, Dominik
影响因子：
2.9
作者：
Wang, Chia C.;Kornilov, Oleg;Neumark, Daniel M.
通讯作者：
Neumark, Daniel M.
影响因子：
8.6
作者：
Brauer, Nils B.;Smolarek, Szymon;Drabbels, Marcel
通讯作者：
Drabbels, Marcel
影响因子：
8.6
作者：
Koch, Markus;Auboeck, Gerald;Ernst, Wolfgang E.
通讯作者：
Ernst, Wolfgang E.
影响因子：
3.3
作者：
Leal, Antonio;Mateo, David;Barranco, Manuel
通讯作者：
Barranco, Manuel