Shepperson Benjamin, Søndergaard Anders A, Christiansen Lars, Kaczmarczyk Jan, Zillich Robert E, Lemeshko Mikhail, Stapelfeldt Henrik
Department of Chemistry, Aarhus University, 8000 Aarhus C, Denmark.
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark.
Phys Rev Lett. 2017 May 19;118(20):203203. doi: 10.1103/PhysRevLett.118.203203.
Rotation of molecules embedded in helium nanodroplets is explored by a combination of fs laser-induced alignment experiments and angulon quasiparticle theory. We demonstrate that at low fluence of the fs alignment pulse, the molecule and its solvation shell can be set into coherent collective rotation lasting long enough to form revivals. With increasing fluence, however, the revivals disappear-instead, rotational dynamics as rapid as for an isolated molecule is observed during the first few picoseconds. Classical calculations trace this phenomenon to transient decoupling of the molecule from its helium shell. Our results open novel opportunities for studying nonequilibrium solute-solvent dynamics and quantum thermalization.
通过飞秒激光诱导取向实验和角振子准粒子理论相结合的方法，对嵌入氦纳米液滴中的分子旋转进行了研究。我们证明，在飞秒取向脉冲的低通量下，分子及其溶剂化壳层可以被设置为持续足够长时间以形成复苏的相干集体旋转。然而，随着通量的增加，复苏消失——取而代之的是，在最初的几皮秒内观察到与孤立分子一样快速的旋转动力学。经典计算将这种现象归因于分子与其氦壳层的瞬态解耦。我们的结果为研究非平衡溶质-溶剂动力学和量子热化开辟了新的机会。
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