He纳米液滴中碘分子的Laser诱导旋转:回复和自由断裂
Laser-induced rotation of iodine molecules in He-nanodroplets: revivals and breaking-free
摘要:
利用飞秒激光诱导取向实验和角动量准粒子理论研究了氦纳米液滴中分子的旋转。我们证明,在低通量的fs对齐脉冲,分子和它的溶剂化壳层可以设置为相干集体旋转持续足够长的时间,形成复苏。然而,随着能量密度的增加,复兴消失了-相反,在最初的几皮秒期间观察到与孤立分子一样快的旋转动力学。经典计算将这种现象追溯到分子与其He壳层的瞬时解耦。我们的研究结果打开了新的机会,研究非平衡溶质-溶剂动力学和量子热化。
英文摘要:
Rotation of molecules embedded in He 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 He shell. Our results open novel opportunities for studying non-equilibrium solute-solvent dynamics and quantum thermalization.
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