Laboratoire Interdisciplinaire Carnot de Bourgogne (ICB), UMR 6303 CNRS-Université, Bourgogne-Franche Comté, 9 Ave. A. Savary, BP 47 870, F-21078 Dijon Cedex, France.
J Chem Phys. 2018 Mar 28;148(12):124303. doi: 10.1063/1.5019356.
The field-free molecular alignment of symmetric-top molecules, ethane, induced by intense non-resonant linearly polarized femtosecond laser pulses is investigated experimentally in the presence of collisional relaxation. The dissipation dynamics of field-free molecular alignment are measured by the balanced detection of ultrafast molecular birefringence of ethane gas samples at high pressures. By separating the molecular alignment into the permanent alignment and the transient alignment, the decay time-constants of both components are quantified at the same pressure. It is observed that the permanent alignment always decays slower compared to the transient alignment within the measured pressure range. This demonstrates that the propensity of molecules to conserve the orientation of angular momentum during collisions, previously observed for linear species, is also applicable to symmetric-top molecules. The results of this work provide valuable information for further theoretical understanding of collisional relaxation within nonlinear polyatomic molecules, which are expected to present interesting and nontrivial features due to an extra rotational degree of freedom.
在碰撞弛豫的情况下,实验研究了强非共振线偏振飞秒激光脉冲诱导的对称陀螺分子(乙烷)的无场分子取向。通过平衡检测高压乙烷气体样品的超快分子双折射,测量无场分子取向的耗散动力学。通过将分子取向分为永久取向和瞬态取向,在相同压力下量化了两个分量的衰减时间常数。观察到,在所测量的压力范围内,永久取向的衰减总是比瞬态取向慢。这表明,分子在碰撞过程中保持角动量方向的倾向,以前在直线物种中观察到,也适用于对称陀螺分子。这项工作的结果为进一步理解非线性多原子分子中的碰撞弛豫提供了有价值的信息,由于额外的转动自由度,预计这些分子将呈现出有趣和非平凡的特征。