Balakrishnan Naduvalath, Jambrina Pablo G, Croft James F E, Guo Hua, Aoiz F Javier
Department of Chemistry and Biochemistry, University of Nevada, Las Vegas, Nevada 89154, USA.
Departamento de Química Física, Universidad de Salamanca, Salamanca 37008, Spain.
Chem Commun (Camb). 2024 Jan 30;60(10):1239-1256. doi: 10.1039/d3cc04762h.
Advances in quantum state preparations combined with molecular cooling and trapping technologies have enabled unprecedented control of molecular collision dynamics. This progress, achieved over the last two decades, has dramatically improved our understanding of molecular phenomena in the extreme quantum regime characterized by translational temperatures well below a kelvin. In this regime, collision outcomes are dominated by isolated partial waves, quantum threshold and quantum statistics effects, tiny energy splitting at the spin and hyperfine levels, and long-range forces. Collision outcomes are influenced not only by the quantum state preparation of the initial molecular states but also by the polarization of their rotational angular momentum, , stereodynamics of molecular collisions. The Stark-induced adiabatic Raman passage technique developed in the last several years has become a versatile tool to study the stereodynamics of light molecular collisions in which alignment of the molecular bond axis relative to initial collision velocity can be fully controlled. Landmark experiments reported by Zare and coworkers have motivated new theoretical developments, including formalisms to describe four-vector correlations in molecular collisions that are revealed by the experiments. In this Feature article, we provide an overview of recent theoretical developments for the description of stereodynamics of cold molecular collisions and their implications to cold controlled chemistry.
量子态制备技术与分子冷却和俘获技术的进步，使得人们能够以前所未有的方式控制分子碰撞动力学。过去二十年来取得的这一进展，极大地增进了我们对极端量子态下分子现象的理解，这种极端量子态的特征是平移温度远低于一开尔文。在这种状态下，碰撞结果主要由孤立的分波、量子阈值和量子统计效应、自旋和超精细能级的微小能量分裂以及长程力主导。碰撞结果不仅受初始分子态的量子态制备影响，还受其旋转角动量的极化、分子碰撞的立体动力学影响。过去几年发展起来的斯塔克诱导绝热拉曼通道技术，已成为研究轻分子碰撞立体动力学的通用工具，在这种碰撞中，分子键轴相对于初始碰撞速度的取向可得到完全控制。扎雷及其同事报道的具有里程碑意义的实验推动了新的理论发展，包括用于描述分子碰撞中四矢量相关性的形式体系，这些相关性由实验揭示。在这篇专题文章中，我们概述了用于描述冷分子碰撞立体动力学的近期理论发展及其对冷控化学的意义。
