化学激光条件下氢原子和溴分子反应的态－态量子动力学研究

由于其丰富的谱线，氟化氢化学激光作为传统的高能化学激光之一,在国家战略需求中占居了重要位置。类似的，做为特定波长的化学激光体系，溴化氢分子最近也成为高能化学激光武器研发一个关注的体系。HBr分子和HF分子谱线差异显著，可以丰富化学激光武器的谱线范围。H+Br2反应是产生HBr激光过程中一个最重要的基元反应。同时，也是研究重-轻-重反应的一个典型的动力学体系。本项目将运用神经网络拟合方法构建包括自旋轨道耦合效应的描述H+Br2反应的相关电子基态的高精度的全维全域势能面。采用态－态反应动力学计算的含时波包方法,发展化学激光实际条件下计算态－态分辨的速率常数的理论计算方法，详细研究H＋Br2反应中产生粒子数反转的微观动力学机制，得到精确的高温下态－态分辨的速率常数。通过本项目的实施,深入理解该反应的动力学本质,并在指导探索HBr化学激光波长的可调性和增强目标激光谱功率上获得坚实的理论基础。

As one of the traditional high energy chemical lasers, HF laser has been playing an important role in national strategic demand for its rich spectral range. Similarly, the HBr molecule has recently become a system of interest in the development of high energy chemical laser weapon as a specific wavelength chemical laser system. The spectral lines of HBr and HF molecules are significantly different, which enriches the spectral range of chemical laser weapons. The H+Br2 reaction is one of the most important elementary reactions in the generation of HBr laser. And it is also a typical dynamical system for studying triatomic reactions involving two heavy atoms. In this project, the neural network fitting method will be applied to construct an accurate global potential energy surface for the ground electronic state of H+Br2 system, including spin-orbit coupling effect. The time-dependent wave packet method will be applied and developed for calculating the product ro-vibrational state-resolved rate constants under the realistic conditions of chemical lasers. The dynamics mechanism of population inversion in H+Br2 reaction will be studied in detail, and the product ro-vibrational state-resolved accurate rate constants at high temperature will be obtained. Through the implementation of this project, the dynamical nature of the reaction will be deeply understood, and a solid theoretical foundation will be obtained for guiding the exploration of the wavelength tunability of HBr chemical laser and enhancing the power of HBr laser with target spectral lines.