Theoretical Study of Chemical Reaction Dynamics

纽约大学的John Zhang在理论和计算化学计划的支持下，开发了实用的计算方法来研究多原子分子的反应动力学，重点是气体-表面反应。降维策略被用来消除不重要的自由度，同时保留重要的动力效应和量化处理。理论方法使用半刚性振动转子靶(SVRT)模型作为一种通用的、实用的、定量的动力学方法来研究涉及复杂或多原子分子的反应动力学。基本的SVRT模型将得到改进，包括对忽略的自由度和附加振动坐标的绝热修正。这些理论方法将被应用于多原子分子的化学吸附动力学的研究，重点是甲烷和其他在催化中起重要作用的碳氢化合物。研究多原子反应动力学的定量计算方法的发展对于能够利用计算机模拟来理解和预测复杂的化学和生物现象具有极其重要的意义。尽管几种反应散射方法在处理化学反应方面取得了成功，但由于密集的计算要求，这些方法目前无法处理大规模的散射计算。这一努力旨在开发可实际应用于利用现有计算资源研究复杂化学反应的方法。应用将着眼于更好地理解对理解化学催化很重要的系统，例如甲烷和其他碳氢化合物在金属表面的反应。

John Zhang of New York University is supported by the Theoretical and Computational Chemistry Program to develop practical computational methods to study reaction dynamics of polyatomic molecules with an emphasis on gas-surface reaction. A reduced dimensionality strategy is used to eliminate unimportant degrees of freedom, while preserving important dynamical effects and the quantitative treatment. The theoretical method uses the semi-rigid vibrating rotor target (SVRT) model as a general, practical, and quantitative dynamics approach to study reaction dynamics involving complex or polyatomic molecules. The basic SVRT model will be improved by including adiabatic correction for neglected degrees of freedom and additional vibrational coordinates. These theoretical methods will be applied to the study of chemisorption dynamics of polyatomic molecules, focusing on methane and other hydrocarbons that are important in catalysis. The development of quantitative computational methods to study polyatomic reaction dynamics is of enormous importance in enabling the understanding and prediction of complex chemical and biological phenomena using computer simulations. Despite the success of several reactive scattering approaches in treating chemical reactions, these approaches currently cannot handle large scale scattering calculations because of intensive computational requirements. This effort aims to develop methodology that can be realistically applied to study complex chemical reactions using currently available computational resources. Applications will be geared toward improved understanding of systems that are important in understanding chemical catalysis, such as the reaction of methane and other hydrocarbons on metal surfaces.