Quantum Simulation of Chemical Dynamics in Solution

溶液中化学动力学的量子模拟

• 批准号: 9314066
• 负责人: Peter Rossky
• 金额: $ 58.8万
• 依托单位: University of Texas at Austin
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 1993
• 资助国家: 美国
• 起止时间: 1993-12-01 至 1999-11-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9314066&HistoricalAwards=false
• 关键词: Quantum; Simulation; Chemical; Dynamics; Solution

Peter Rossky is supported by a grant from the Theoretical and Computational Chemistry Program to continue his work in the area of quantum simulation of chemical dynamics in solution. This research focuses on both the development and application of mixed quantum and classical mechanical simulation methods for the description of chemical processes in solution. Emphasis is placed on the simulation of nonadiabatic quantum dynamics. The work will address in detail: 1) The fundamental molecular level description of the solvent modes associated with the non-radiative relaxation of solute excited electronic states in liquid solution; 2) New applications of algorithms for quantum nonadiabatic simulation to the dynamics of molecular photoionization and to intramolecular charge transfer dynamics in both aqueous and non-aqueous solution; 3) The development and implementation of new algorithms for nonadiabatic quantum dynamics; and 4) Generalization and testing of current nonadiabatic algorithms with emphasis on an analysis of the role of quantum coherence in the results obtained in the condensed phase. The majority of chemical reactions occur in solution. This fact has stimulated a tremendous research effort to elucidate a set of unifying principles describing chemical dynamics in liquids. To fully address this issue requires a detailed understanding of both the molecular motions that occur during the course of a chemical event and the energy flow within the solute and between the solute and the solvent. Exceptional recent progress in clarifying these aspects has been made. Advances in laser technology enable direct experimental measurement of dynamical behavior of chemical systems on the time scale of the fundamental events. At the same time, significant advances have been made in theoretical methods and models used in describing solution chemistry. Rossky's research in the development of new computational algorithms will allow for both cl assical and quantum mechanical dynamical simulations of phenomena on time scales accessible by these new experimental techniques.

Peter Rossky获得了理论和计算化学项目的资助，继续他在溶液中化学动力学的量子模拟领域的工作。本研究的重点是发展和应用混合量子和经典力学模拟方法来描述溶液中的化学过程。重点放在非绝热量子动力学的模拟上。本工作将详细讨论：1)与液体溶液中溶质激发态非辐射弛豫相关的溶剂模式的基本分子水平描述；2)量子非绝热模拟算法在分子光离动力学和分子内电荷转移动力学中的新应用；3)非绝热量子动力学新算法的开发与实现；4)推广和测试现有的非绝热算法，重点分析量子相干性在凝聚态所得结果中的作用。大多数化学反应发生在溶液中。这一事实激发了巨大的研究努力，以阐明一套描述液体化学动力学的统一原则。为了充分解决这个问题，需要详细了解化学事件过程中发生的分子运动以及溶质内部和溶质与溶剂之间的能量流动。最近在澄清这些方面取得了非凡的进展。激光技术的进步使得在基本事件的时间尺度上对化学系统的动力学行为进行直接的实验测量成为可能。同时，在描述溶液化学的理论方法和模型方面也取得了重大进展。Rossky在新计算算法开发方面的研究将允许这些新的实验技术在时间尺度上对现象进行经典和量子力学的动态模拟。