Methods for Simulating Nonadiabatic Dynamics with Trajectories

用轨迹模拟非绝热动力学的方法

• 批准号: 1764209
• 负责人: Craig Martens
• 金额: $ 42万
• 依托单位: University of California-Irvine
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-08-01 至 2022-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1764209&HistoricalAwards=false
• 关键词: Methods; Simulating; Nonadiabatic; Dynamics; Trajectories

Craig C. Martens of the University of California, Irvine is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop computational methods to simulate quantum processes in molecular systems. Ordinary Newtonian or classical mechanics is used to understand the motion of everyday objects such as golf balls or airplanes. Very light particles such as electrons, however, must be described using quantum mechanics. The motion of atoms and electrons that accompany chemical reactions falls in the frontier separating classical and quantum mechanical descriptions of matter. Martens and his research group explore this frontier by incorporating quantum effects into the conceptually intuitive and computationally efficient framework of classical mechanics. They focus on nonadiabatic dynamics of molecules, where quantum electronic transitions accompany the nearly classical vibrations and chemical rearrangements of the constituent atoms. Martens' goal is to gain an understanding of the nature of quantum mechanics at a fundamental level while at the same time developing methods that are more efficient and accurate than existing approaches. Their research activities are paralleled by an outreach program that includes mentoring undergraduate and high school students to write educational computer games that add quantum effects to familiar but inherently classical gameplay to illustrate quantum mechanics in a manner that is accessible to nonscientists, and even to children. Martens and his group are developing a new stochastic surface hopping approach that captures quantum nonlocality and coherence fully and accurately in a classical trajectory context. Unlike current methodology, the novel approach describes quantum properties of the system such as the populations, coherence, and the partitioning of energy collectively through interrelationships between the trajectories of the ensemble taken as a whole. Martens and coworkers aim to achieve a quantitatively accurate trajectory-based method for simulating molecular dynamics with electronic transitions within this framework, both as a fundamental achievement and as a benchmark for the introduction of further approximations. Ultimately, they seek accurate but economical and efficient methodologies based on well-understood and tested compromises rather than ad hoc simplifications. They are constructing an independent trajectory approach incorporating rigorously derived quantum generalized forces that avoid ad hoc features of standard methodology with the goal of broader applicability while being roughly equal in cost. The Martens group is pursuing extensions to multidimensional systems, where energy partitioning and geometric phase effects provide challenging tests of the new approach. In addition, Martens is implementing an outreach program that bridges the gap between performing arts and science, with the goals of enhancing the image and accessibility of science as a career. He is also mentoring undergraduate and high school students in the development of video games that illustrate the fundamentals of quantum mechanics to youth and nonscientists.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

克雷格C.加州大学欧文分校的Martens获得了化学系化学理论、模型和计算方法项目的奖励，以开发模拟分子系统中量子过程的计算方法。 普通的牛顿力学或经典力学被用来理解高尔夫球或飞机等日常物体的运动。然而，像电子这样非常轻的粒子必须用量子力学来描述。 伴随着化学反应的原子和电子的运动福尔斯处于分离物质的经典和量子力学描述的前沿。 马滕斯和他的研究小组通过将量子效应纳入经典力学概念上直观和计算效率高的框架来探索这一前沿。 他们专注于分子的非绝热动力学，其中量子电子跃迁伴随着组成原子的近经典振动和化学重排。 马滕斯的目标是在基础层面上理解量子力学的本质，同时开发比现有方法更有效和准确的方法。 他们的研究活动是由一个推广计划，包括指导本科生和高中生编写教育计算机游戏，增加量子效应熟悉，但固有的经典游戏，以说明量子力学的方式，是非科学家，甚至儿童访问。Martens和他的团队正在开发一种新的随机表面跳跃方法，该方法可以在经典轨迹背景下完全准确地捕获量子非定域性和相干性。 与目前的方法不同，新的方法描述了系统的量子特性，如人口，相干性，并通过作为一个整体的合奏轨迹之间的相互关系，集体分配能量。 Martens及其同事的目标是实现一种基于定量精确度的方法，用于在此框架内模拟具有电子跃迁的分子动力学，这既是一项基本成就，也是引入进一步近似的基准。 最终，他们寻求准确但经济有效的方法，这些方法基于充分理解和测试的妥协，而不是临时简化。 他们正在构建一种独立的轨道方法，该方法结合了严格推导的量子广义力，避免了标准方法的特殊特征，目标是在成本大致相等的情况下实现更广泛的适用性。 Martens小组正在寻求多维系统的扩展，其中能量划分和几何相位效应为新方法提供了具有挑战性的测试。 此外，马滕斯正在实施一项外展计划，弥合表演艺术和科学之间的差距，目标是提高科学作为一种职业的形象和可及性。 他还指导本科生和高中生开发视频游戏，向年轻人和非科学家说明量子力学的基础知识。该奖项反映了NSF的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Study of the Vibrational Predissociation of the NeBr2 Complex by Computational Simulation Using the Trajectory Surface Hopping Method

采用轨迹表面跳跃法的计算模拟研究 NeBr2 配合物的振动预解离

• DOI: 10.3390/math8112029
• 发表时间: 2020
• 期刊: Mathematics
• 影响因子: 2.4
• 作者: García-Alfonso, Ernesto;Márquez-Mijares, Maykel;Rubayo-Soneira, Jesús;Halberstadt, Nadine;Janda, Kenneth C.;Martens, Craig C.
• 通讯作者: Martens, Craig C.

Photofragmentation dynamics study of ArBr$$_2$$ $$(v=16,\ldots ,25)$$ using two theoretical methods: trajectory surface hopping and quasiclassical trajectories

使用两种理论方法对 ArBr$$_2$$ $$(v=16,ldots ,25)$$ 进行光碎裂动力学研究：轨迹表面跳跃和准经典轨迹

• DOI: 10.1140/epjd/s10053-022-00392-9
• 发表时间: 2022
• 期刊: The European Physical Journal D
• 作者: García-Alfonso, Ernesto;Márquez-Mijares, Maykel;Rubayo-Soneira, Jesús;Halberstadt, Nadine;Janda, Kenneth C.;Martens, Craig C.
• 通讯作者: Martens, Craig C.

Classical and nonclassical effects in surface hopping methodology for simulating coupled electronic-nuclear dynamics

模拟耦合电子核动力学的表面跳跃方法中的经典和非经典效应

• DOI: 10.1039/c9fd00042a
• 发表时间: 2019
• 期刊: Faraday Discussions
• 影响因子: 3.4
• 作者: Martens, Craig C.