CCI Phase I: NSF Center for First Principles Design of Quantum Processes

量子力学在最基本、最小尺度的水平上描述了所有的自然--亚原子粒子、原子和光。化学反应的核心是涉及电子和原子核运动的量子力学过程。了解化学反应发生的方式对于预测新的反应很重要。NSF量子过程第一原理设计中心将理论家和实验学家聚集在一起，开发新的方法来理解、预测和设计与化学反应有关的量子力学现象。这些研究活动在该领域具有相当广泛的影响，因为这些过程是许多化学应用的核心，包括开发新的光收集材料(用于可再生能源)和改进的生物医学成像技术。新理论工具的开发、理论和实验相结合的研究生培训、来自不同背景的本科生的早期研究机会，以及使用可视化设备向广大受众传达量子过程的复杂性，也产生了更广泛的影响。NSF量子过程第一原理设计中心致力于为原子量子力学分子动力学开发完全预测的理论方法，以实现分子和材料的合理理论辅助设计。与实验者的紧密联系确保了这些方法得到了很好的验证。具体的合作项目包括：(1)定制质子缺陷在金属有机骨架(MOF)和界面等复杂环境中的传输和反应；(2)了解和操纵自然光合作用系统中的激发能量传输；(3)阐明和控制荧光蛋白质中荧光和光异构化的影响因素。其核心理论框架是从头算分子动力学(AIMD)，包括定域和周期基组、基态和激发态模拟，以及包括大空间和时间尺度的非绝热和其他量子力学效应在内的有效动力学技术。研究活动产生的更广泛的影响是重大的，因为改进的理论方法允许对难以通过实验解决的领域进行前所未有的洞察和控制。新理论工具的开发、理论和实验相结合的研究生培训、为不同背景的本科生提供的早期研究机会，以及使用可视化和触觉设备向广大受众传达量子过程的复杂性，也产生了更广泛的影响。该中心模式将理论和实验相结合，为研究生和博士后研究人员提供创新培训。还在开发新的软件工具，并向专业化学家和学生的不同受众传播。

Quantum mechanics describes all nature at the most fundamental, smallest-scale level -- sub-atomic particles, atoms and light. Chemical reactions are, at their core, quantum mechanical processes that involve the motion of electrons and nuclei. Understanding the ways that chemical reactions occur is important to being able to predict new reactions. The NSF Center for First Principles Design of Quantum Processes brings together theorists and experimentalists to develop new methods to understand, predict and design quantum mechanical phenomena as they relate to chemical reactions. The research activities have substantial broader impacts in the field since these processes are central to many chemical applications, including the development of new light-harvesting materials (for renewable energy) and improved bio-medical imaging techniques. Broader impacts also result from the development of new theory tools, graduate student training at the interface of theory and experiment, early research opportunities for undergraduates from diverse backgrounds, and the use of visualization devices to convey the complexities of quantum processes to broad audiences. The NSF Center for First Principles Design of Quantum Processes is focused on developing fully-predictive theoretical methods for atomistic quantum mechanical molecular dynamics for the rational theory-aided-design of molecules and materials. Strong ties to experimentalists ensure that the methods are well validated. Specific collaborative projects include: (1) tailoring transport and reactivity of proton defects in complicated environments such as metal organic frameworks (MOFs) and interfaces, (2) understanding and manipulating excitation energy transport in natural photosynthetic systems, and (3) elucidating and controlling the factors governing fluorescence vs. photoisomerization in fluorescent proteins. The central theoretical framework is ab initio molecular dynamics (AIMD), including localized and periodic basis sets, ground and excited-state simulations, and efficient dynamics techniques including non-adiabatic and other quantum mechanical effects for large spatial and temporal scales. Broader impacts from the research activities are significant since the enhanced theoretical methods allow for unprecedented insight and control in areas that are difficult to address experimentally. Broader impacts also result from the development of new theory tools, graduate student training at the interface of theory and experiment, early research opportunities for undergraduates from diverse backgrounds, and the use of visualization and haptic devices to convey the complexities of quantum processes to broad audiences. The Center model integrates theory and experiment and provides innovative training of graduate students and postdoctoral researchers. New software tools are also being developed and disseminated to a diverse audience of professional chemists and students.