Non-Born-Oppenheimer Effects between Electrons and Protons

电子和质子之间的非玻恩奥本海默效应

• 批准号: 1361293
• 负责人: Sharon Hammes-Schiffer
• 金额: $ 63.7万
• 依托单位: University of Illinois at Urbana-Champaign
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2014
• 资助国家: 美国
• 起止时间: 2014-07-15 至 2018-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1361293&HistoricalAwards=false
• 关键词: Non; Born; Oppenheimer; Effects; between

Sharon Hammes-Schiffer of the University of Illinois at Urbana-Champaign is supported by an award from the Chemical Theory, Models and Computational Methods program in the Chemistry Division and the Division of Advanced Cyberinfrastructure to develop efficient and accurate computational methods that describe the coupled motion of electrons and protons in chemical and biological systems. The coupling between electrons and protons plays a vital role in a wide range of biological and chemical processes, including photosynthesis, respiration, and energy production in solar cells. It is difficult to develop computational approaches to accurately describe this coupling because electrons and protons are so light that they must be treated quantum mechanically. After extensive assessment and validation, these computational methods will be incorporated into a computer program that will be available to the public. Moreover, these computational methods will be applied to specific processes of biological and chemical relevance to elucidate the underlying fundamental principles that determine the processes. Professor Hammes-Schiffer and her research group maintain a web site that contains software and educational tools related to this topic. The computer programs, tools, demonstrations, and tutorials available on this web site enable scientists in a broad range of fields to learn about the coupled motion of electrons and protons. In addition, this project will facilitate technological and biomedical advances through a better understanding of this important research area. An important example is the design of more effective solar cells and other alternative, renewable energy sources. Another example is the design of more effective drugs through modification of enzymes that rely on the coupling between electrons and protons. The objective of this project is to develop new theoretical and computational approaches to provide insight into the underlying fundamental principles of proton-coupled electron transfer (PCET) reactions. These reactions play a vital role in a broad range of biological and chemical processes. The specific issues to be examined include the roles of nuclear quantum effects, hydrogen tunneling, and non-Born-Oppenheimer effects, which are thought to be significant in PCET. These issues will be explored using the nuclear-electronic orbital (NEO) approach, in which all electrons and the transferring proton(s) are treated quantum mechanically on the same level with molecular orbital methods or density functional theory. This approach enables the calculation of key quantities in PCET theories for determining rates and mechanisms. It is also applicable to a wide range of other chemical and biological systems. A major goal of this project is to develop algorithms to enhance the computational efficiency of this approach, assess and validate the methodology, and port the NEO code to GAMESS, a general quantum chemistry package available to the public. The NEO method benefits from the optimized components of other parts of the general electronic structure package, and portions of the NEO code will be useful to other scientists. This software development enables calculations that are not currently possible with existing codes. In addition, a web site on PCET is maintained and enhanced to convey useful information to the general community.

伊利诺伊大学在Urbana-Champaign的Sharon Hammes-Schiffer得到了化学理论，模型和计算方法计划的奖励，并在化学分区和先进的网络基础设施的划分中提供了有效，准确的计算方法，以开发有效且准确的计算方法，这些方法描述了化学和生物学系统中电子和蛋白质运动的辅助运动。 电子和质子之间的耦合在广泛的生物学和化学过程中起着至关重要的作用，包括光合作用，呼吸和太阳能电池的能量产生。很难开发计算方法来准确描述这种耦合，因为电子和质子很轻，必须机械地对其进行量子处理。经过广泛的评估和验证后，这些计算方法将被纳入一个计算机程序中，该程序将向公众使用。 此外，这些计算方法将应用于生物学和化学相关的特定过程，以阐明确定过程的基本原理。 Hammes-Schiffer教授和她的研究小组维护了一个网站，其中包含与此主题相关的软件和教育工具。 该网站上提供的计算机程序，工具，演示和教程使科学家在广泛的领域中可以了解电子和质子的耦合运动。 此外，该项目将通过更好地理解这一重要研究领域来促进技术和生物医学的进步。 一个重要的例子是设计更有效的太阳能电池和其他替代性可再生能源。 另一个例子是通过修饰依赖于电子和质子之间耦合的酶来设计更有效的药物。该项目的目的是开发新的理论和计算方法，以洞悉质子耦合电子传递（PCET）反应的基本基本原理。 这些反应在广泛的生物学和化学过程中起着至关重要的作用。要研究的具体问题包括核量子效应，氢隧穿和非出生的烟雾效应的作用，这些效应在PCET中被认为很重要。 这些问题将使用核电子轨道（NEO）方法进行探索，其中所有电子和转移质子（S）通过分子轨道方法或密度功能理论在相同水平上机械地处理量子。 这种方法可以计算PCET理论中的关键量，以确定速率和机制。 它也适用于广泛的其他化学和生物系统。 该项目的主要目标是开发算法，以提高这种方法的计算效率，评估和验证方法，并将NEO CODE移植到Gamess，这是公众可供公众使用的通用量子化学软件包。 NEO方法受益于一般电子结构包的其他部分的优化组成部分，而NEO代码的一部分将对其他科学家有用。该软件开发实现了现有代码当前无法进行的计算。 此外，维护和增强了PCET上的网站，以向一般社区传达有用的信息。