Non-Born-Oppenheimer Effects in the Framework of Multicomponent Time-Dependent Density Functional Theory

多分量时变密度泛函理论框架中的非玻恩奥本海默效应

• 批准号: 2415034
• 负责人: Sharon Hammes-Schiffer
• 金额: $ 68万
• 依托单位: Princeton University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-01-15 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2415034&HistoricalAwards=false
• 关键词: Non; Born; Oppenheimer; Effects; Framework

Professor Sharon Hammes-Schiffer of Yale University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop computational methods for describing the role of electrons and protons in chemical processes. The interaction or coupling of 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. The development of computational methods that accurately describe this coupling is challenging because electrons and protons are so light that they must be treated specially, which is computationally expensive. Professor Hammes-Schiffer is developing methods that describe electrons and protons in a computationally practical manner. She is applying these methods to specific processes of biological and chemical relevance to elucidate the fundamental principles of these processes. In addition, she and her research group are incorporating these computational methods into established quantum chemistry software packages to benefit the general scientific community. Professor Hammes-Schiffer is also maintaining and enhancing a website containing software and educational tools including computer programs, tools, demonstrations, and tutorials. This research facilitates technological and biomedical advances in more effective solar cells and other renewable energy sources as well as improved understanding of enzymes. Professor Hammes-Schiffer is developing new theoretical and computational approaches that provide insight into the underlying fundamental principles of photoinduced proton transfer and proton-coupled electron transfer (PCET) reactions, which play a vital role in a broad range of biological and chemical processes. These approaches are designed to include nuclear quantum effects, such as proton delocalization and zero-point energy, as well as non-Born-Oppenheimer effects, in a computationally practical manner. Hammes-Schiffer is developing these methods within the framework of the nuclear-electronic orbital density functional theory (NEO-DFT) approach, which treats key nuclei, such as the transferring proton(s), quantum mechanically on the same level as the electrons within the framework of DFT. The multicomponent time-dependent DFT (NEO-TDDFT) approach enables the calculation of excited electronic, proton vibrational, and electron-proton vibronic states. Hammes-Schiffer is developing NEO methods for computing minimum energy paths and tunneling splittings for proton transfer and PCET reactions, as well as mixed electron-proton vibronic excited states for photoinduced reactions. She is also developing real-time NEO-TDDFT methods and other nonadiabatic dynamics methods for the simulation of ultrafast electronic and nuclear dynamics, targeting applications to photoinduced PCET reactions. She is incorporating these approaches into well-established quantum chemistry software packages and is creating tutorials to explain how to perform NEO calculations and highlight the unique capabilities of this approach. Furthermore, she is maintaining and enhancing a web site on PCET to convey useful information to the community and to provide valuable tools, scripts, and programs relevant to studying PCET.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.

耶鲁大学的莎朗·哈姆斯·西弗（Sharon Hammes-Schiffer）教授得到了化学理论，模型和计算方法计划的奖项，以开发计算方法来描述电子和质子在化学过程中的作用。电子和质子的相互作用或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。准确描述这种耦合的计算方法的开发是具有挑战性的，因为电子和质子很轻，必须对其进行特殊处理，这在计算上很昂贵。 Hammes-Schiffer教授正在开发以计算实际方式描述电子和质子的方法。她将这些方法应用于生物学和化学相关性的特定过程，以阐明这些过程的基本原理。此外，她和她的研究小组正在将这些计算方法纳入已建立的量子化学软件软件包中，以使一般科学界受益。 Hammes-Schiffer教授还正在维护和增强包含软件和教育工具在内的网站，包括计算机程序，工具，演示和教程。这项研究促进了更有效的太阳能电池和其他可再生能源的技术和生物医学进步，并提高了对酶的理解。 Hammes-Schiffer教授正在开发新的理论和计算方法，这些方法可深入了解光诱导的质子传递和质子偶联电子转移（PCET）反应的基本原理，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。这些方法旨在以计算上实用的方式包括核量子效应，例如质子离域和零点能以及非出生的烟雾效应。 Hammes-Schiffer正在核电子轨道密度功能理论（NEO-DFT）方法的框架内开发这些方法，该方法处理关键核，例如转移质子（S），与DFT框架内的电子水平相同。多组分时间依赖性DFT（NEO-TDDFT）方法可以计算激发电子，质子振动和电子蛋白振动状态。 Hammes-Schiffer正在开发用于计算质子转移和PCET反应的最小能量路径和隧道分裂的NEO方法，以及用于光诱导反应的混合电子 - 蛋白质振动激发态。她还开发了实时的NEO-TDDFT方法和其他非绝热动力学方法，以模拟超快电子和核动力学，将应用靶向光诱导的PCET反应。她将这些方法纳入了完善的量子化学软件软件包中，并正在创建教程，以解释如何执行NEO计算并突出这种方法的独特功能。此外，她正在维护和增强PCET上的网站，以向社区传达有用的信息，并提供与研究PCET相关的有价值的工具，脚本和计划。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛的审查标准通过评估来通过评估来支持的。