Collaborative Proposal: Frameworks: Sustainable Open-Source Quantum Dynamics and Spectroscopy Software

合作提案：框架：可持续开源量子动力学和光谱软件

• 批准号: 2103717
• 负责人: Xiaosong Li
• 金额: $ 75万
• 依托单位: University of Washington
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-08-01 至 2027-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2103717&HistoricalAwards=false
• 关键词: Collaborative; Proposal; Frameworks; Sustainable; Open

With support from the Office of Advanced Cyberinfrastructure and the Division of Chemistry at NSF, Professor Li and his team will work to expand the capabilities of the open-source software platform, Chronus Quantum (ChronusQ), to include time-resolved spectroscopy for supporting quantum chemistry calculations. The new capabilities will include novel computational methods to provide unprecedented capabilities to simulate chemical processes of electrons and nuclei that exhibit quantum behaviors. The physical insights gleaned through applications of ChronusQ underlie the advancement of new technologies that are crucial to sustainable energy, catalysis, quantum computing, and other applications that can immediately impact society. This project provides a mechanism for advanced interdisciplinary education and training in the areas of inorganic, theoretical, physical, and materials chemistry. The collaborative academic research serves as a test ground for identifying and deploying ways that the scientific community as a whole can both increase awareness of the importance of active engagement in professional skill development for graduate students and post-doctoral scholars, and develop tools to facilitate professional development in an academic setting.ChronusQ seamlessly integrates time-dependent quantum mechanical theories, spectral analysis tools, and modular high-performance numerical libraries that are highly parallelized, extensible, reusable, community-driven, and open-sourced. The Team develops in ChronusQ the complete time-dependent quantum description of coupled nuclear and electronic dynamics within the time-dependent density functional theory and equation-of-motion coupled cluster framework. The project enables computational studies of ultrafast time-resolved spectroscopies and simulations of chemical processes in the strongly nonadiabatic regime. Software modules are bolstered by algebraic and integral acceleration engines that can make it feasible to simulate fully quantum mechanically molecular dynamics. The collaborative project advances the theoretical description of quantum dynamics across time scales, bridging the attosecond and subnanosecond regimes, enabling the development of spectroscopic technologies to probe molecular and materials properties with state specificity that is beyond the Born-Oppenheimer approximation.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.

在 NSF 高级网络基础设施办公室和化学部的支持下，李教授和他的团队将致力于扩展开源软件平台 Chronus Quantum (ChronusQ) 的功能，以包括支持量子的时间分辨光谱化学计算。新功能将包括新颖的计算方法，以提供前所未有的能力来模拟表现出量子行为的电子和原子核的化学过程。通过 ChronusQ 的应用收集到的物理见解是新技术进步的基础，这些技术对于可持续能源、催化、量子计算和其他可以立即影响社会的应用至关重要。该项目为无机化学、理论化学、物理化学和材料化学领域的高级跨学科教育和培训提供了机制。合作学术研究作为一个试验场，用于确定和部署整个科学界既可以提高研究生和博士后学者积极参与专业技能发展重要性的认识，又可以开发促进专业技能发展的工具。 ChronusQ 无缝集成了时间相关的量子力学理论、光谱分析工具和模块化高性能数值库，这些库具有高度并行性、可扩展性、可重用性、社区驱动性和开源性。该团队在 ChronusQ 中，在瞬态密度泛函理论和运动方程耦合簇框架内，开发了耦合核和电子动力学的完整瞬态量子描述。该项目能够对超快时间分辨光谱进行计算研究，并在强非绝热条件下模拟化学过程。软件模块由代数和积分加速引擎支持，可以使模拟完全量子力学分子动力学成为可能。该合作项目推进了跨时间尺度的量子动力学的理论描述，连接了阿秒和亚纳秒体系，使光谱技术的发展能够探测分子和材料特性，其状态特异性超出了玻恩-奥本海默近似。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

Simultaneous Optimization of Nuclear–Electronic Orbitals

核电子轨道的同步优化

• DOI: 10.1021/acs.jpca.2c05172
• 发表时间: 2022-10
• 期刊: The Journal of Physical Chemistry A
• 作者: Liu, Aodong;Chow, Mathew;Wildman, Andrew;Frisch, Michael J.;Hammes;Li, Xiaosong
• 通讯作者: Li, Xiaosong

Solvent Induced Proton Polarization within the Nuclear−Electronic Orbital Framework

核电子轨道框架内溶剂诱导质子极化

• DOI: 10.1021/acs.jpclett.3c00471
• 发表时间: 2023-03
• 期刊: The Journal of Physical Chemistry Letters
• 作者: Lambros, Eleftherios;Link, Benjamin;Chow, Mathew;Hammes;Li, Xiaosong
• 通讯作者: Li, Xiaosong