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

在美国国家科学基金会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努力扩展开源软件平台Chronus Quantum （ChronusQ）的功能，以包括支持量子化学计算的时间分辨光谱。新的能力将包括新的计算方法，以提供前所未有的能力来模拟电子和原子核的化学过程，表现出量子行为。通过ChronusQ的应用收集到的物理见解为新技术的进步奠定了基础，这些新技术对可持续能源、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一种机制。合作学术研究作为一个试验场，可以识别和部署科学界作为一个整体，既可以提高对研究生和博士后学者积极参与专业技能发展的重要性的认识，又可以开发工具来促进学术环境中的专业发展。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化、可扩展、可重用、社区驱动和开源的特点。该团队在ChronusQ中开发了在时变密度泛函理论和运动方程耦合簇框架内耦合核和电子动力学的完整时变量子描述。该项目使超快时间分辨光谱的计算研究和强非绝热状态下化学过程的模拟成为可能。软件模块由代数和积分加速引擎支持，可以模拟完全的量子力学分子动力学。该合作项目推进了跨时间尺度量子动力学的理论描述，连接了阿秒和亚纳秒的机制，使光谱技术的发展能够探测分子和材料的特性，其状态特异性超出了Born-Oppenheimer近似。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.