Collaborative Research: Elements: GPU-accelerated First-Principles Simulation of Exciton Dynamics in Complex Systems

发展具有重要社会意义的能量收集方法，如光催化或光伏发电，需要详细了解新材料中电子与离子耦合的快速动力学。现代超级计算机可以通过复杂的量子力学模拟来帮助我们理解这一点。然而，这样的科学努力需要开发精确的模拟技术，并且有效使用底层超级计算机硬件是至关重要的。本项目通过采用新颖的技术来描述量子力学电子-电子相互作用和电子动力学与离子的相互作用，以满足这些突出的挑战。在图形处理单元上使用和测试这些新发展是科学的进步，因为它为下一代超级计算机的量子力学模拟做了准备。将这些先进的模拟应用于对能量收集非常重要的复杂系统的建模，进一步推动了计算科学界朝着促进国家繁荣和福利的目标迈进。该项目将这些技术免费提供给广泛的社区，包括文档和教程，并通过组织暑期学校和讲习班培训下一代计算研究人员。该项目利用了一个多组织的团队，从两种可能的解决方案中产生的协同效应中受益，以解决当前的科学障碍：基于远程校正的交换和相关性描述，以及混合功能，即使对于具有数千个电子的大型系统也可以实现和应用。非绝热动力学的描述被实现并应用于研究激子的长期动力学，在此过程中与原子核的相互作用变得重要。在图形处理单元上高效运行的尖端电子结构代码中进行此操作，为比较准确性、对广泛系统的适用性和计算成本提供了独特的机会。本研究提高了这些近似的可靠性及其对实际相关扩展系统（包括半导体-分子界面等复杂异质系统）的计算成本的认识。这些努力包括建立、增加和发展一个技术社区，特别是在一个经常性的暑期学校的美国研究人员。该提案通过计算机和信息科学与工程理事会的先进网络基础设施办公室以及数学和物理科学理事会的材料研究司获得资金。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。

The development of societally-important energy harvesting approaches, such as photocatalysis or photovoltaics, requires detailed understanding of fast dynamics of electrons coupled with ions in novel materials. Modern supercomputers can help obtain such an understanding using sophisticated quantum-mechanical simulations. However, such a scientific effort requires accurate simulation techniques to be developed and efficient use of the underlying supercomputer hardware is crucial. This project meets these outstanding challenges by implementing novel techniques to describe the quantum-mechanical electron-electron interaction and interactions of electron dynamics with ions. Using and testing these new developments on graphical processing units advances science as it prepares quantum-mechanical simulations for next-generation supercomputers. Applying these advanced simulations to model complex systems of great importance for energy harvesting furthers the computational science community towards the goal of advancing national prosperity and welfare. The project makes these techniques freely available for a broad community, including documentation and tutorials, and trains the next generation of computational researchers through organizing summer schools and workshops.This project leverages a multi-organizational team to benefit from synergies that emerge from two possible solutions to current scientific barriers: Descriptions of exchange and correlation based on a long-range correction and on hybrid functionals that can scale favorably even for large systems with thousands of electrons are implemented and applied. Descriptions of non-adiabatic dynamics are implemented and applied to study long-term dynamics of excitons during which the interaction with the nuclei becomes important. Doing so within a cutting-edge electronic-structure code that runs efficiently on graphics processing units, provides a unique opportunity to compare accuracy, applicability to a broad range of systems, and computational cost. Knowledge on the reliability of these approximations and their computational cost for extended systems of practical relevance, including complex heterogeneous systems like semiconductor-molecule interfaces, are advanced by this research. The efforts include building, increasing, and growing a skilled community especially of US based researchers in a recurrent summer school.This proposal receives funds through the Office of Advanced Cyberinfrastructure in the Computer and Information Science and Engineering Directorate and the Division of Materials Research in the Mathematical and Physical Sciences Directorate.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.