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

开发具有重要社会意义的能量获取方法，如光催化或光伏技术，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使用复杂的量子力学模拟来帮助获得这样的理解。然而，这样的科学努力需要开发准确的模拟技术，有效利用底层超级计算机硬件是至关重要的。该项目通过实施新技术来描述量子力学、电子-电子相互作用以及电子动力学与离子的相互作用，从而应对了这些突出的挑战。在图形处理单元上使用和测试这些新的发展，在为下一代超级计算机准备量子力学模拟的同时，促进了科学的发展。将这些先进的模拟应用于对能源收集具有重要意义的复杂系统的建模，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。该项目使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工作坊培训下一代计算研究人员。该项目利用一个多组织团队，从针对当前科学障碍的两种可能解决方案中出现的协同效应中受益：基于远程校正的交换和关联描述，以及即使对于具有数千个电子的大型系统也可以很好地扩展的混合泛函。实现了非绝热动力学的描述，并将其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这样做，提供了一个独特的机会来比较准确性、对广泛系统的适用性和计算成本。通过这项研究，对于具有实际意义的扩展系统，包括像半导体-分子界面这样的复杂多相系统，这些近似的可靠性及其计算成本方面的知识得到了提升。这些努力包括建立、增加和发展一个熟练的社区，特别是在定期的暑期学校中的美国研究人员。这项提议通过计算机和信息科学与工程局的高级网络基础设施办公室和数学和物理科学局的材料研究部获得资金。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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.