Theory and Simulation of Non-adiabatic Excited State Dynamics in Nanoscale systems

南加州大学的奥列格·普雷日多教授得到了化学部化学理论、模型和计算方法(CTMC)项目的支持，该项目旨在研究现代纳米材料和设备中的超快过程，旨在收集太阳能和光电子应用。在光伏、光催化、电子学、成像、检测以及新兴的自旋电子学、等离子激元、电子电子和量子信息技术方面的进一步进展，需要设备小型化，并且涉及非常快的时间尺度。为了推动这些领域的发展，奥列格·普雷日多的团队已经并将进一步开发理论和计算方法，使他们能够以原子精度和精细的时间分辨率对新材料和工艺进行建模。这个模型将最接近地模拟自然界中发生的关键现象，提供对实验数据的基本解释，并指导未来在材料和器件设计方面的努力。理论研究对于推动对我们的社会未来至关重要的技术至关重要。奥列格·普雷日多教授和他的团队将开发非绝热分子动力学的新的理论和模拟方法，在实时含时密度泛函理论中实现这些方法，并研究现代纳米材料和多组分杂化材料中的激发态动力学。理论和应用相结合的平衡程序将提供详细的、原子化的光激发动力学在时间域中的图景，并与实验直接联系和协作。方法的发展和实现将集中在改进的Ehrenfest型方法、Liouville-空间表面跳跃方法、具有表面跳跃速率的Lindblad和Pauli主方程以及非绝热分子动力学的机器学习分析和加速。这些应用包括金属卤化物钙钛矿、过渡金属二卤化物和二维材料、金属和半导体量子点以及包括其中几种材料的杂化材料的激发态动力学研究。这种材料和系统在太阳能收集和光电子学中有重要的应用。奥列格·普雷日多的工作推进了量子动力学的基本方面，并解决了纳米级激发和电荷转移方面的实际问题。这一奖项反映了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。

Professor Oleg Prezhdo of the University of Southern California is supported by an award from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry to investigate ultrafast processes in modern nanoscale materials and devices aimed at solar energy harvesting and optoelectronic applications. Further progress in photovoltaics, photocatalysis, electronics, imaging, detection, as well as in the emerging spintronics, plasmonics, valleytronics and quantum information technologies, requires device miniaturization and involves very fast timescales. In order to advance these fields, Oleg Prezhdo’s group has pioneered and will further develop theoretical and computational methods that allow them to model the new materials and processes with atomistic precision and fine time-resolution. This modeling will mimic most closely the key phenomena as they occur in nature, provide fundamental interpretation of the experimental data, and guide future efforts in design of materials and devices. The theoretical studies are essential for advancing the technologies that are critical for our society future.Professor Oleg Prezhdo and his group will develop novel theoretical and simulation approaches for nonadiabatic molecular dynamics, implementing them within real-time time-dependent density functional theory, and investigating excited state dynamics in modern nanoscale materials and multi-component hybrids. The balanced program combining theory and applications will provide a detailed, atomistic picture of the photo-excitation dynamics in time-domain, and in direct connection and collaboration with experiment. The methods development and implementation will focus on modified Ehrenfest-type methods, Liouville-space surface hopping approaches, Lindblad and Pauli master equations with surface hopping rates, and machine learning analysis and acceleration of nonadiabatic molecular dynamics. The applications include studies of excited state dynamics in metal halide perovskites, transition metal dichalcogenides and two-dimensional materials, metallic and semiconducting quantum dots, and hybrids including several of these materials. Such materials and systems find important applications in solar energy harvesting and optoelectronics. Oleg Prezhdo’s work advances the fundamental aspects of quantum dynamics and addresses practical questions in excitation and charge transfer on the nanoscale.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.