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

纳米级系统非绝热激发态动力学的理论与模拟

• 批准号: 2154367
• 负责人: Oleg Prezhdo
• 金额: $ 51万
• 依托单位: University of Southern California
• 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: 2022-05-01 至 2025-04-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2154367&HistoricalAwards=false
• 关键词: Theory; Simulation; Non; adiabatic; Excited

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.

南加州大学的 Oleg Prezhdo 教授获得了化学系化学理论、模型和计算方法 (CTMC) 项目的资助，以研究旨在太阳能收集和光电应用的现代纳米级材料和设备中的超快过程光伏、光催化、电子学、成像、检测以及新兴的自旋电子学、等离激元学、谷电子学和量子信息技术的进一步进展需要设备小型化并涉及为了推进这些领域的发展，Oleg Prezhdo 的团队开创了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。自然界中发生的关键现象，提供了对实验数据的基本解释，并指导未来材料和设备设计的努力，对于推进对我们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理论新颖和模拟方法，在实时依赖于时间的密度泛函理论中实现它们，并研究现代纳米级材料和多组分混合体中的激发态动力学。结合理论和应用的平衡程序将提供一个平衡程序。时域光激发动力学的详细原子图，并与实验直接联系和协作，该方法的开发和实施将侧重于改进的埃伦菲斯特型方法、刘维尔空间表面跳跃方法、林德布拉德和泡利方法。具有表面跳跃率的主方程，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、过渡金属二硫属化物和二维材料、金属和半导体量子点以及多种混合材料的激发态动力学研究。这些材料和系统在太阳能收集和光电子学方面有着重要的应用，它推进了量子动力学的基本方面，并解决了激发和电荷方面的实际问题。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

The twist angle has weak influence on charge separation and strong influence on recombination in the MoS 2 /WS 2 bilayer: ab initio quantum dynamics

扭转角对 MoS 2 /WS 2 双层中的电荷分离影响较弱，但对复合影响较大：从头算量子动力学

• DOI: 10.1039/d1ta10788g
• 发表时间: 2022-04
• 期刊: Journal of Materials Chemistry A
• 影响因子: 11.9
• 作者: Zhu, Yonghao;Fang, Wei;Rubio, Angel;Long, Run;Prezhdo, Oleg V.
• 通讯作者: Prezhdo, Oleg V.

Excitonic Quantum Coherence in Light Emission from CsPbBr 3 Metal-Halide Perovskite Nanocrystals

CsPbBr 3 金属卤化物钙钛矿纳米晶体发光中的激子量子相干性

• DOI: 10.1021/acs.nanolett.3c03180
• 发表时间: 2024-01
• 期刊: Nano Letters
• 影响因子: 10.8
• 作者: Strandell, Dallas;Mora Perez, Carlos;Wu, Yifan;Prezhdo, Oleg V.;Kambhampati, Patanjali
• 通讯作者: Kambhampati, Patanjali

Interlayer Charge Transport in 2D Lead Halide Perovskites from First Principles

第一原理中二维卤化铅钙钛矿的层间电荷传输

• DOI: 10.1021/acs.jctc.3c00904
• 发表时间: 2023-12
• 期刊: Journal of Chemical Theory and Computation
• 影响因子: 5.5
• 作者: Li, Wei;Giannini, Samuele;Quarti, Claudio;Hou, Zhufeng;Prezhdo, Oleg V.;Beljonne, David
• 通讯作者: Beljonne, David

Design of Boron and Transition Metal Embedded Two-Dimensional Porous Carbon Nitride for Electrocatalytic Synthesis of Urea

硼和过渡金属嵌入二维多孔氮化碳电催化合成尿素的设计

• DOI: 10.1021/jacs.3c12017
• 发表时间: 2024-01-10
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Cao, Xin;Zhang, Dewei;Gao, Yongqi;Prezhdo, Oleg V.;Xu, Lai
• 通讯作者: Xu, Lai

Tuning Octahedral Tilting by Doping to Prevent Detrimental Phase Transition and Extend Carrier Lifetime in Organometallic Perovskites

通过掺杂调节八面体倾斜以防止有害的相变并延长有机金属钙钛矿中的载流子寿命

• DOI: 10.1021/jacs.2c13593
• 发表时间: 2023-03
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Yin, Junwen;Xu, Zhongfei;Hu, Qi;Teobaldi, Gilberto;Liu, Li;Prezhdo, Oleg V.
• 通讯作者: Prezhdo, Oleg V.