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教授得到了化学理论，模型和计算方法（CTMC）的奖项，以调查现代纳米级材料和旨在用于太阳能收集和光电的应用程序的超快过程。光伏，光催化，电子学，成像，检测以及新兴的旋转型，等离子体，等离子体，瓣膜和量子信息技术的进一步进展，需要设备小型化并涉及非常快的时间表。为了促进这些领域，Oleg Prezhdo的小组已经率先开发，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良好的时间分辨率对新材料和过程进行建模。这种建模将最亲密地模仿它们在自然界中发生的关键现象，提供实验数据的基本解释，并指导材料和设备设计中的未来努力。理论研究对于推进对我们社会未来至关重要的技术至关重要。prepsoroleg prezhdo及其小组将开发针对非绝热分子动力学的新型理论和仿真方法，并在实时时间依赖于时间依赖的密度功能理论中实现它们，并在现代Nansoscale材料材料和多组分中研究激发的状态动力学。将理论和应用结合的平衡程序将提供时间域中的光启动动态以及与实验的直接联系和协作。方法开发和实施将集中于经过改进的Ehrenfest型方法，Liouville Space Surface Hopping方法，Lindblad和Pauli Master方程，并具有表面跳跃速率，以及机器学习分析和非绝热分子动力学的加速。这些应用包括对金属卤化物钙钛矿中激发状态动力学的研究，过渡金属二甲构元和二维材料，金属和半导体量子点以及包括其中几种材料在内的杂种。这样的材料和系统在太阳能收集和光电子学中找到了重要的应用。 Oleg Prezhdo的工作促进了量子动态的基本方面，并在纳米级上的兴奋和指控转移中解决了实际问题。该奖项反映了NSF的法定任务，并通过基金会的知识分子优点和更广泛的影响标准通过评估来诚实地对支持进行评估。

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
• 期刊: Journal of Materials Chemistry A
• 影响因子: 11.9
• 作者: Zhu, Yonghao;Fang, Wei-Hai;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
• 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

Breaking Phonon Bottlenecks through Efficient Auger Processes in Perovskite Nanocrystals

• DOI: 10.1021/acsnano.2c12220
• 发表时间: 2023-02-16
• 期刊: ACS NANO
• 影响因子: 17.1
• 作者: Baker, Harry;Perez, Carlos Mora;Kambhampati, Patanjali
• 通讯作者: Kambhampati, Patanjali

Ab initio quantum dynamics of plasmonic charge carriers

• DOI: 10.1016/j.trechm.2023.02.010
• 发表时间: 2023-03
• 期刊: Trends in Chemistry
• 影响因子: 15.7
• 作者: Wei Li;Ting Xue;Carlos Mora-Perez;O. Prezhdo

Control of Hot Carrier Cooling in Lead Halide Perovskites by Point Defects

• DOI: 10.1021/jacs.2c08487
• 发表时间: 2022-09-20
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Zhou, Zhaobo;He, Junjie;Wang, Jinlan
• 通讯作者: Wang, Jinlan