Time-Domain Atomistic Theory and Simulation of Excitation Dynamics on the Nanoscale

时域原子理论与纳米尺度激发动力学模拟

• 批准号: 1900510
• 负责人: Oleg Prezhdo
• 金额: $ 51.2万
• 依托单位: University of Southern California
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-07-01 至 2023-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1900510&HistoricalAwards=false
• 关键词: Time; Domain; Atomistic; Theory; Simulation

Oleg V. Prezhdo of the University of Southern California is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop computational approaches to study nanoscale materials. The award is cofunded by the Condensed Matter and Materials Theory program in the Division of Materials Research. Studying matter at the nanoscale allows scientists and engineers to develop smaller and faster electronic and electro-optic devices. These devices have many technological benefits. For example, they can improve the efficiency and lower the cost of solar cells. Many new technologies, such as those relevant to quantum information science also emerge from nanoscale research. Bridging the gap between molecular and bulk scales, nanoscale materials exhibit novel phenomena. An atom-level description and fine time-resolution are needed to understand these phenomena. To gain this detailed understanding, Professor Prezhdo and his research group develop novel theoretical methods and use them to study ultrafast dynamics in nanomaterials. This theoretical research is performed in close collaboration with experimentalists. The current focus of the Prezhdo group is on hybrid organic/inorganic perovskites, which show record solar cell efficiencies, as well as on two-dimensional materials, such as metal dichalcogenides and black phosphorus, which can lead to the development of devices that are just a few atoms in thickness. Professor Prezhdo is engaged at curriculum development aimed at increasing student involvement in energy sciences.These studies are rooted in the recent advances in nonadiabatic (NA) and semi-classical molecular dynamics (MD), and their implementation within time-domain density functional theory (TDDFT). The focus is on the investigation of the fundamental questions posed in the recent time resolved experiments performed on nanoscale materials. Specific attention is given to the development and testing of new simulation approaches and algorithms for NAMD with focus on rigor, accuracy, efficiency and applicability to large systems, which undergo practically important non-equilibrium processes involving excited electronic states and ultrafast timescales. The implementation and testing of the NAMD approaches within TDDFT with the goal of extending the applicability of NAMD to new problems and larger systems is also a goal of this research. The larger systems have electronic structure can be described by ab initio and tight binding DFT, including a new family of NAMD techniques (Liouville space NAMD) and types of processes (many-particle and spin-orbit interactions). Finally, the study of the excitation dynamics in two-dimensional materials and halide perovskites, which are under intense experimental investigation are investigated. These materials carry great promise for photovoltaic, photocatalytic, electronic, spintronic, plasmonic, valleytronic and related technologies, underlying future societal advances in energy harvesting and information processes.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 V. Prezhdo得到了化学系化学理论、模型和计算方法项目的一个奖项的支持，以开发研究纳米材料的计算方法。 该奖项由材料研究部的凝聚态物质和材料理论项目共同资助。 在纳米尺度上研究物质可以使科学家和工程师开发出更小更快的电子和电光设备。 这些设备具有许多技术优势。 例如，它们可以提高太阳能电池的效率并降低成本。 许多新技术，如与量子信息科学相关的技术，也是从纳米研究中产生的。 纳米材料是分子尺度和体尺度之间的差距，它表现出许多新的现象。 要理解这些现象，需要原子级的描述和精细的时间分辨率。 为了获得这种详细的理解，Prezhdo教授和他的研究小组开发了新的理论方法，并使用它们来研究纳米材料中的超快动力学。 这项理论研究是与实验学家密切合作进行的。 Prezhdo小组目前的重点是混合有机/无机钙钛矿，它显示出创纪录的太阳能电池效率，以及二维材料，如金属二硫属化物和黑磷，这可以导致开发厚度只有几个原子的设备。Prezhdo教授致力于课程开发，旨在提高学生对能源科学的参与。这些研究植根于非绝热（NA）和半经典分子动力学（MD）的最新进展，以及它们在时域密度泛函理论（TDDFT）中的实现。重点是在最近的时间解决纳米材料上进行的实验所提出的基本问题的调查。特别注意的是开发和测试的新的模拟方法和算法NAMD专注于严谨性，准确性，效率和适用性的大型系统，这经历了实际上重要的非平衡过程，涉及激发电子态和超快的时间尺度。 在TDDFT中实施和测试NAMD方法，以将NAMD的适用性扩展到新问题和更大的系统，这也是本研究的目标。 具有电子结构的较大系统可以通过从头算和紧束缚DFT来描述，包括新的NAMD技术家族（Liouville空间NAMD）和过程类型（多粒子和自旋轨道相互作用）。最后，对二维材料和卤化物钙钛矿中激发动力学的研究进行了深入的实验研究。 这些材料为光伏、光催化、电子、自旋电子、等离子体、谷电子和相关技术带来了巨大的希望，为能源收集和信息处理的未来社会进步奠定了基础。该奖项反映了NSF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。

项目成果

Significance of the Chemical Environment of an Element in Nonadiabatic Molecular Dynamics: Feature Selection and Dimensionality Reduction with Machine Learning

• DOI: 10.1021/acs.jpclett.1c03469
• 发表时间: 2021-12-09
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY LETTERS
• 影响因子: 5.7
• 作者: Bin How, Wei;Wang, Bipeng;V. Prezhdo, Oleg
• 通讯作者: V. Prezhdo, Oleg

Tuning charge transfer and recombination in exTTF/CNT nanohybrids by choice of chalcogen: A time-domain density functional analysis

• DOI: 10.1063/5.0034561
• 发表时间: 2021-01
• 期刊: Journal of Applied Physics
• 影响因子: 3.2
• 作者: Ritabrata Sarkar;Md Habib;Sougata Pal;O. Prezhdo

Ultrafast charge transfer coupled to quantum proton motion at molecule/metal oxide interface

分子/金属氧化物界面处与量子质子运动耦合的超快电荷转移

• DOI: 10.1126/sciadv.abo2675
• 发表时间: 2022-06-17
• 期刊: SCIENCE ADVANCES
• 影响因子: 13.6
• 作者: Chu, Weibin;Tan, Shijing;Zhao, Jin
• 通讯作者: Zhao, Jin

Influence of intrinsic defects on the structure and dynamics of the mixed Pb–Sn perovskite: first-principles DFT and NAMD simulations

固有缺陷对混合 Pb-Sn 钙钛矿结构和动力学的影响：第一性原理 DFT 和 NAMD 模拟

• DOI: 10.1039/d1ta09027e
• 发表时间: 2021
• 期刊: Journal of Materials Chemistry A
• 影响因子: 11.9
• 作者: Liu, Qi;Li, Akang;Chu, Weibin;Prezhdo, Oleg V.;Liang, WanZhen
• 通讯作者: Liang, WanZhen

Mixed Metals Slow Down Nonradiative Recombination in Saddle-Shaped Porphyrin Nanorings: A Time-Domain Atomistic Simulation

• DOI: 10.1021/acs.jpcc.1c04749
• 发表时间: 2021-08
• 期刊: The Journal of Physical Chemistry C
• 作者: Ritabrata Sarkar;M. Habib;S. Kovalenko;Sougata Pal;O. Prezhdo