Linear and nonlinear exciton dynamics with time-dependent density-functional theory

具有瞬态密度泛函理论的线性和非线性激子动力学

• 批准号: 2149082
• 负责人: Carsten Ullrich
• 金额: $ 39万
• 依托单位: University of Missouri-Columbia
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-03-01 至 2025-02-28
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2149082&HistoricalAwards=false
• 关键词: Linear; nonlinear; exciton; dynamics; time

NON-TECHNICAL SUMMARYThe interaction of light and matter is of fundamental importance in science and technology: it determines the characterization of materials through optical spectroscopy, forms the basis of photovoltaics as a renewable energy resource, and opens up new technologies in the area of quantum information. This award supports research and education activities with an aim to develop theoretical and computational methods for modeling light-matter interactions that are more accurate and efficient than existing approaches.When light gets absorbed in a material, electrons are excited into higher states, leaving positively charged “hole” states behind. The electrons and holes can team up and form pairs, called excitons, which give rise to characteristic spectroscopic features and often dominate the optical properties of materials. The theoretical and computational description of excitonic effects is challenging, since the electron-hole pairs exist within a solid-state environment of many electrons, and are influenced by subtle interaction effects between them. This project will especially focus on such interactions in two-dimensional materials.This project will utilize a quantum-mechanical method called time-dependent density-functional theory, which has been very successful in describing the dynamics of interacting electronic systems in many areas in physics, chemistry and materials science. Within this theoretical framework, the PI will develop new ways of accounting for the quantum behavior of many-electron systems in two-dimensional materials. Another focus will be on a real-time description of light-matter interactions that explicitly accounts for fast dynamical effects which allow the simulation of experiments probing exciton dynamics on very short time scales in 2D materials.The research activities will go hand in hand with educational efforts focusing on the training and mentoring of graduate students and postdocs and the development of innovative teaching methods. An open-source library of computer simulations will be developed, to be used as teaching tools for introductory courses in density-functional theory. This addresses a clear need to make these advanced quantum mechanical topics more accessible to learners from various backgrounds.TECHNICAL SUMMARYThis award supports theoretical and computational research and education activities with an aim to develop and apply time-dependent density-functional theory (TDDFT) based approaches for excitons in the linear and nonlinear regime. The first research goal is to extend the long-range corrected and the dielectrically screened hybrid functional based approaches to describe excitons at finite momentum and in two-dimensional (2D) materials. This requires the development of long-range corrected exchange-correlation functionals with explicit matrix form in reciprocal space, and of hybrid functionals that use momentum-dependent dielectric screening models. These methods will be applied to describe dark excitons, which are potential candidates for qubits in future quantum information devices. The second goal is to describe ultrafast and nonlinear excitonic effects in real time via the time-dependent Kohn-Sham equation for solids. This will be accomplished through a time-dependent version of the long-range corrected exchange-correlation functional, suitably modified to enforce the so-called zero-force theorem, and via hybrid functionals with explicitly time-dependent dielectric screening. These methods will be developed and tested with the help of 2D model systems, and they will be implemented in two codes, INQ and Octopus. Applications will address exciton formation and dynamics in 2D materials, the dynamical Franz-Keldysh effect, and excitonic effects in high-harmonic generation. The research activities will go hand in hand with educational efforts focusing on the training and mentoring of graduate students and postdocs and the development of innovative teaching methods. An open-source library of Python-based computer simulations will be developed, to be used as teaching tools for introductory courses in density-functional theory. This addresses a clear need to make TDDFT more accessible to learners from various backgrounds.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.

光与物质的相互作用在科学和技术中具有根本的重要性：它通过光学光谱确定材料的特性，形成作为可再生能源的光化学的基础，并开辟了量子信息领域的新技术。该奖项支持研究和教育活动，旨在开发比现有方法更准确和有效的光-物质相互作用建模的理论和计算方法。当光被材料吸收时，电子被激发到更高的状态，留下带正电的“空穴”状态。电子和空穴可以组合并形成对，称为激子，其产生特征光谱特征，并且通常主导材料的光学性质。激子效应的理论和计算描述是具有挑战性的，因为电子-空穴对存在于许多电子的固态环境中，并且受到它们之间的微妙相互作用效应的影响。本项目将特别关注二维材料中的这种相互作用，本项目将利用一种称为时间依赖密度泛函理论的量子力学方法，该方法在物理学、化学和材料科学的许多领域中非常成功地描述了相互作用的电子系统的动力学。在这个理论框架内，PI将开发新的方法来解释二维材料中多电子系统的量子行为。另一个重点将是光-物质相互作用的实时描述，明确说明快速动力学效应，从而允许在二维材料中模拟在非常短的时间尺度上探测激子动力学的实验。研究活动将与教育工作齐头并进，重点是研究生和博士后的培训和指导以及创新教学方法的发展。将开发一个开放源码的计算机模拟图书馆，用作密度泛函理论入门课程的教学工具。这解决了一个明确的需要，使这些先进的量子力学课题更容易为学习者从不同的背景。技术总结该奖项支持理论和计算研究和教育活动，旨在开发和应用依赖于时间的密度泛函理论（TDDFT）为基础的方法激子在线性和非线性政权。第一个研究目标是扩展远程校正和介电屏蔽混合功能的方法来描述激子在有限动量和二维（2D）材料。这就需要开发长程校正交换相关泛函与明确的矩阵形式在倒易空间，和混合泛函，使用动量依赖的介电屏蔽模型。这些方法将被应用于描述暗激子，这是未来量子信息器件中量子比特的潜在候选者。第二个目标是描述超快和非线性激子效应在真实的时间通过时间依赖的Kohn-Sham方程的固体。这将是通过一个时间依赖版本的远程校正交换相关功能，适当修改，以执行所谓的零力定理，并通过混合泛函与明确的时间依赖性介电屏蔽。这些方法将在2D模型系统的帮助下开发和测试，并将在INQ和Octopus两个代码中实现。应用程序将解决激子的形成和动力学在二维材料，动态Franz-Keldysh效应，激子的高次谐波产生的影响。研究活动将与教育工作齐头并进，重点是研究生和博士后的培训和指导以及创新教学方法的发展。将开发一个基于Python的计算机模拟开源库，用作密度泛函理论入门课程的教学工具。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

DFT exchange: sharing perspectives on the workhorse of quantum chemistry and materials science.

• DOI: 10.1039/d2cp02827a
• 发表时间: 2022-12-07
• 期刊: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
• 影响因子: 3.3
• 作者: Teale, Andrew M.;Helgaker, Trygve;Savin, Andreas;Adamo, Carlo;Aradi, Balint;Arbuznikov, Alexei, V;Ayers, Paul W.;Baerends, Evert Jan;Barone, Vincenzo;Calaminici, Patrizia;Cances, Eric;Carter, Emily A.;Chattaraj, Pratim Kumar;Chermette, Henry;Ciofini, Ilaria;Crawford, T. Daniel;De Proft, Frank;Dobson, John F.;Draxl, Claudia;Frauenheim, Thomas;Fromager, Emmanuel;Fuentealba, Patricio;Gagliardi, Laura;Galli, Giulia;Gao, Jiali;Geerlings, Paul;Gidopoulos, Nikitas;Gill, Peter M. W.;Gori-Giorgi, Paola;Gorling, Andreas;Gould, Tim;Grimme, Stefan;Gritsenko, Oleg;Jensen, Hans Jorgen Aagaard;Johnson, Erin R.;Jones, Robert O.;Kaupp, Martin;Koster, Andreas M.;Kronik, Leeor;Krylov, Anna, I;Kvaal, Simen;Laestadius, Andre;Levy, Mel;Lewin, Mathieu;Liu, Shubin;Loos, Pierre-Francois;Maitra, Neepa T.;Neese, Frank;Perdew, John P.;Pernal, Katarzyna;Pernot, Pascal;Piecuch, Piotr;Rebolini, Elisa;Reining, Lucia;Romaniello, Pina;Ruzsinszky, Adrienn;Salahub, Dennis R.;Scheffler, Matthias;Schwerdtfeger, Peter;Staroverov, Viktor N.;Sun, Jianwei;Tellgren, Erik;Tozer, David J.;Trickey, Samuel B.;Ullrich, Carsten A.;Vela, Alberto;Vignale, Giovanni;Wesolowski, Tomasz A.;Xu, Xin;Yang, Weitao
• 通讯作者: Yang, Weitao

Retardation effects in atom-wall interactions

原子-壁相互作用的延迟效应

• DOI: 10.1103/physreva.109.022808
• 发表时间: 2024
• 期刊: Physical Review A
• 影响因子: 2.9
• 作者: Das, T.;Ullrich, C. A.;Jentschura, U. D.
• 通讯作者: Jentschura, U. D.