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.

非技术总结在科学和技术中，光与物质的相互作用至关重要：它通过光谱法确定了材料的特征，构成了光伏电源作为可再生能源的基础，并在量子信息领域开放了新技术。该奖项支持研究和教育活动，目的是开发理论和计算方法，用于建模比现有方法更准确和更有效的光结合相互作用。当光吸收到材料中时，电子会激发到更高的状态，从而使带电的“孔”状态产生。电子和孔可以组合并形成称为激子的对，这会产生特征性的光谱特征，并经常主导材料的光学特性。令人兴奋效应的理论和计算描述具有挑战性，因为电子孔对存在于许多电子设备的固态环境中，并且受其之间微妙的相互作用效应的影响。该项目将特别关注二维材料中的这种相互作用。该项目将利用一种称为时间依赖的密度功能理论的量子力学方法，该方法在描述物理，化学和材料科学领域许多领域相互作用的电子系统的动态方面非常成功。在这个理论框架内，PI将开发新的方式来计算二维材料中多电子系统的量子行为。另一个重点将是对光线相互作用的实时描述，这些相互作用明确说明了快速动态效应，这些效果允许模拟2D材料中非常短的时间尺度上探索令人兴奋的动态的实验。研究活动将与教育努力齐头并进，重点关注研究生和研究生的培训和心理，以及创新的教学方法的发展。将开发一个开源的计算机模拟库，以用作介绍密度功能理论课程的教学工具。该地址明确需要使这些先进的量子机械主题更容易被各种背景学习。摘要摘要这一奖项支持理论和计算研究和教育活动，旨在开发和应用时间相关的密度功能理论（TDDDFT）基于线性和非线性制度的基于激进的方法。第一个研究目标是扩展远程校正和稍微筛选的基于混合功能的方法，以描述有限动量和二维（2D）材料的激子。这就需要在相互空间中具有显式矩阵形式的远程校正交换相关功能以及使用动量依赖性词典筛选模型的混合功能。这些方法将应用于描述深色激子，这些激发子是未来量子信息设备中数量的潜在候选者。第二个目标是通过时间依赖的固体方程来实时描述超快和非线性刺激效果。这将通过远程校正的交换相关功能的时间相关版本来实现，并适当修改以执行所谓的零强制定理，以及通过具有明确时间与时间相关的动态筛选的混合功能。这些方法将在2D模型系统的帮助下开发和测试，并将在两个代码INQ和章鱼中实现。应用将解决2D材料中的Inventon组和动力学，动态的Franz-keldysh效果以及高谐波产生的激动人心的效果。研究活动将与教育努力息息相关，重点是对研究生和博士后的培训和心理，以及创新教学方法的发展。将开发一个基于Python的计算机模拟的开源库，用作介绍密度功能理论课程的教学工具。该奖项明确地解决了从各种背景的学习者更容易获得TDDFT的需求。该奖项反映了NSF的法定任务，并且使用基金会的知识分子优点和更广泛的影响评估标准，被认为是通过评估来获得的支持。

项目成果

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.

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