CAREER: Quantum-mechanical methods for electronic excited states in complex systems

职业：复杂系统中电子激发态的量子力学方法

• 批准号: 1554354
• 负责人: Albert DePrince
• 金额: $ 47.34万
• 依托单位: Florida State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-05-01 至 2022-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1554354&HistoricalAwards=false
• 关键词: CAREER; Quantum; mechanical; methods; electronic; CAREER; Quantum; mechanical; methods; electronic

Professor Eugene DePrince of Florida State University is funded by the Chemical Theory, Models, and Computational Methods program of the Chemistry Division to develop new theories and computer algorithms to aid in the description of the electronic structure of complex molecules and materials. Dr. DePrince and his group are developing techniques that describe a system with many electrons using an approach (two-electron reduced-density matrix: 2-RDM) that reduces the problem to two electrons, rather than the more familiar and complicated many-electron techniques. Because the 2-RDM approach is more compact than the many-electron wave function, these methods enable large computations on complex systems that are not possible using conventional approaches. The theories and algorithms being developed facilitate the discovery and characterization of novel molecules and materials relevant energy conversion, catalysis, and advanced energy storage technologies. Professor DePrince is also developing Chemical Physics courses, a lecture series, and online educational content with the goal of establishing a Chemical Physics PhD track in the Department of Chemistry and Biochemistry at Florida State University.The project aims to develop a theoretical and computational framework for the description of electronically excited states in complex systems. Here, the term complex refers to systems that fall into one of two categories: (i) molecules whose electronic wave functions cannot be described qualitatively by a single electronic configuration (i.e. strongly correlated systems) or (ii) molecules embedded in extreme environments, such as those in the vicinity of a plasmonic nanoparticle, where intense external electric fields can significantly perturb the electron density for the molecule. For the former category, frequency- and time-domain methods are being developed to extract excited-state information from variational two-electron reduced-density matrix (2-RDM)-driven complete active space self-consistent field computations. For the latter category, the investigator and his group are developing fully-quantum mechanical approaches that simulate plasmon-molecule interactions in the time domain. Because the plasmon is modeled in a quantum-mechanical way, such an approach captures quantum-mechanical effects, such as entanglement and coherences between plasmon excitations. Professor DePrince places the codes developed as part of this research effort in the public domain in either free or commercial electronic structure packages. Making these codes available to the public facilitates the discovery of novel materials and the advancement of the numerical methods developed throughout the project.

佛罗里达州立大学的尤金·德里丝教授由化学理论，模型和计算方法计划提供资金，以开发新的理论和计算机算法，以帮助描述复杂分子和材料的电子结构。 Deprince博士及其小组正在开发技术，这些技术用方法（两电子降低密度矩阵：2-RDM）来描述许多电子，从而将问题降低到两个电子，而不是更熟悉和复杂的多电子技术。 由于2-RDM方法比许多电子波函数更紧凑，因此这些方法可以在复杂系统上进行大型计算，而这些计算是不可能使用常规方法的。 开发的理论和算法有助于发现和表征新颖的分子和材料相关的能量转换，催化和先进的储能技术。 Deprince教授还正在开发化学物理课程，讲座系列和在线教育内容，其目的是在佛罗里达州立大学的化学和生物化学系中建立化学物理学博士学位轨道。该项目旨在开发一个理论和计算框架，以描述复杂系统中电子激发州的描述。 在这里，复合术语是指属于两类的系统：（i）无法通过单个电子配置（即强相关系统）或（ii）分子嵌入极端环境中的分子，例如在极端的纳米机构中涉及摩尔电位的高质量，这些分子无法定性地描述。对于前一种类别，正在开发频率和时域方法，以从变量两电子降低密度矩阵（2-RDM）驱动的完整的活跃空间自洽的场计算中提取激发状态信息。 对于后一种类别，研究者及其小组正在开发完全量词的机械方法，以模拟时域中的等离激子分子相互作用。由于等离子是以量子力学方式建模的，因此这种方法捕获了量子力学效应，例如纠缠和等离子体激发之间的连贯性。 Deprince教授将根据免费或商业电子结构包的公共领域中的这项研究工作的一部分开发了代码。将这些代码提供给公众，促进了新型材料的发现以及整个项目中开发的数值方法的进步。