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Polaritonic Quantum Chemistry

极化子量子化学

基本信息

批准号：
2100984
负责人：
Albert DePrince
金额：
$ 44.47万
依托单位：
Florida State University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2021
资助国家：
美国
起止时间：
2021-06-01 至 2025-05-31
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2100984&HistoricalAwards=false
关键词：
Polaritonic Quantum Chemistry

项目摘要

Eugene DePrince of Florida State University is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop theoretical tools for the description of strongly-coupled light-matter systems. Strong interactions between nanoconfined photons and molecular systems can lead to the creation of hybrid light-matter states, known as polaritons, that may display remarkably different chemical and physical properties than their parent components. The technological and chemical applications of these polariton states are wide-ranging. Recent examples of cavity-based catalysis, polariton lasing, and plasmon-based photostabilization offer only a glimpse into the transformative potential of polaritonic approaches to chemistry and materials science. In order for the field to fully live up to its promise, the experimental realization of ultra-strong light-matter coupling must be accompanied by high-quality theoretical descriptions of the properties of polaritonic features. The DePrince group will develop a robust, reliable, and systematically improvable framework for the ab initio description of polaritonic structure. The theories and software that will be developed will fill a gap in the existing computational tool kit for the high-accuracy description of polariton-mediated processes. Such tools have the potential to facilitate the rational design of new polariton-based technologies relevant to light harvesting, super conductivity, and quantum information science. All software developed under this program will be released in a free and open-source manner. Under this award, the DePrince group also will be developing readily accessible online educational materials for quantum chemistry and computer science education. Dr. DePrince and his team will take a many-body approach to the polaritonic structure problem, with an emphasis on the equation-of-motion (EOM) coupled-cluster (CC) hierarchy of methods. Polaritonic formulations of excitation-energy (EE), ionization potential (IP), and electron affinity (EA) EOM-CC theory and software will be developed and applied to a variety of problems involving cavity-bound molecules. Ab initio descriptions of strong and ultra-strong light-matter coupling are rare, with only a few existing examples of many-body approaches to this problem having recently emerged. Given that the exact form of the electron-photon exchange-correlation functional in polaritonic formulations of density functional theory (DFT) is unknown, it appears that many-body methods such as the EOM-CC approaches that will be developed under this program offer the only route to universally reliable and systematically improvable descriptions of cavity-molecule interactions.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.

佛罗里达州立大学的尤金·德普林斯 (Eugene DePrince) 获得化学系化学理论、模型和计算方法项目的资助，致力于开发用于描述强耦合光物质系统的理论工具。纳米限制光子和分子系统之间的强烈相互作用可以导致混合光物质状态的产生，称为极化激元，其可能表现出与其母体成分显着不同的化学和物理特性。这些极化子态的技术和化学应用非常广泛。最近基于空腔的催化、极化子激光和基于等离激元的光稳定化的例子只能让我们一睹极化子方法对化学和材料科学的变革潜力。为了使该领域完全兑现其承诺，超强光-物质耦合的实验实现必须伴随着对极化子特征特性的高质量理论描述。 DePrince 小组将开发一个稳健、可靠且可系统改进的框架，用于从头开始描述极化子结构。将开发的理论和软件将填补现有计算工具包的空白，用于高精度描述极化子介导的过程。这些工具有可能促进与光收集、超导性和量子信息科学相关的基于极化子的新型技术的合理设计。根据该计划开发的所有软件都将以免费和开源的方式发布。根据该奖项，DePrince 集团还将开发易于访问的量子化学和计算机科学教育在线教育材料。 DePrince 博士和他的团队将采用多体方法来解决极化子结构问题，重点是运动方程 (EOM) 耦合簇 (CC) 方法层次结构。激发能 (EE)、电离势 (IP) 和电子亲和力 (EA) 的极化公式 EOM-CC 理论和软件将被开发并应用于涉及空腔束缚分子的各种问题。对强和超强光-物质耦合的从头开始的描述很少见，最近只出现了一些解决这个问题的多体方法的例子。鉴于密度泛函理论 (DFT) 极化子公式中电子光子交换相关泛函的确切形式尚不清楚，看来该计划下将开发的多体方法（例如 EOM-CC 方法）提供了普遍可靠且系统可改进的空腔分子相互作用描述的唯一途径。该奖项反映了 NSF 的法定使命，并被认为值得通过评估支持利用基金会的智力优势和更广泛的影响审查标准。