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）得到了化学理论，模型和计算方法计划的奖项，以开发理论工具，以描述强耦合的轻质系统。纳米夹子光子和分子系统之间的强烈相互作用会导致杂交光晶状体（称为极性子）的产生，这种状态可能显示出与其母体成分明显不同的化学和物理性质。这些极化状态的技术和化学应用是广泛的。最新的基于腔的催化，极化激光和基于等离子的光稳定的例子只能瞥见偏光层方法的化学和材料科学方法的变革潜力。为了使该领域充分实现其承诺，必须伴有对极性特征的性质的高质量理论描述。 Deprince集团将开发一个可靠，可靠且系统地改进的框架，用于从头开始描述极化结构。将要开发的理论和软件将填补现有的计算工具套件的空白，以对极化介导的过程进行高准确的描述。这样的工具有可能促进与光收集，超电导率和量子信息科学相关的新型基于极化的技术的合理设计。该程序下开发的所有软件将以免费和开源方式发布。根据该奖项，Deprince集团还将开发易于访问的在线教育材料，用于量子化学和计算机科学教育。 Deprince博士和他的团队将针对极化结构问题采取多体方法，重点是动作方程（EOM）耦合群集（CC）方法的层次结构。激发能源（EE），电离电位（IP）和电子亲和力（EA）EOM-CC理论和软件的极化配方将被开发，并应用于涉及腔体结合分子的各种问题。从头开始描述强和超强的轻度耦合，很少见，最近出现了多个多体方法的现有示例。鉴于未知的是在密度功能理论（DFT）的极性配方中功能功能的电子 - 光子交换相关性的确切形式，因此似乎在该程序下将开发的多体方法（例如EOM-CC方法）提供了通用唯一可靠的可靠和系统性地互动的途径的途径。利用基金会的知识分子和更广泛的影响审查标准。