Elements: An Integrated Software Platform for Simulating Polariton Photochemical and Photophysical Processes

Elements：用于模拟极化子光化学和光物理过程的集成软件平台

• 批准号: 2311442
• 负责人: Yihan Shao
• 金额: $ 59.96万
• 依托单位: University of Oklahoma Norman Campus
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-07-01 至 2026-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2311442&HistoricalAwards=false
• 关键词: Elements; Integrated; Software; Platform; Simulating

Coupling electronic states with the quantized radiation field inside an optical cavity creates polariton states, which are composed from the collective and delocalized excitations among molecules and the cavity mode. As forming polariton states have been shown to facilitate new chemical reactivities, polariton chemistry provides a new strategy to control chemical reactivities in a general way by tuning the fundamental properties of photons and provides a new paradigm for enabling chemical transformations that can profoundly impact catalysis, energy production, and the field of chemistry at large. Computer simulations play a crucial role in understanding the new principles in this emerging field. Simulating the time-dependent polariton quantum dynamics of such hybrid matter-field systems is a necessary and essential task, as these polariton photochemical reactions often involve a complex dynamical interplay among the electronic, nuclear, and photonic degrees of freedom. The overarching objective of this project is to provide a software infrastructure to facilitate such simulations of time-dependent polariton quantum dynamics. Towards the objective, software elements are developed within open-source software packages. In particular, software modules are implemented in open-source electronic structure packages to provide ab initio quantum mechanics and semi-empirical based descriptions for the polaritonic states and dark states. In parallel, surface-hopping and wavepacket-based polariton non-adiabatic quantum dynamics methods are implemented in open-source electron dynamics packages, so that efficient and accurate polariton quantum dynamics simulations can be carried out routinely using the interfaces between electron structure and non-adiabatic dynamics packages.This award by the NSF Office of Advanced Cyberinfrastructure is jointly supported by the Division of Chemistry and Division of Materials Research.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.

将电子状态与量化辐射场的耦合式光腔中产生偏振状态，这些状态是由分子之间的集体和离域激发组成的，并且是腔模式的。 由于已显示形成的极化状态可以促进新的化学反应率，因此Polariton Chemistry通过调整光子的基本特性来控制化学反应率的新策略，并为实现化学转化提供了新的范式，可以极大地影响催化，能量生产，能量生产和整个化学的领域。计算机模拟在理解这个新兴领域的新原理方面起着至关重要的作用。模拟此类混合物质领域系统的时间依赖性极化量子动力学是必不可少的和必不可少的任务，因为这些极性光化学反应通常涉及电子，核和光子自由度之间的复杂动力学相互作用。该项目的总体目的是提供软件基础架构，以促进有关时间依赖性极化量子动力学的模拟。针对目标，软件元素是在开源软件包中开发的。 特别是，软件模块以开源电子结构套件实现，以为极化状态和黑暗状态提供量子量的量子力学和基于半经验的描述。同时，在开源电子动力包中实施了并行，基于表面的偏振子非绝热量子动力学方法，因此可以通过电子结构和非化学动力学措施之间的insod cyberinfres ins nsfres insifres insfres ofdrond cyberinfrase insfress ofdrond cyberinfrase insf ofdrond cyberinfress of先生级拟曲，从而在开源电子动态套件中实现，以便进行有效，准确的极性量子量子动力学模拟。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛影响的评论标准来评估值得支持的。