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

电子态与光学腔内量子化辐射场耦合产生极化激子态，极化激子态由分子间的集体激发和离域激发以及腔模式组成。由于形成极化态已被证明可以促进新的化学反应，极化化学提供了一种通过调整光子的基本性质来控制化学反应的新策略，并为实现化学转化提供了一种新的范式，这种化学转化可以深刻地影响催化、能源生产和整个化学领域。计算机模拟在理解这一新兴领域的新原理方面起着至关重要的作用。由于这些极化子光化学反应通常涉及电子、核和光子自由度之间复杂的动力学相互作用，因此模拟这种混合物质场系统的随时间变化的极化子量子动力学是一项必要和必不可少的任务。这个项目的首要目标是提供一个软件基础设施，以促进这种时间依赖的极化量子动力学的模拟。为了实现这一目标，在开源软件包中开发软件元素。特别是，软件模块在开源电子结构包中实现，提供从头算量子力学和基于半经验的极化态和暗态描述。同时，在开源的电子动力学包中实现了基于表面跳变和波包的极化子非绝热量子动力学方法，从而可以利用电子结构和非绝热动力学包之间的界面进行高效、准确的极化子量子动力学模拟。该奖项由美国国家科学基金会高级网络基础设施办公室颁发，由化学部门和材料研究部门共同支持。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.