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

光腔中的量子化辐射场与电子态耦合产生极化激元态，极化激元态由分子间的集体激发和离域激发以及腔模组成。 由于形成极化子态已被证明可以促进新的化学反应，极化子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，并提供了一种新的范式，用于实现可以深刻影响催化、能源生产和整个化学领域的化学转化。计算机模拟在理解这一新兴领域的新原理方面发挥着至关重要的作用。模拟这种混合物质场系统的时间相关极化子量子动力学是一项必要和基本的任务，因为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。这个项目的首要目标是提供一个软件基础设施，以促进这种模拟的时间依赖极化激元量子动力学。为实现这一目标，在开放源码软件包内开发了软件要素。 特别是，软件模块在开源电子结构包中实现，以提供从头算量子力学和基于半经验的描述的极化激元态和暗态。同时，表面跳跃和基于波包的极化激元非绝热量子动力学方法在开源电子动力学软件包中实现，因此，可以使用电子结构和非电子结构之间的界面来常规地进行有效和准确的极化子量子动力学模拟。绝热动力学软件包。该奖项由NSF高级网络基础设施办公室颁发，由化学部和材料部联合支持。研究。该奖项反映了NSF的法定使命，并被认为是值得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的支持。

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.