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

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.