Quantum systems host spectacular excited-state effects, but many of these phenomena remain challenging to control and, consequently, technologically under-explored. By creating predictive approaches to study dynamics, decoherence and photo-induced correlations in molecules and matter, our work could enable technologies that are inherently more powerful than their classical counterparts ranging from quantum information science, to ultra-high efficiency optoelectronic and energy conversion systems. In this talk, I will present work from my research group on describing, from first principles approaches, the microscopic dynamics and optically-excited collective phenomena at finite temperature in quantum systems. Capturing these dynamics poses unique theoretical and computational challenges. The simultaneous contribution of processes that occur on many time and length-scales have remained elusive for state-of-the-art calculations and model Hamiltonian approaches alike, necessitating the development of new methods in theoretical and computational quantum chemistry. I will introduce our work at the intersection of ab initio cavity quantum-electrodynamics and electronic structure methods to treat electrons, photons and phonons on the same quantized footing, accessing new observables in strong light-matter coupling. Building on this, I will show selected examples of our approach in driving quantum chemical systems far out-of-equilibrium to control the coupled electronic and vibrational degrees-of-freedom.

Predicting strongly correlated light-quantum matter interactions

ACS Fall 2021

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