Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles

• URL: http://arxiv.org/abs/2002.10461v1
• Date: Mon, 24 Feb 2020 19:00:00 GMT
• Title: Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles
• Authors: Derek S. Wang, Tom\'a\v{s} Neuman, Johannes Flick, Prineha Narang
• Abstract summary: We generalize ab initio quantum-electrodynamical density functional theory to account for dissipative dynamics. We study excited-state dynamics and spectral responses of benzene and toluene under weak-to-strong light-matter coupling.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Cavity-mediated light-matter coupling can dramatically alter opto-electronic and physico-chemical properties of a molecule. Ab initio theoretical predictions of these systems need to combine non-perturbative, many-body electronic structure theory-based methods with cavity quantum electrodynamics and theories of open quantum systems. Here we generalize quantum-electrodynamical density functional theory to account for dissipative dynamics and describe coupled cavity-molecule interactions in the weak-to-strong-coupling regimes. Specifically, to establish this generalized technique, we study excited-state dynamics and spectral responses of benzene and toluene under weak-to-strong light-matter coupling. By tuning the coupling we achieve cavity-mediated energy transfer between electronic excited states. This generalized ab initio quantum-electrodynamical density functional theory treatment can be naturally extended to describe cavity-mediated interactions in arbitrary electromagnetic environments, accessing correlated light-matter observables and thereby closing the gap between electronic structure theory and quantum optics.

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