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arXiv · 2002.10461

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

Derek S. Wang·Tomáš Neuman·Johannes Flick·Prineha Narang
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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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quant-phphysics.chem-phphysics.comp-phphysics.optics

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Derek S. Wang, Tomáš Neuman, Johannes Flick, Prineha Narang. 2020-02-24. Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles. https://doi.org/10.1063/5.0036283

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