Quantum to Classical Cavity Chemistry Electrodynamics

• URL: http://arxiv.org/abs/2312.06815v1
• Date: Mon, 11 Dec 2023 20:04:46 GMT
• Title: Quantum to Classical Cavity Chemistry Electrodynamics
• Authors: Leonardo F. Calder\'on, Humberto Trivi\~no, Leonardo A. Pach\'on
• Abstract summary: This work presents a quantum-classical approach addressing issues of realizing cavity chemistry effects without actual cavities. It is demonstrated that classical light sources can mimic quantum effects up to the second order of light-matter interaction. Numerical simulations show that the quantum-classical method aligns more closely with exact quantum molecular-only dynamics for quantum light states such as Fock states, superpositions of Fock states, and vacuum squeezed states than the conventional semiclassical approach.
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• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: Polaritonic chemistry has ushered in new avenues for controlling molecular dynamics. However, two key questions remain: (i) Can classical light sources elicit the same effects as certain quantum light sources on molecular systems? (ii) Can semiclassical treatments of light-matter interaction capture nontrivial quantum effects observed in molecular dynamics? This work presents a quantum-classical approach addressing issues of realizing cavity chemistry effects without actual cavities. It also highlights the limitations of the standard semiclassical light-matter interaction. It is demonstrated that classical light sources can mimic quantum effects up to the second order of light-matter interaction, provided that the mean-field contribution, symmetrized two-time correlation function, and the linear response function are the same in both situations. Numerical simulations show that the quantum-classical method aligns more closely with exact quantum molecular-only dynamics for quantum light states such as Fock states, superpositions of Fock states, and vacuum squeezed states than the conventional semiclassical approach.

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