Understanding the Cavity Born-Oppenheimer Approximation

• URL: http://arxiv.org/abs/2401.03532v1
• Date: Sun, 7 Jan 2024 16:05:18 GMT
• Title: Understanding the Cavity Born-Oppenheimer Approximation
• Authors: Marit R. Fiechter and Jeremy O. Richardson
• Abstract summary: vibrational strong coupling between molecular vibrations and light modes can significantly change molecular properties. We show that we can recover CBO energies and spectra to high accuracy using only out-of-cavity quantities.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Experiments have demonstrated that vibrational strong coupling between molecular vibrations and light modes can significantly change molecular properties, such as ground-state reactivity. Theoretical studies towards the origin of this exciting observation can roughly be divided in two categories, with studies based on Hamiltonians that simply couple a molecule to a cavity mode via its ground-state dipole moment on the one hand, and on the other hand ab initio calculations that self-consistently include the effect of the cavity mode on the electronic ground state within the cavity Born-Oppenheimer (CBO) approximation; these approaches are not equivalent. The CBO approach is more rigorous, but unfortunately it requires the rewriting of electronic-structure code, and gives little physical insight. In this work, we exploit the relation between the two approaches and demonstrate on a real molecule (hydrogen fluoride) that for realistic coupling strengths, we can recover CBO energies and spectra to high accuracy using only out-of-cavity quantities from standard electronic-structure calculations. In doing so, we discover what the physical effects underlying the CBO results are. Our methodology can aid in incorporating more, possibly important features in models, play a pivotal role in demystifying CBO results and provide a practical and efficient alternative to full CBO calculations.

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