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Understanding the polaritonic ground state in cavity quantum electrodynamics
Tor S Haugland1, John P Philbin2, Tushar K Ghosh3
1Department of Chemistry, Norwegian University of Science and Technology, 7491 Trondheim, Norway.
The Journal of Chemical Physics
|May 16, 2025
Summary
Strong light-matter interactions create molecular polaritons, enabling control over chemical reactions. Perturbation theory accurately predicts ground state energies in optical cavities, revealing new insights into polaritonic chemistry.
Area of Science:
- Quantum Chemistry
- Physical Chemistry
- Spectroscopy
Background:
- Molecular polaritons form from strong light-matter interactions, hybridizing molecules and light.
- This hybridization alters molecular properties and allows for external field-free control of chemical reactions.
Purpose of the Study:
- Investigate the impact of strong light-matter coupling on molecular electronic structure.
- Demonstrate the efficacy of perturbation theory for calculating polaritonic ground state energies.
- Explore cavity-induced intermolecular forces.
Main Methods:
- Utilized perturbative approaches, specifically Rayleigh-Schrödinger perturbation theory.
- Employed response functions for implementation.
- Compared results with ab initio cavity quantum electrodynamics methodologies.
Main Results:
- Rayleigh-Schrödinger perturbation theory accurately reproduces ground state energies in optical cavities.
- The method is effective across low and high cavity frequency regimes.
- Established relations between cavity-induced intermolecular forces and van der Waals forces.
Conclusions:
- Perturbation theory offers an accurate and straightforward method for studying molecular polaritons.
- Findings provide insights into manipulating ground-state polaritonic energy landscapes.
- Identified conditions for achieving modifications in molecular systems via light-matter coupling.
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