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High-harmonic generation under electronic strong coupling: A time-dependent combined quantum electrodynamics/quantum
Paul A Albrecht1, Eric W Fischer2, Tillmann Klamroth1
1Institut für Chemie, Universität Potsdam, Karl-Liebknecht-Straße 24-25, D-14476 Potsdam-Golm, Germany.
The Journal of Chemical Physics
|October 22, 2025
Summary
Strongly coupling atoms and molecules to cavity light modifies High-Harmonic Generation (HHG) spectra. This quantum electrodynamics study shows suppressed cutoffs and enhanced harmonics due to light-matter hybrid states called polaritons.
Area of Science:
- Quantum Optics
- Molecular Physics
- Quantum Electrodynamics
Background:
- Cavity quantum electrodynamics enables the creation of light-matter hybrid states (polaritons).
- Polaritons offer novel ways to control molecular electronic structure and dynamics.
- High-Harmonic Generation (HHG) is a sensitive probe of electron dynamics in intense laser fields.
Purpose of the Study:
- Investigate the impact of strong light-matter coupling on HHG spectra.
- Explore the influence of polaritons on molecular response to laser fields.
- Analyze spectral modifications in HHG due to cavity effects.
Main Methods:
- Theoretical model study employing the Pauli-Fierz Hamiltonian.
- Quantum Electrodynamics Time-Dependent Configuration Interaction (QED-TD-CI) method.
- Numerical exact treatment for a 1D hydrogen atom model.
Main Results:
- Observed suppression of the harmonic cutoff in HHG spectra.
- Harmonic cutoff suppression correlates with quantum light excitation in the cavity.
- Demonstrated enhancement of specific harmonics in the coupled system.
Conclusions:
- Strong coupling to cavity modes significantly alters HHG spectra.
- Polariton formation can lead to distinct spectral features in HHG.
- Cavity-enhanced molecular quantum dynamics offers new control pathways.
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