On-the-fly Cavity–Molecular Dynamics of Vibrational Polaritons

Key Points

• The aim is to simulate vibrational polaritons formed by coupling molecular vibrations to light in confined environments.
• Combined density functional tight-binding (DFTB) approach with light-matter Hamiltonian.
• Expanded beyond the long-wavelength approximation for enhanced accuracy.
• Conducted simulations to observe interactions between molecular vibrations and electromagnetic fields.
• Demonstrated effective coupling between molecular vibrations and cavity light modes.
• Revealed novel vibrational polariton behavior in confined systems.
• Highlighted the limitations of traditional models focused solely on long-wavelength approximations.