Ultrafast dynamics in the vicinity of quantum light-induced conical intersections

Abstract

Nonadiabatic effects appear due to avoided crossings or conical intersections that are either intrinsic properties in field-free space or induced by a classical laser field in a molecule. It was demonstrated that avoided crossings in diatomics can also be created in an optical cavity. Here, the quantized radiation field mixes the nuclear and electronic degrees of freedom creating hybrid field-matter states called polaritons. In the present theoretical study we go further and create conical intersections in diatomics by means of a radiation field in the framework of cavity quantum electrodynamics (QED). By treating all degrees of freedom, that is the rotational, vibrational, electronic and photonic degrees of freedom on an equal footing we can control the nonadiabatic quantum light-induced dynamics by means of conical intersections. First, the pronounced difference between the the quantum light-induced avoided crossing and the conical intersection with respect to the nonadiabatic dynamics of the molecule is demonstrated. Second, we discuss the similarities and differences between the classical and the quantum field description of the light for the studied scenario.

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Cited by in corpus (17)

• The Shape of the Electric Dipole Function Determines the Sub-Picosecond Dynamics of Anharmonic Vibrational Polaritons
• Reduced Density-Matrix Approach to Strong Matter-Photon Interaction
• Nonadiabatic phenomena in molecular vibrational polaritons
• Three-player polaritons: nonadiabatic fingerprints in an entangled atom-molecule-photon system
• Probing Light-Induced Conical Intersections by Monitoring Multidimensional Polaritonic Surfaces
• Cooperative molecular structure in polaritonic and dark states
• Pulse reverse-engineering for strong field-matter interaction
• Radiative Emission of Polaritons Controlled by Light-Induced Geometric Phase
• Coupling Polyatomic Molecules to Lossy Nanocavities: Lindblad versus Schrödinger description
• Classical and quantum light-induced non-adiabaticity in molecular systems
• Impact of Cavity on Molecular Ionization Spectra
• Extending Non-Perturbative Simulation Techniques for Open-Quantum Systems to Excited-State Proton Transfer and Ultrafast Non-Adiabatic Dynamics
• Impact of dipole self-energy on cavity-induced nonadiabatic dynamics
• Practical guide to the statistical mechanics of molecular polaritons
• Indirect probing of light-induced nonadiabatic dynamics in lossy nanocavities
• Polarized Fock States for Polariton Photochemistry
• Not dark yet: strong light-matter coupling can accelerate singlet fission dynamics