Driving chemical reactions with polariton condensates

Abstract

When molecular transitions strongly couple to photon modes, they form hybrid light-matter modes called polaritons. Collective vibrational strong coupling is a promising avenue for control of chemistry, but this can be deterred by the large number of quasi-degenerate dark modes. The macroscopic occupation of a single polariton mode by excitations, as observed in Bose-Einstein condensation, offers promise for overcoming this issue. Here we theoretically investigate the effect of vibrational polariton condensation on the kinetics of electron transfer processes. Compared with excitation with infrared laser sources, the condensate changes the reaction yield significantly due to additional channels with reduced activation barriers resulting from the large accumulation of energy in the lower polariton, and the many modes available for energy redistribution during the reaction. Our results offer tantalizing opportunities to use condensates for driving chemical reactions, kinetically bypassing usual constraints of fast intramolecular vibrational redistribution in condensed phase.

Published in Nature Communications

References in corpus (5)

• Coherent coupling of molecular resonators with a micro-cavity mode
• Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode
• Electron transfer in confined electromagnetic fields
• Raman scattering with strongly coupled vibron-polaritons
• Exploiting vibrational strong coupling to make an optical parametric oscillator out of a Raman laser

Cited by in corpus (10)

• Generalization of the Tavis-Cummings model for multi-level anharmonic systems: insights on the second excitation manifold
• When do molecular polaritons behave like optical filters?
• Understanding the Energy Gap Law under Vibrational Strong Coupling
• Amplifying Frequency Up-Converted Infrared Signals with a Molecular Optomechanical Cavity
• Multidimensional quantum calculation of the infrared spectra under polaritonic vibrational strong and ultrastrong coupling
• Large Cumulant Eigenvalue as a Signature of Exciton Condensation
• Sympathetic Mechanism for Vibrational Condensation Enabled by Polariton Optomechanical Interaction
• Practical guide to the statistical mechanics of molecular polaritons
• Cavity-Mediated Collective Resonant Suppression of Local Molecular Vibrations
• Beyond mean-field dynamics of the Dicke model with non-Markovian dephasing