2023/02/08 by Arghadip Koner, Matthew Du, Koner, Arghadip +7
Computer Science · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Mechanical and Optical Resonators #Quantum Information and Cryptography #Strong Light-Matter Interactions
paper · pdf · doi:10.48550/arxiv.2302.03880
openalex publication_date 2023/02/08 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/01
Interaction between light and molecular vibrations leads to hybrid light-matter states called vibrational polaritons. Even though many intriguing phenomena have been predicted for single-molecule vibrational strong coupling (VSC), several studies suggest that these effects tend to be diminished in the many-molecule regime due to the presence of dark states. Achieving single or few-molecule vibrational polaritons has been constrained by the need for fabricating extremely small mode volume infrared cavities. In this work, we propose an alternative strategy to achieve single-molecule VSC in a cavity-enhanced Raman spectroscopy (CERS) setup, based on the physics of cavity optomechanics. We then present a scheme harnessing few-molecule VSC to thermodynamically couple two reactions, such that a spontaneous electron transfer can now fuel a thermodynamically uphill reaction that was non-spontaneous outside the cavity.