Ultrafast collapse of molecular polaritons in photoswitch-nanoantennas at room temperature
arXiv:2205.06358 · doi:10.1038/s41467-023-39413-5
Abstract
Molecular polaritons are hybrid light-matter states that emerge when a molecular transition strongly interacts with photons in a resonator. At optical frequencies, this interaction unlocks a way to explore and control new chemical phenomena at the nanoscale. Achieving such a control at ultrafast timescales, however, is an outstanding challenge, as it requires a deep understanding of the dynamics of the collectively coupled molecular excitation and the nanoconfined electromagnetic fields. Here, we investigate the dynamics of collective polariton states, realized by coupling molecular photoswitches to optically anisotropic plasmonic nanoantennas. Pump-probe experiments reveal an ultrafast collapse of polaritons to a single-molecule transition triggered by femtosecond-pulse excitation at room-temperature. Through a synergistic combination of experiments and quantum mechanical modelling, we show that the response of the system is governed by intramolecular dynamics, occurring one order of magnitude faster with respect to the unperturbed excited molecule relaxation to the ground state.
References in corpus (9)
- Observation of Superfluidity of Polaritons in Semiconductor Microcavities
- Theoretical Challenges in Polaritonic Chemistry
- Ultrafast control of Rabi oscillations in a polariton condensate
- Photoprotecting uracil by coupling with lossy nanocavities
- Strong coupling with light enhances the photoisomerization quantum yield of azobenzene
- Multimode Organic Polariton Lasing
- Ultrafast all-optical switching enabled by epsilon-near-zero modes in metal-insulator nanocavities
- Strong coupling between localized surface plasmons and molecules by coupled cluster theory
- Femtosecond Photophysics of Molecular Polaritons