Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas
Artikel i vetenskaplig tidskrift, 2023
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 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 light modes. 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 pure molecular 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 uncoupled excited molecule relaxation to the ground state.
Författare
Joel Kuttruff
Universität Konstanz
Marco Romanelli
Università di Padova
Esteban Pedrueza Villalmanzo
Institutionen för fysik, GU
Göteborgs universitet
Jonas Allerbeck
Eidgenössische Materialprüfungs- und Forschungsanstalt (Empa)
Universität Konstanz
Jacopo Fregoni
Universidad Autonoma de Madrid (UAM)
Valeria Saavedra
Chalmers, Kemi och kemiteknik, Kemi och biokemi
Joakim Andreasson
Chalmers, Kemi och kemiteknik, Kemi och biokemi
Daniele Brida
Université du Luxembourg
Alexander Dmitriev
Göteborgs universitet
Stefano Corni
Università di Padova
Consiglo Nazionale Delle Richerche
N. Maccaferri
Umeå universitet
Université du Luxembourg
Nature Communications
2041-1723 (ISSN) 20411723 (eISSN)
Vol. 14 1 3875Ämneskategorier
Fysikalisk kemi
Atom- och molekylfysik och optik
Teoretisk kemi
DOI
10.1038/s41467-023-39413-5
PubMed
37414750