Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas
Journal article, 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.
Author
Joel Kuttruff
University of Konstanz
Marco Romanelli
University of Padua
Esteban Pedrueza Villalmanzo
Institution of physics at Gothenburg University
University of Gothenburg
Jonas Allerbeck
Swiss Federal Laboratories for Materials Science and Technology (Empa)
University of Konstanz
Jacopo Fregoni
Universidad Autonoma de Madrid (UAM)
Valeria Saavedra
Chalmers, Chemistry and Chemical Engineering, Chemistry and Biochemistry
Joakim Andreasson
Chalmers, Chemistry and Chemical Engineering, Chemistry and Biochemistry
Daniele Brida
University of Luxembourg
Alexander Dmitriev
University of Gothenburg
Stefano Corni
University of Padua
Consiglo Nazionale Delle Richerche
N. Maccaferri
Umeå University
University of Luxembourg
Nature Communications
2041-1723 (ISSN) 20411723 (eISSN)
Vol. 14 1 3875Subject Categories
Physical Chemistry
Atom and Molecular Physics and Optics
Theoretical Chemistry
DOI
10.1038/s41467-023-39413-5
PubMed
37414750