Pulsed molecular optomechanics in plasmonic nanocavities

from nonlinear vibrational instabilities to bond-breaking

Anna Lombardi, Mikołaj K. Schmidt, Lee Weller, William M. Deacon, Felix Benz, Bart de Nijs, Javier Aizpurua, Jeremy J. Baumberg

Research output: Contribution to journalArticle

28 Citations (Scopus)
17 Downloads (Pure)


Small numbers of surface-bound molecules are shown to behave as would be expected for optomechanical oscillators placed inside plasmonic nanocavities that support extreme confinement of optical fields. Pulsed Raman scattering reveals superlinear Stokes emission above a threshold, arising from the stimulated vibrational pumping of molecular bonds under pulsed excitation shorter than the phonon decay time, and agreeing with pulsed optomechanical quantum theory. Reaching the parametric instability (equivalent to a phonon laser or "phaser" regime) is, however, hindered by the motion of gold atoms and molecular reconfiguration at phonon occupations approaching unity. We show how this irreversible bond breaking can ultimately limit the exploitation of molecules as quantum-mechanical oscillators, but accesses optically driven chemistry.
Original languageEnglish
Article number011016
Pages (from-to)1-17
Number of pages17
JournalPhysical Review X
Issue number1
Publication statusPublished - 2018

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