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 journalArticleResearchpeer-review

Abstract

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.
LanguageEnglish
Article number011016
Pages1-17
Number of pages17
JournalPhysical Review X
Volume8
Issue number1
DOIs
Publication statusPublished - 2018

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mechanical oscillators
chemical bonds
exploitation
quantum theory
occupation
molecules
unity
pumping
oscillators
chemistry
Raman spectra
gold
thresholds
decay
excitation
lasers
atoms

Cite this

Lombardi, Anna ; Schmidt, Mikołaj K. ; Weller, Lee ; Deacon, William M. ; Benz, Felix ; de Nijs, Bart ; Aizpurua, Javier ; Baumberg, Jeremy J. / Pulsed molecular optomechanics in plasmonic nanocavities : from nonlinear vibrational instabilities to bond-breaking. In: Physical Review X. 2018 ; Vol. 8, No. 1. pp. 1-17.
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Lombardi, A, Schmidt, MK, Weller, L, Deacon, WM, Benz, F, de Nijs, B, Aizpurua, J & Baumberg, JJ 2018, 'Pulsed molecular optomechanics in plasmonic nanocavities: from nonlinear vibrational instabilities to bond-breaking', Physical Review X, vol. 8, no. 1, 011016, pp. 1-17. https://doi.org/10.1103/PhysRevX.8.011016

Pulsed molecular optomechanics in plasmonic nanocavities : from nonlinear vibrational instabilities to bond-breaking. / Lombardi, Anna; Schmidt, Mikołaj K.; Weller, Lee; Deacon, William M.; Benz, Felix; de Nijs, Bart; Aizpurua, Javier; Baumberg, Jeremy J.

In: Physical Review X, Vol. 8, No. 1, 011016, 2018, p. 1-17.

Research output: Contribution to journalArticleResearchpeer-review

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AU - Aizpurua, Javier

AU - Baumberg, Jeremy J.

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