Work

Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering

Year: 2023

Type: article

Abstract: Molecular vibrations couple to visible light only weakly, have small mutual interactions, and hence are often ignored for non-linear optics. Here we show the extreme confinement provided by plasmonic nano- and pico-cavities can sufficiently enhance optomechanical coupling so that intense laser illumination drastically softens the molecular bonds. This optomechanical pumping regime produces strong distortions of the Raman vibrational spectrum related to giant vibrational frequency shifts from an optical spring effect which is hundred-fold larger than in traditional cavities. The theoretical simulations accounting for the multimodal nanocavity response and near-field-induced collective phonon interactions are consistent with the experimentally-observed non-linear behavior exhibited in the Raman spectra of nanoparticle-on-mirror constructs illuminated by ultrafast laser pulses. Further, we show indications that plasmonic picocavities allow us to access the optical spring effect in single molecules with continuous illumination. Driving the collective phonon in the nanocavity paves the way to control reversible bond softening, as well as irreversible chemistry.

Source: Nature Communications

DOI: 10.1038/s41467-023-38124-1

Authors: Lukas A. Jakob, William M. Deacon, Yuan Zhang, Bart de Nijs, Elena Pavlenko, Shu Hu, Cloudy Carnegie, Tomas Neuman, Ruben Esteban, Javier Aizpurua, Jeremy J. Baumberg

Institutions: University of Cambridge, Zhengzhou University, Material Physics Center, Donostia International Physics Center, University of the Basque Country

Language: English

Topic: Mechanical and Optical Resonators

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: gold

Estimated APC paid: $6,290

Funders: Royal Society, European Commission, National Natural Science Foundation of China, Eusko Jaurlaritza, Ministerio de Economía y Competitividad, Cambridge Trust, Engineering and Physical Sciences Research Council, Agencia Estatal de Investigación, H2020 European Research Council

Awards: G105268529, G1175115578, G1305393325, G1338257350, G2045186918, G2102580215, G2262748287, G2281333282, G2713276326, G2993574131, G300979063, G3428307696, G34346518, G3435407688, G3480869486, Pulsed interaction in plasmonic nanocavities, G387506447, G4033406476, G425668148, G4369982300, Pico-Photonic Forces at the Atomic Scale, G4526231891, Roll-to-roll Self-assembly of Advanced Photonic NanoMaterials (R2R-4Photonics), G5080475149, G5280117016, G5507171923, G5560776957, G5662792045, G5675890980, G5943232429, G6051805555, G6200043914, G6687049611, Nano-Optics to controlled Nano-Chemistry Programme Grant (NOtCH), G7084143925, EPSRC Centre for Doctoral Training in Sustainable and Functional Nano, NanoPhOtonic devices applying SElf-assembled colloIDs for novel ON-chip light sources, TeraHertz detection enabled by mOleculaR optomechanics, G8603513261, G8684520763

OpenAlex ID: W4379537374

FWCI: 7.142

Cites: 73

Cited by: 72

Related to: 10