16
views
0
recommends
+1 Recommend
0 collections
    0
    shares
      • Record: found
      • Abstract: found
      • Article: found
      Is Open Access

      Nanocavities for Molecular Optomechanics: Their Fundamental Description and Applications

      review-article

      Read this article at

      Bookmark
          There is no author summary for this article yet. Authors can add summaries to their articles on ScienceOpen to make them more accessible to a non-specialist audience.

          Abstract

          Vibrational Raman scattering—a process where light exchanges energy with a molecular vibration through inelastic scattering—is most fundamentally described in a quantum framework where both light and vibration are quantized. When the Raman scatterer is embedded inside a plasmonic nanocavity, as in some sufficiently controlled implementations of surface-enhanced Raman scattering (SERS), the coupled system realizes an optomechanical cavity where coherent and parametrically amplified light–vibration interaction becomes a resource for vibrational state engineering and nanoscale nonlinear optics. The purpose of this Perspective is to clarify the connection between the languages and parameters used in the fields of molecular cavity optomechanics (McOM) versus its conventional, “macroscopic” counterpart and to summarize the main results achieved so far in McOM and the most pressing experimental and theoretical challenges. We aim to make the theoretical framework of molecular cavity optomechanics practically usable for the SERS and nanoplasmonics community at large. While quality factors ( Q) and mode volumes ( V) essentially describe the performance of a nanocavity in enhancing light-matter interaction, we point to the light-cavity coupling efficiencies (η) and optomechanical cooperativities ( ) as the key parameters for molecular optomechanics. As an illustration of the significance of these quantities, we investigate the feasibility of observing optomechanically induced transparency with a molecular vibration—a measurement that would allow for a direct estimate of the optomechanical cooperativity.

          Related collections

          Most cited references160

          • Record: found
          • Abstract: not found
          • Article: not found

          Cavity optomechanics

            Bookmark
            • Record: found
            • Abstract: not found
            • Article: not found

            Raman spectra of pyridine adsorbed at a silver electrode

              Bookmark
              • Record: found
              • Abstract: found
              • Article: not found

              Chemical mapping of a single molecule by plasmon-enhanced Raman scattering.

              Visualizing individual molecules with chemical recognition is a longstanding target in catalysis, molecular nanotechnology and biotechnology. Molecular vibrations provide a valuable 'fingerprint' for such identification. Vibrational spectroscopy based on tip-enhanced Raman scattering allows us to access the spectral signals of molecular species very efficiently via the strong localized plasmonic fields produced at the tip apex. However, the best spatial resolution of the tip-enhanced Raman scattering imaging is still limited to 3-15 nanometres, which is not adequate for resolving a single molecule chemically. Here we demonstrate Raman spectral imaging with spatial resolution below one nanometre, resolving the inner structure and surface configuration of a single molecule. This is achieved by spectrally matching the resonance of the nanocavity plasmon to the molecular vibronic transitions, particularly the downward transition responsible for the emission of Raman photons. This matching is made possible by the extremely precise tuning capability provided by scanning tunnelling microscopy. Experimental evidence suggests that the highly confined and broadband nature of the nanocavity plasmon field in the tunnelling gap is essential for ultrahigh-resolution imaging through the generation of an efficient double-resonance enhancement for both Raman excitation and Raman emission. Our technique not only allows for chemical imaging at the single-molecule level, but also offers a new way to study the optical processes and photochemistry of a single molecule.
                Bookmark

                Author and article information

                Journal
                ACS Photonics
                ACS Photonics
                ph
                apchd5
                ACS Photonics
                American Chemical Society
                2330-4022
                06 November 2024
                20 November 2024
                : 11
                : 11
                : 4486-4501
                Affiliations
                []Nano-optics Group, CIC nanoGUNE BRTA , E-20018 Donostia-San Sebastián, Spain
                []Center for Biomolecular Nanotechnologies, Istituto Italiano di Tecnologia , via Barsanti 14, Arnesano, 73010, Italy
                [§ ]Center for Nanophotonics, NWO Institute AMOLF , Science Park 104, 1098 XG Amsterdam, The Netherlands
                []Department of Physics, Freie Universität Berlin , 14195 Berlin, Germany
                []Institute of Physics, Swiss Federal Institute of Technology Lausanne (EPFL) , CH-1015 Lausanne, Switzerland
                [# ]Center of Quantum Science and Engineering, Swiss Federal Institute of Technology Lausanne (EPFL) , CH-1015 Lausanne, Switzerland
                Author notes
                Author information
                https://orcid.org/0000-0002-1582-2301
                https://orcid.org/0000-0001-8284-9494
                https://orcid.org/0000-0002-0276-8430
                https://orcid.org/0000-0002-2391-0256
                https://orcid.org/0000-0001-5627-0796
                Article
                10.1021/acsphotonics.4c01548
                11583369
                39584033
                6a0e540c-2272-4317-9332-7595b4ad815b
                © 2024 The Authors. Published by American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 15 August 2024
                : 19 September 2024
                : 17 September 2024
                Funding
                Funded by: H2020 European Research Council, doi 10.13039/100010663;
                Award ID: 820196
                Funded by: Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, doi 10.13039/501100001711;
                Award ID: 214993
                Funded by: Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, doi 10.13039/501100001711;
                Award ID: 206926
                Funded by: Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, doi 10.13039/501100001711;
                Award ID: 198898
                Funded by: H2020 Marie Sklodowska-Curie Actions, doi 10.13039/100010665;
                Award ID: 101065661
                Funded by: H2020 Future and Emerging Technologies, doi 10.13039/100010664;
                Award ID: 829067
                Categories
                Perspective
                Custom metadata
                ph4c01548
                ph4c01548

                plasmonic antennas,surface-enhanced raman scattering,cavity optomechanics,molecular vibrations,raman spectroscopy

                Comments

                Comment on this article