Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering
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 la...
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| Language: | English |
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Nature Portfolio
2023-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-38124-1 |
| _version_ | 1827928547741663232 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Lukas A. Jakob |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-13T06:10:18Z |
| format | Article |
| id | doaj.art-455f3290550247ce96b6a42f8c315d50 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T06:10:18Z |
| publishDate | 2023-06-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj.art-455f3290550247ce96b6a42f8c315d502023-06-11T11:18:30ZengNature PortfolioNature Communications2041-17232023-06-0114111110.1038/s41467-023-38124-1Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scatteringLukas A. Jakob0William M. Deacon1Yuan Zhang2Bart de Nijs3Elena Pavlenko4Shu Hu5Cloudy Carnegie6Tomas Neuman7Ruben Esteban8Javier Aizpurua9Jeremy J. Baumberg10Nanophotonics Centre, Cavendish Laboratory, University of CambridgeNanophotonics Centre, Cavendish Laboratory, University of CambridgeHenan Key Laboratory of Diamond Optoelectronic Materials and Devices, Key Laboratory of Material Physics, Ministry of Education, School of Physics and Microelectronics, Zhengzhou UniversityNanophotonics Centre, Cavendish Laboratory, University of CambridgeNanophotonics Centre, Cavendish Laboratory, University of CambridgeNanophotonics Centre, Cavendish Laboratory, University of CambridgeNanophotonics Centre, Cavendish Laboratory, University of CambridgeCenter for Material Physics (CSIC—UPV/EHU and DIPC), Paseo Manuel de Lardizabal 5Center for Material Physics (CSIC—UPV/EHU and DIPC), Paseo Manuel de Lardizabal 5Center for Material Physics (CSIC—UPV/EHU and DIPC), Paseo Manuel de Lardizabal 5Nanophotonics Centre, Cavendish Laboratory, University of CambridgeAbstract 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.https://doi.org/10.1038/s41467-023-38124-1 |
| spellingShingle | 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 Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering Nature Communications |
| title | Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering |
| title_full | Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering |
| title_fullStr | Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering |
| title_full_unstemmed | Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering |
| title_short | Giant optomechanical spring effect in plasmonic nano- and picocavities probed by surface-enhanced Raman scattering |
| title_sort | giant optomechanical spring effect in plasmonic nano and picocavities probed by surface enhanced raman scattering |
| url | https://doi.org/10.1038/s41467-023-38124-1 |
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