Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering
[EN] CONSPECTUS: Molecular vibrations constitute one of the smallest mechanical oscillators available for micro-/nanoengineering. The energy and strength of molecular oscillations depend delicately on the attached specific functional groups as well as on the chemical and physical environments. By ex...
| Autores: | , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2022 |
| País: | España |
| Institución: | Universidad del País Vasco |
| Repositorio: | Addi. Archivo Digital para la Docencia y la Investigación |
| OAI Identifier: | oai:addi.ehu.eus:10810/57455 |
| Acceso en línea: | http://hdl.handle.net/10810/57455 |
| Access Level: | acceso abierto |
| Palabra clave: | single molecule energy transfer light |
| id |
ES_c6852a9deff243f49d64b85eb8c1d8fa |
|---|---|
| oai_identifier_str |
oai:addi.ehu.eus:10810/57455 |
| network_acronym_str |
ES |
| network_name_str |
España |
| repository_id_str |
|
| dc.title.none.fl_str_mv |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering |
| title |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering |
| spellingShingle |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering Esteban Llorente, Rubén single molecule energy transfer light |
| title_short |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering |
| title_full |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering |
| title_fullStr |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering |
| title_full_unstemmed |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering |
| title_sort |
Molecular Optomechanics Approach to Surface-Enhanced Raman Scattering |
| dc.creator.none.fl_str_mv |
Esteban Llorente, Rubén Baumberg, Jeremy J. Aizpurua Iriazabal, Francisco Javier |
| author |
Esteban Llorente, Rubén |
| author_facet |
Esteban Llorente, Rubén Baumberg, Jeremy J. Aizpurua Iriazabal, Francisco Javier |
| author_role |
author |
| author2 |
Baumberg, Jeremy J. Aizpurua Iriazabal, Francisco Javier |
| author2_role |
author author |
| dc.contributor.none.fl_str_mv |
European Commission |
| dc.subject.none.fl_str_mv |
single molecule energy transfer light |
| topic |
single molecule energy transfer light |
| description |
[EN] CONSPECTUS: Molecular vibrations constitute one of the smallest mechanical oscillators available for micro-/nanoengineering. The energy and strength of molecular oscillations depend delicately on the attached specific functional groups as well as on the chemical and physical environments. By exploiting the inelastic interaction of molecules with optical photons, Raman scattering can access the information contained in molecular vibrations. However, the low efficiency of the Raman process typically allows only for characterizing large numbers of molecules. To circumvent this limitation, plasmonic resonances supported by metallic nanostructures and nanocavities can be used because they localize and enhance light at optical frequencies, enabling surface-enhanced Raman scattering (SERS), where the Raman signal is increased by many orders of magnitude. This enhancement enables few- or even single-molecule characterization. The coupling between a single molecular vibration and a plasmonic mode constitutes an example of an optomechanical interaction, analogous to that existing between cavity photons and mechanical vibrations. Optomechanical systems have been intensely studied because of their fundamental interest as well as their application in practical implementations of quantum technology and sensing. In this context, SERS brings cavity optomechanics down to the molecular scale and gives access to larger vibrational frequencies associated with molecular motion, offering new possibilities for novel optomechanical nanodevices. The molecular optomechanics description of SERS is recent, and its implications have only started to be explored. In this Account, we describe the current understanding and progress of this new description of SERS, focusing on our own contributions to the field. We first show that the quantum description of molecular optomechanics is fully consistent with standard classical and semiclassical models often used to describe SERS. Furthermore, we note that the molecular optomechanics framework naturally accounts for a rich variety of nonlinear effects in the SERS signal with increasing laser intensity. Furthermore, the molecular optomechanics framework provides a tool particularly suited to addressing novel effects of fundamental and practical interest in SERS, such as the emergence of collective phenomena involving many molecules or the modification of the effective losses and energy of the molecular vibrations due to the plasmon-vibration interaction. As compared to standard optomechanics, the plasmonic resonance often differs from a single Lorentzian mode and thus requires a more detailed description of its optical response. This quantum description of SERS also allows us to address the statistics of the Raman photons emitted, enabling the interpretation of two-color correlations of the emerging photons, with potential use in the generation of nonclassical states of light. Current SERS experimental implementations in organic molecules and two-dimensional layers suggest the interest in further exploring intense pulsed illumination, situations of strong coupling, resonant-SERS, and atomic-scale field confinement. |
| publishDate |
2022 |
| dc.date.none.fl_str_mv |
2022 2022 2022 |
| dc.type.none.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
http://hdl.handle.net/10810/57455 |
| url |
http://hdl.handle.net/10810/57455 |
| dc.language.none.fl_str_mv |
Inglés |
| language_invalid_str_mv |
Inglés |
| dc.relation.none.fl_str_mv |
info:eu-repo/grantAgreement/EC/H2020/829067 info:eu-repo/grantAgreement/EC/H2020/883703 info:eu-repo/grantAgreement/MICINN/PID2019-107432GB-I00/ https://pubs.acs.org/doi/10.1021/acs.accounts.1c00759 |
| dc.rights.none.fl_str_mv |
info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/3.0/es/ Atribución 3.0 España |
| eu_rights_str_mv |
openAccess |
| rights_invalid_str_mv |
http://creativecommons.org/licenses/by/3.0/es/ Atribución 3.0 España |
| dc.format.none.fl_str_mv |
application/pdf |
| dc.publisher.none.fl_str_mv |
American Chemical Society |
| publisher.none.fl_str_mv |
American Chemical Society |
| dc.source.none.fl_str_mv |
reponame:Addi. Archivo Digital para la Docencia y la Investigación instname:Universidad del País Vasco |
| instname_str |
Universidad del País Vasco |
| reponame_str |
Addi. Archivo Digital para la Docencia y la Investigación |
| collection |
Addi. Archivo Digital para la Docencia y la Investigación |
| repository.name.fl_str_mv |
|
| repository.mail.fl_str_mv |
|
| _version_ |
1869419080057880576 |
| spelling |
Molecular Optomechanics Approach to Surface-Enhanced Raman ScatteringEsteban Llorente, RubénBaumberg, Jeremy J.Aizpurua Iriazabal, Francisco Javiersingle moleculeenergy transferlight[EN] CONSPECTUS: Molecular vibrations constitute one of the smallest mechanical oscillators available for micro-/nanoengineering. The energy and strength of molecular oscillations depend delicately on the attached specific functional groups as well as on the chemical and physical environments. By exploiting the inelastic interaction of molecules with optical photons, Raman scattering can access the information contained in molecular vibrations. However, the low efficiency of the Raman process typically allows only for characterizing large numbers of molecules. To circumvent this limitation, plasmonic resonances supported by metallic nanostructures and nanocavities can be used because they localize and enhance light at optical frequencies, enabling surface-enhanced Raman scattering (SERS), where the Raman signal is increased by many orders of magnitude. This enhancement enables few- or even single-molecule characterization. The coupling between a single molecular vibration and a plasmonic mode constitutes an example of an optomechanical interaction, analogous to that existing between cavity photons and mechanical vibrations. Optomechanical systems have been intensely studied because of their fundamental interest as well as their application in practical implementations of quantum technology and sensing. In this context, SERS brings cavity optomechanics down to the molecular scale and gives access to larger vibrational frequencies associated with molecular motion, offering new possibilities for novel optomechanical nanodevices. The molecular optomechanics description of SERS is recent, and its implications have only started to be explored. In this Account, we describe the current understanding and progress of this new description of SERS, focusing on our own contributions to the field. We first show that the quantum description of molecular optomechanics is fully consistent with standard classical and semiclassical models often used to describe SERS. Furthermore, we note that the molecular optomechanics framework naturally accounts for a rich variety of nonlinear effects in the SERS signal with increasing laser intensity. Furthermore, the molecular optomechanics framework provides a tool particularly suited to addressing novel effects of fundamental and practical interest in SERS, such as the emergence of collective phenomena involving many molecules or the modification of the effective losses and energy of the molecular vibrations due to the plasmon-vibration interaction. As compared to standard optomechanics, the plasmonic resonance often differs from a single Lorentzian mode and thus requires a more detailed description of its optical response. This quantum description of SERS also allows us to address the statistics of the Raman photons emitted, enabling the interpretation of two-color correlations of the emerging photons, with potential use in the generation of nonclassical states of light. Current SERS experimental implementations in organic molecules and two-dimensional layers suggest the interest in further exploring intense pulsed illumination, situations of strong coupling, resonant-SERS, and atomic-scale field confinement.We thank Mikołaj K. Schmidt, Tomáš Neuman, Yuan Zhang, and Felix Benz for input and discussions. We also are grateful for financial support from FET-Open project no. 829067 (THOR), ERC grant no. 883703 (PICOFORCE), grant PID2019- 107432GB-I00 funded by MCIN/AEI/10.13039/ 501100011033/, and grant no. IT 1526-22 from the Basque Government for consolidated groups of the Basque University.American Chemical SocietyEuropean Commission202220222022info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/57455reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/EC/H2020/829067info:eu-repo/grantAgreement/EC/H2020/883703info:eu-repo/grantAgreement/MICINN/PID2019-107432GB-I00/https://pubs.acs.org/doi/10.1021/acs.accounts.1c00759info:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by/3.0/es/© 2022 The Authors. Published by American Chemical Society. Attribution 4.0 International (CC BY 4.0)Atribución 3.0 Españaoai:addi.ehu.eus:10810/574552026-06-18T09:23:17Z |
| score |
15,300724 |