Philippe Roelli, Huatian Hu, Ewold Verhagen, Stephanie Reich, Christophe Galland
{"title":"Nanocavities for Molecular Optomechanics: Their Fundamental Description and Applications","authors":"Philippe Roelli, Huatian Hu, Ewold Verhagen, Stephanie Reich, Christophe Galland","doi":"10.1021/acsphotonics.4c01548","DOIUrl":null,"url":null,"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 (<i>Q</i>) and mode volumes (<i>V</i>) essentially describe the performance of a nanocavity in enhancing light-matter interaction, we point to the light-cavity coupling efficiencies (η) and optomechanical cooperativities (<i></i><span style=\"color: inherit;\"><span><span>C</span></span></span><span style=\"\" tabindex=\"0\"><nobr><span overflow=\"scroll\"><span style=\"display: inline-block; position: relative; width: 0em; height: 0px; font-size: 110%;\"><span style=\"position: absolute;\"><span><span style=\"font-family: STIXMathJax_Script-italic;\">𝒞</span></span></span></span></span></nobr></span><script type=\"math/mml\"><math display=\"inline\" overflow=\"scroll\"><mi mathvariant=\"script\">C</mi></math></script>) 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.","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Photonics","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1021/acsphotonics.4c01548","RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
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 (C𝒞) 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.
期刊介绍:
Published as soon as accepted and summarized in monthly issues, ACS Photonics will publish Research Articles, Letters, Perspectives, and Reviews, to encompass the full scope of published research in this field.