Mid-infrared-perturbed molecular vibrational signatures in plasmonic nanocavities

作     者：Rohit Chikkaraddy Angelos Xomalis Lukas A.Jakob Jeremy J.Baumberg Rohit Chikkaraddy;Angelos Xomalis;Lukas A.Jakob;Jeremy J.Baumberg

作者机构：NanoPhotonics CentreCavendish LaboratoryDepartment of PhysicsJJ Thompson AvenueUniversity of CambridgeCambridge CB30HEUK EmpaSwiss Federal Laboratories for Materials Science and TechnologyLaboratory for Mechanics of Materials and NanostructuresThunSwitzerland 

出 版 物：《Light(Science & Applications)》 (光（科学与应用)（英文版）)

年 卷 期：2022年第11卷第1期

页      面：127-135页

核心收录：

学科分类：07[理学] 070204[理学-等离子体物理] 0702[理学-物理学] 

基　　金：The authors acknowledge support from European Research Council(ERC)under Horizon 2020 research and innovation programme PICOFORCE(Grant Agreement No.861950) THOR(Grant Agreement No.829067) POSEIDON(Grant Agreement No.861950) the EPSRC(Cambridge NanoDTC EP/L015978/1,EP/L027151/1,EP/S022953/1,EP/P029426/1,and EP/R020965/1) R.C.acknowledges support from Trinity College,University of Cambridge 

主　　题：visible signature utilize 

摘      要：Recent developments in surface-enhanced Raman scattering(SERS)enable observation of single-bond vibrations in real time at room *** contrast,mid-infrared(MIR)vibrational spectroscopy is limited to inefficient slow *** we develop a new method for MIR sensing using *** method utilizes nanoparticle-on-foil(NPoF)nanocavities supporting both visible and MIR plasmonic hotspots in the same nanogap formed by a monolayer of *** SERS signals from individual NPoF nanocavities are modulated in the presence of MIR *** strength of this modulation depends on the MIR wavelength,and is maximized at the 6–12μm absorption bands of SiO_(2) or polystyrene placed under the *** a single-photon lock-in detection scheme we time-resolve the rise and decay of the signal in a few 100 *** observations reveal that the phonon resonances of SiO_(2) can trap intense MIR surface plasmons within the Reststrahlen band,tuning the visible-wavelength localized plasmons by reversibly perturbing the localized few-nm-thick water shell trapped in the nanostructure *** suggests new ways to couple nanoscale bond vibrations for optomechanics,with potential to push detection limits down to single-photon and single-molecule regimes.