Coherent phonon and surface-enhanced Raman scattering dynamics in solids

We have demonstrated coherent phonon and surface-enhanced Raman scattering (SERS) dynamics of carbon-related materials: gold (Au) deposited graphite and benzenethiol (BT) self-assembled monolayer (SAM) adsorbed on Au film with roughness. Using ultrafast pump-probe spectroscopy with the enhanced electric field via Au hemispheres or Au film with nanoscale roughness, transient behaviors of high frequency phonons located at surface/interface were sensitively detected. In Au deposited graphite, the electric field near graphite surface around Au nanoparticles, whose typical diameter is ~10 nm, is strongly enhanced. As a result, the disorder-induced mode (D-mode) near the surface was clearly observed. In BT-SAM, the nanoscale roughness of the Au film might contribute to the amplitude enhancement of coherent vibrations up to the detected level. From these results, we believe that coherent SERS spectroscopy will open the door to observe coherent phonon dynamics even at the level of monolayer and single molecules for future.