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Raman spectroscopy is a powerful technique to characterize materials. Itprobes non-destructively chemical composition, crystallinity, defects, strainand coupling phenomena. However, the Raman response of surfaces or thin filmsis often weak and obscured by dominant bulk signals. Here we overcome thislimitation by placing a transferable porous gold membrane (PAuM) on top of thesurface of interest. Slot-like nanopores in the membrane act as plasmonic slotantennas and enhance the Raman response of the surface or thin film underneath.Simultaneously, the PAuM suppresses the penetration of the excitation laserinto the bulk, efficiently blocking the bulk Raman signal. Using graphene as amodel surface, we show that these two simultaneous effects lead to an increasein the surface-to-bulk Raman signal ratio by three orders of magnitude. We findthat 90% of the Raman enhancement occurs within the top 2.5 of the material,demonstrating truly surface-sensitive Raman scattering. To validate ourapproach, we analyze the surface of a LaNiO3 thin film. We observe a Raman modesplitting for the LaNiO3 surface-layer, which is spectroscopic evidence thatthe surface structure differs from the bulk. This result underpins that PAuMgive direct access to Raman signatures of surfaces and their structuralproperties.

Surface-Sensitive Raman Scattering by Transferable Nanoporous Plasmonic Membranes