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Optical field localization at plasmonic tip-sample nanojunctions has enabledhigh spatial resolution chemical analysis through tip-enhanced linear opticalspectroscopies, including Raman scattering and photoluminescence. Here, weillustrate that nonlinear optical processes, including parametric four-wavemixing (4WM), second harmonic/sum-frequency generation (SHG and SFG), andtwo-photon photoluminescence (TPPL), can be enhanced at plasmonic junctions andspatio-spectrally resolved simultaneously with few-nm spatial resolution underambient conditions. More importantly, through a detailed analysis of ourspectral nano-images, we find that the efficiencies of the local nonlinearsignals are determined by sharp tip-sample junction resonances that vary overthe few-nanometer length scale because of the corrugated nature of the probe.Namely, plasmon resonances centered at or around the different nonlinearsignals are tracked through TPPL, and they are found to selectively enhancenonlinear signals with closely matched optical resonances.

Multimodal Tip-Enhanced Nonlinear Optical Nano-Imaging of Plasmonic Silver Nanocubes