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Multimodal Tip-Enhanced Nonlinear Optical Nanoimaging of Plasmonic Silver Nanocubes

Journal Article · · Journal of Physical Chemistry Letters
Optical field localization at plasmonic tip-sample nanojunctions has enabled high spatial resolution chemical analysis through tip-enhanced linear optical spectroscopies, including Raman scattering and photoluminescence. In this work, we illustrate that nonlinear optical processes, including parametric four-wave mixing (4WM), second harmonic/sum-frequency generation (SHG and SFG), and two-photon photoluminescence (TPPL), can be enhanced at plasmonic junctions and spatio-spectrally resolved simultaneously with few-nm spatial resolution under ambient conditions. More importantly, through a detailed analysis of our spectral nano-images, we find that the efficiencies of the local nonlinear signals are determined by sharp tip-sample junction resonances that vary over the few-nanometer length scale because of the corrugated nature of the probe. Namely, plasmon resonances centered at or around the different nonlinear signals are tracked through TPPL, and they are found to selectively enhance nonlinear signals with closely matched optical resonances.
Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1922065
Report Number(s):
PNNL-SA-166319
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 44 Vol. 12; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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