Super-Resolution Chemical Imaging with Plasmonic Substrates Aeli P. Olson Christopher T. Ertsgaard Sarah N. Elliott Nathan C. Lindquist 10.1021/acsphotonics.5b00647.s002 https://acs.figshare.com/articles/media/Super_Resolution_Chemical_Imaging_with_Plasmonic_Substrates/2579275 We demonstrate super-resolution chemical imaging with plasmonic nanoholes via surface-enhanced Raman spectroscopy (SERS). Due to large field enhancements, blinking behavior of SERS hot spots was observed and processed using a stochastic optical reconstruction microscopy (STORM) algorithm. This enabled localization to within 10 nm and high-resolution imaging. However, illumination of the sample with a static laser beam produced only SERS hot spots in fixed locations, leaving noticeable gaps in the final images. By randomly altering the phase profile of the incident beam with a simple optical diffuser, the hot spots were shifted across the plasmonic surface to illuminate different areas of the sample, thereby rendering a final image without the gaps. A tunable band-pass filter was used to preserve spectral information, allowing chemical contrast imaging. Images were then compared to those obtained with a scanning electron microscope. Finally, we show that super-resolution SERS images can also be obtained with our dynamic illumination technique on even the most basic plasmonic substrate: as-deposited rough silver films. These results show significant potential for the use of simple plasmonic substrates with straightforward illumination and collection schemes for super-resolution chemical imaging. 2016-02-17 00:00:00 plasmonic substrates image plasmonic substrate plasmonic nanoholes SERS sample field enhancements laser beam incident beam Plasmonic Substrates 10 nm gap phase profile scanning electron microscope collection schemes reconstruction microscopy silver films results show illumination technique plasmonic surface chemical contrast imaging