Surface sensing systems and methods for imaging a scanned surface (32) of a sample (30) via sum-frequency vibrational spectroscopy are disclosed herein. The systems include a sample holder (20), a visible light source (40) configured to direct a visible light beam (42) incident upon a sampled location (34) of the scanned surface (32) and a tunable IR source (50) configured to direct a tunable IR beam (52) coincident with the visible light beam (42) upon the sampled location (34). The systems also include a scanning structure (60) configured to scan the visible light beam (42) and the tunable IR beam (52) across the scanned surface (32), and a light filter (70) configured to receive an emitted beam (38) from the scanned surface (32) and to filter the emitted beam (38) to generate a filtered light beam (72). The systems further include a light detection system (80) configured to receive the filtered light beam (72), and an alignment structure (90). The methods include methods of operating the systems.
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