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The past decades have witnessed marked progresses on the research ofinterfacial science in complex systems promoted by the advances in novelexperimental techniques. Despite its success in many fields, implementation ofcoherent anti-Stokes Raman spectroscopy (CARS) for tackling the problems atinterfaces was hindered by the huge resonant and non-resonant background fromthe bulk. Here we have developed a novel CARS scheme that is capable of probinga buried interface via suppression of the non-resonant and resonant bulkcontribution by at least $10^5$ times. The method utilizes self-destructiveinterference between the forward and backward CARS generated in the bulk nearthe Brewster angle. As a result, we are able to resolve the vibrationalspectrum of sub-monolayer interfacial species immersed in the surrounding mediawith huge CARS responses. We expect our approach not only opens up theopportunity for interrogation of the interfaces that involve apolar molecules,but also benefits other nonlinear optical spectroscopic techniques in promotingsignal-to-background noise ratio.

Self-suppression of the Giant CARS Background for Detection of Buried Interface with Sub-monolayer Sensitivity