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Tip enhanced IR spectra and imaging have been widely used in cutting-edgestudies for the in-depth understanding of the composition, structure andfunction of interfaces at the nanoscale. However, molecular monolayersensitivity has only been demonstrated on solid/gas interfaces. In aqueousenvironment, the reduced sensitivity due to strong damping of the cantileveroscillation and background IR absorption extremely limits the practicalapplications of tip enhanced IR nanospectroscopy. Here, we demonstratehypersensitive nanoscale IR spectra and imaging in aqueous environment with thecombination of photoinduced force (PiF) microscopy and resonant antennas. Thehighly confined electromagnetic field inbetween the tip end and antennaextremely amplifies the photoinduced force to the detectable level, while theexcitation via plasmon internal reflection mode minimizes the environmentalabsorption. A polydimethylsiloxane (PDMS) layer (~1-2 nm thickness)functionalized on the AFM tip has been successfully identified in water withantennas of different sizes. Sampling volume of ~604 chemical bonds from PDMSwas demonstrated with sub-10 nm spatial resolution confirmed by electric (E)field distribution mapping on antennas, which strongly suggests the desiredrequirements for interfacial spectroscopy. This platform demonstrates for thefirst time the application of photoinduced force microscopy in aqueousenvironments, providing a brand-new configuration to achieve highly enhancednanoscale IR signals, which is extremely promising for future research ofinterfaces and nanosystems in aqueous environments.

Antenna enhanced infrared photoinduced force imaging in aqueous environment with super-resolution and hypersensitivity