Broadband-infrared assessment of phonon resonance in scattering-type near-field microscopy

Optical near fields exist close to any illuminated object. They account for interesting effects such as enhanced pinhole transmission or enhanced Raman scattering enabling single-molecule spectroscopy. Also, they enable high-resolution (below 10 nm) optical microscopy. The plasmon-enhanced near-field coupling between metallic nanostructures opens new ways of designing optical properties and of controlling light on the nanometre scale. Here we study the strong enhancement of optical near-field coupling in the infrared by lattice vibrations (phonons) of polar dielectrics. We combine infrared spectroscopy with a near-field microscope that provides a confined field to probe the local interaction with a SiC sample. The phonon resonance occurs at 920 cm(-1). Within 20 cm(-1) of the resonance, the near-field signal increases 200-fold; on resonance, the signal exceeds by 20 times the value obtained with a gold sample. We find that phonon-enhanced near-field coupling is extremely sensitive to chemical and structural composition of polar samples, permitting nanometre-scale analysis of semiconductors and minerals. The excellent physical and chemical stability of SiC in particular may allow the design of nanometre-scale optical circuits for high-temperature and high-power operation.

Interferometric near-field optical microscopy achieving a resolution of 10 angstroms is demonstrated. The scattered electric field variation caused by a vibrating probe tip in close proximity to a sample surface is measured by encoding it as a modulation in the optical phase of one arm of an interferometer. Unlike in regular near-field optical microscopes, where the contrast results from a weak source (or aperture) dipole interacting with the polarizability of the sample, the present form of imaging relies on a fundamentally different contrast mechanism: sensing the dipole-dipole coupling of two externally driven dipoles (the tip and sample dipoles) as their spacing is modulated.