LAUSR

Optical media endowed with large nonlinear susceptibilities are highly prized for their employment in frequency conversion and the generation of nonclassical states of light. Although the presence of an optical resonance can greatly increase the nonlinear response (e.g., in epsilon-near-zero materials), the non-negligible increase in linear absorption often precludes the application of such materials in nonlinear optics. Absorbing materials prepared as thin films, however, can support a low-loss surface wave: the long-range surface exciton polariton (LRSEP). Its propagation lifetime increases with greater intrinsic absorption and reduced film thickness, provided that the film is embedded in a transparent medium (symmetric cladding). We explore LRSEP propagation in a molybdenum film by way of a prism-coupling configuration. Our observations show that excitation of the LRSEP mode leads to a dramatic increase in the yield of second-harmonic generation. This implies that the LRSEP mode is an effective vehicle for utilizing the nonlinear response of absorbing materials.