Second Harmonic Generation from Phononic Epsilon-Near-Zero Berreman Modes in Ultrathin Polar Crystal Films

Abstract: Immense optical field enhancement was predicted to occur for the Berreman mode in ultrathin films at frequencies in the vicinity of epsilon near zero (ENZ). Here, we report the first experimental proof of this prediction in the mid-infrared by probing the resonantly enhanced second harmonic generation (SHG) at the longitudinal optic phonon frequency from a deeply subwavelength-thin aluminum nitride (AlN) film. Employing a transfer matrix formalism, we show that the field enhancement is completely localized inside the AlN layer, revealing that the observed SHG signal of the Berreman mode is solely generated in the AlN film. Our results demonstrate that ENZ Berreman modes in intrinsically low-loss polar dielectric crystals constitute a promising platform for nonlinear nanophotonic applications.