Enhanced Second Harmonic Generation from Ferroelectric HfO2-Based Hybrid Metasurfaces

ACS Nano. 2019 Feb 26;13(2):1213-1222. doi: 10.1021/acsnano.8b06308. Epub 2019 Jan 23.

Abstract

Integrated nonlinear metasurfaces leading to high-efficiency optical second harmonic generation (SHG) are highly desirable for optical sensing, imaging, and quantum photonic systems. Compared to traditional metal-only metasurfaces, their hybrid counterparts, where a noncentrosymmetric nonlinear photonic material is incorporated in the near-field of a metasurface, can significantly boost SHG efficiency. However, it is difficult to integrate such devices on-chip due to material incompatibilities, thickness scaling challenges, and the narrow band gaps of nonlinear optical materials. Here, we demonstrate significantly enhanced SHG in on-chip integrated metasurfaces by using nanometer thin films of ferroelectric Y:HfO2. This material has the merit of CMOS compatibility, ultraviolet transparency up to 250 nm, and significant scalability down to sub-10 nm when deposited on silicon. We observe a 20-fold magnitude enhancement of the SHG intensity from the hybrid metasurface compared to a bare ferroelectric HfO2 thin film. Moreover, a 3-fold SHG enhancement is observed from the hybrid metasurface compared to a control structure using nonferroelectric HfO2, demonstrating a major contribution to the SHG signal from ferroelectric Y:HfO2. The effective second-order nonlinear optical coefficient χ(2) of Y:HfO2 is determined to be 6.0 ± 0.5 pm/V, which is comparable to other complex nonlinear photonic oxide materials. Our work provides a general pathway to build an efficient on-chip nanophotonic nonlinear light source for SHG using ferroelectric HfO2 thin films.

Keywords: ferroelectric Y:HfO2; metasurface; nonlinear photonics; plasmonics; second harmonic generation.