Ultrastrong Optical Harmonic Generations in Layered Platinum Disulfide in the Mid-Infrared

Nonlinear optical activities (e.g., harmonic generations) in two-dimensional (2D) layered materials have attracted much attention due to the great promise in diverse optoelectronic applications such as nonlinear optical modulators, nonreciprocal optical device, and nonlinear optical imaging. Exploration of nonlinear optical response (e.g., frequency conversion) in the infrared, especially the mid-infrared (MIR) region, is highly desirable for ultrafast MIR laser applications ranging from tunable MIR coherent sources, MIR supercontinuum generation, and MIR frequency-comb-based spectroscopy to high harmonic generation. However, nonlinear optical effects in 2D layered materials under MIR pump are rarely reported, mainly due to the lack of suitable 2D layered materials. Van der Waals layered platinum disulfide (PtS₂) with a sizable bandgap from the visible to the infrared region is a promising candidate for realizing MIR nonlinear optical devices. In this work, we investigate the nonlinear optical properties including third-and fifth-harmonic generation (THG and FHG) in thin layered PtS₂ under infrared pump (1550-2510 nm). Strikingly, the ultrastrong third-order nonlinear susceptibility χ⁽³⁾(-3ω;ω,ω,ω) of thin layered PtS₂ in the MIR region was estimated to be over 10^-18 m²/V², which is about one order of that in traditional transition metal chalcogenides. Such excellent performance makes air-stable PtS₂ a potential candidate for developing next-generation MIR nonlinear photonic devices.