K4GeP4Se12: a case for phase-change nonlinear optical chalcogenide.

We report on broadband nonlinear optical (NLO) responses from a phase-change chalcogenide compound K(4)GeP(4)Se(12). Its glassy phase exhibits unusual second-harmonic generation (SHG) due to the preservation of local crystallographic order. The SHG efficiency of the glassy form can be boosted by more than 2 orders of magnitude by simple heat treatment. Strong SHG and third-harmonic generation from both glassy and crystalline compounds were characterized over a wide wavelength range of 1.2-4.0 μm. Our results imply that K(4)GeP(4)Se(12) can be utilized for various NLO applications in the mid-infrared spectrum.