In-plane Anisotropic Third-Harmonic Generation from Germanium Arsenide Thin Flakes

A newly introduced two-dimensional (2D) layered germanium arsenide (GeAs) has attracted growing interest due to its promising highly in-plane anisotropic crystal structure and electronic properties for photonic and optoelectronic applications. The potential of 2D layered GeAs for many applications such as anisotropic photodetection, electronics, superconductivity and thermoelectricity is being investigated in recent studies. However, the intrinsic nonlinear optical properties of 2D layered GeAs have not been explored yet. Here, thickness- and incident polarization-dependent in-plane anisotropic third-harmonic generation (THG) from the mechanically exfoliated thin GeAs flakes is reported. Furthermore, the effect of the flake thickness on the THG conversion efficiency is shown to find the optimal thickness range for high conversion efficiency. The polarization state of the emitted THG signal is also analyzed by measuring the Stokes parameters with different polarization states of the pump beam to demonstrate the capability of controlling the intensity and polarization of TH emission. Our results will create new opportunities for advancing anisotropic optical devices used for future photonic integration, optical communication and optical information processing.