PdSe2 single crystals synthesized by the self-flux method

•High quality PdSe2 crystal grown by the self-flux method.•The orthorhombic crystal structure quality and composition stoichiometry confirmed.•Intrinsic p-type carrier densities of ≈3.6 × 1017 cm−3 at room temperature measured.•2D layered structure with anisotropic properties confirmed. Palladium diselenide (PdSe2) is an important transition metal dichalcogenide with a layers-dependent bandgap and many potential applications in electronic and optoelectronic devices. However, the availability of high-quality large-area crystals with phase control is still challenging. Herein, we report the successful growth of large-area PdSe2 single crystals using the self-flux method. The crystal structure, quality, and elemental composition were characterized by X-ray Diffraction, Energy-Dispersive X-ray Spectroscopy, and High-Resolution Transmission Electron Microscopy (HR TEM). The Raman-active vibrational modes of PdSe2 were identified using polarized Raman spectroscopy. The controlled synthesis of PdSe2 enables the potential for a broad range of heterostructures and further integrated optical and electro-optical applications.