To develop next-generation electronic devices, novel semiconductive materials are urgently required. The transition metal dichalcogenides (TMDs) hold the promise of next generation of semiconductor materials for emerging electronic applications. As a member of the group-10 TMDs, PdS2 has a notable layer-number-dependent band structure and tremendously high carrier mobility at room temperature. Here, we demonstrate the experimental realization of centimeter-scale synthesis of the few-layer PdS2 by the combination of physical vapor deposition (PVD) and chemical vapor deposition (CVD) methods. For the first time, the optical anisotropic properties of the few-layer PdS2 were investigated through angle-resolved polarized Raman spectroscopy. Also, the evolution of Raman spectra was studied depending on the temperature in the range of 12–300 K. To further understand the electronic properties of the few-layer PdS2, the field-effect transistor (FET) devices were fabricated and investigated. The electronic measurements of such FET devices reveal that the PdS2 materials exhibit a tunable ambipolar transport mechanism with field-effect mobility of up to ∼388 cm2 V–1 s–1 and the on/off ratio of ∼800, which were not reported before in the literature. To well understand the experimental results, the electronic structure of PdS2 was determined using density functional theory (DFT) calculations. These excellent physical properties are very helpful in developing high-performance opto-electronic applications.
2D materials with mixed crystal phase will lead to the nonuniformity of performance and go against the practical application. Therefore, it is of great significance to develop a valid method to synthesize 2D materials with typical stoichiometry. Here, 2D palladium sulfides with centimeter scale and uniform stoichiometric ratio are synthesized via controlling the sulfurization temperature of palladium thin films. The relationship between sulfurization temperature and products is investigated in depth. Besides, the high-quality 2D PdS 2 films are synthesized via sulfurization at the temperature of 450–550 °C, which would be compatible with back-end-of-line processes in semiconductor industry with considering of process temperature. The PdS 2 films show an n-type semiconducting behavior with high mobility of 10.4 cm 2 V −1 s −1 . The PdS 2 photodetector presents a broadband photoresponse from 450 to 1550 nm. These findings provide a reliable way to synthesizing high-quality and large-area 2D materials with uniform crystal phase. The result suggests that 2D PdS 2 has significant potential in future nanoelectronics and optoelectronic applications.