Tuning the ambipolar behavior in charge carrier transport via defect-engineering is crucial for achieving high mobility transistors for nonlinear logic circuits. Here, we present the electric-field tunable electron and hole transport in a microchannel device consisting of highly air-stable van der Waals (vdW) noble metal dichalcogenide (NMDC), PdSe 2 , as an active layer. Pristine bulk PdSe 2 constitutes Se surface vacancy defects created during the growth or exfoliation process and offers an ambipolar transfer characteristics with a slight electron dominance recorded in field-effect transistor (FET) characteristics showing an ON/OFF ratio < 10 and electron mobility ∼ 21 cm 2 /V.s.However, transfer characteristics of PdSe 2 can be tuned to a hole-dominated transport while using hydrochloric acid (HCl) as a p-type dopant. On the other hand, the chelating agent EDTA, being a strong electron donor, enhances the electron-dominance in PdSe 2 channel. In addition, p-type behavior with a 100 times higher ON/OFF ratio is obtained while cooling the sample down to 10 K. Low-temperature angle-resolved photoemission spectroscopy resembles the p-type band structure of PdSe 2 single crystal. Also, first principle density functional theory calculations justify the tunability observed in PdSe 2 as a result of defect-engineering. Such a defect-sensitive ambipolar vdW architecture may open up new possibilities towards future CMOS (Complementary Metal-Oxide-Semiconductor) device fabrications and high performance integrated circuits.
I. INTRODUCTIONPerformance of a FET based on downscaled two-dimensional (2D) vdW semiconductors like transition metal dichalcogenides (TMDCs) (e.g. MoS 2 , WS 2 , MoSe 2 etc.) as channel depends on the layer's chemical and environmental stability [1][2][3]. In TMDCs, aging effects like gradual oxidation at the TM edges of a micromechanically exfoliated flake transferred from the bulk crystal or at the grain boundaries of a large area sheet hinders its enduring applications in nanoelectronics and optoelectronics. As it happens, easy dissociation of molecular oxygen at the TM edge (e.g. Mo edge in MoS 2 ) with low barrier energy (close to 0.3 eV) compared to its protection at the surface (1.5 eV on the MoS 2 surface) makes the layer more susceptible to wrinkle formation, morphological variation with time. Nonetheless, for the