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We investigate electronic and optoelectronic properties of few-layer palladium diselenide (PdSe 2 ) phototransistors through spatially-resolved photocurrent measurements. A strong photocurrent resonance peak is observed at 1060 nm (1.17 eV), likely attributed to indirect optical transitions in few-layer PdSe 2 . More interestingly, when the thickness of PdSe 2 flakes increases, more and more photocurrent resonance peaks appear in the near-infrared region, suggesting strong interlayer interactions in few-layer PdSe 2 help open up more optical transitions between the conduction and valence bands of PdSe 2 . Moreover, gate-dependent measurements indicate that remarkable photocurrent responses at the junctions between PdSe 2 and metal electrodes primarily result from the photovoltaic effect when a PdSe 2 phototransistor is in the off-state and are partially attributed to the photothermoelectric effect when the device turns on. We also demonstrate PdSe 2 devices with a Seebeck coefficient as high as 74 μV K −1 at room temperature, which is comparable with recent theoretical predications. Additionally, we find that the rise and decay time constants of PdSe 2 phototransistors are ∼156 μs and ∼163 μs, respectively, which are more than three orders of magnitude faster than previous PdSe 2 work and two orders of magnitude over other noble metal dichalcogenide phototransistors, offering new avenues for engineering future optoelectronics. 

Gate‐/wavelength‐dependent scanning photocurrent measurements of black phosphorous (BP)–MoS₂heterojunctions have shown that the Schottky barrier at the MoS₂–metal interface plays an important role in the photoresponse dynamics of the heterojunction. When the Fermi level is close to the conduction band of MoS₂, photoexcited carriers can tunnel through the narrow depletion region at the MoS₂–metal interface, leading to a short response time of 13 µs regardless of the incident laser wavelength. This response speed is comparable or better than that of other few‐layer BP–MoS₂heterojunctions. Conversely, when the MoS₂channel is in the off‐state, the resulting sizeable Schottky barrier and depletion width make it difficult for photoexcited carriers to overcome the barrier. This significantly delays the carrier transit time and thus the photoresponse speed, leading to a wavelength‐dependent response time since the photoexcited carriers induced by short wavelength photons have a higher probability to overcome the Schottky barrier at the MoS₂–metal interface than long wavelength photons. These studies not only shed light on the fundamental understanding of photoresponse dynamics in BP–MoS₂heterojunctions, but also open new avenues for engineering the interfaces between 2D materials and metal contacts to reduce the response time of 2D optoelectronics.