Graphdiyne (GDY)/two-dimensional materials (2DMs) heterostructures present unique opportunities for advanced optoelectronic and neuromorphic devices because of their exceptional electrical, optical, and structural properties. However, the traditional methods for construction of GDY/2DMs heterostructures usually lead to inferior interfaces, which seriously affects the charge separation and transport. Herein, an in situ approach for growing GDY nanowalls (NWs) on WSe2 is employed in this work. The as-prepared GDY NWs/WSe2 heterostructure exhibits self-powered broadband photodetection across 405–980 nm with a high responsivity of 2176 A/W and detectivity of 3.6 × 1012 Jones at 532 nm under 0.02 mW/cm2 illumination, significantly outperforming previously reported GDY-based devices. The efficient charge separation and strong photocarrier trapping in the GDY NWs/WSe2 heterostructure result in pronounced short-term and long-term synaptic plasticity. The nonlinear, wavelength-dependent reservoir state separation enables clear distinction of multiple pulse sequences, which shows great potential for logic processing. The successfully resolved red, green, and violet patterns, and one-shot color image recognition of a 5-letter image highlight transformative potential of GDY NWs/WSe2 device for future adaptive imaging and neuromorphic computing technologies.

Van der Waals heterojunctions (vdWHs) have garnered significant attention for their promising applications in optoelectronics, attributed to their exceptional physical attributes. In this study, we present a straightforward approach to fabricating high-performance vdWHs photodetectors. Specifically, we prepared WSO_x/WS₂ vdWH photodetectors through the ozone oxidation of a WS₂ thin films at 100 °C. To characterize the morphology and optical properties of both the WS₂ and WSO_x/WS₂ thin films, we utilized atomic force microscopy (AFM) and Raman spectroscopy. Additionally, X-ray photoelectron spectroscopy (XPS) was employed to delve into the structural evolution by scrutinizing the bonding states of W, O, and S in the WS₂ before and after the ozone oxidation process. The resultant WSO_x/WS₂ vdWH photodetectors exhibited impressive photoelectric performance at wavelengths of 475 nm and 532 nm. It demonstrated a high responsivity of 230.7 A/W, a remarkable specific detectivity of 1.794 × 10¹¹ Jones, and a swift response speed of 60 ms at 475 nm. Furthermore, first-principles calculations based on density functional theory (DFT) were conducted to validate the oxidation kinetics of monolayer WS₂, the type II energy band alignment, and the interlayer charge transfer within the WSO_x/WS₂ vdWH. This research contributes novel insights into the synthesis of two-dimensional transition metal oxides (TMOs)-transition metal dichalcogenides (TMDCs) heterostructures for photodetector applications.

The study focuses on the optical and electrical properties of Tungsten Ditelluride (WTe2), a type II Weyl semimetal, as well as the influence of its self-limiting oxide (SLO) layer that forms during natural oxidation. WTe2 exhibits promising applications in photodetection and energy harvesting due to its unique gapless linear dispersion and Berry-field-enhanced nonlinear optical effects. However, surface oxidation poses a challenge as it degrades the performance of WTe2. By employing spectroscopic ellipsometry and Raman spectroscopy, the progression of the oxide layer’s thickness and its impact on the optical constants of WTe2 were examined. The results revealed a rapid increase in oxide thickness within the first 24 h, and it reached saturation at ∼10 nm after 45 h of atmospheric exposure. Electrical properties were explored using Kelvin Probe Force Microscopy, uncovering a modification in surface potential and Fermi level following oxidation. Additionally, a SLO/WTe2 heterojunction device exhibited a wide region of positive and negative coexisting photocurrent, highlighting the potential for logical operations in ambient air. Finally, the mechanism of operation of the device is discussed. The electrical and optical properties of the pristine, partially oxidized and fully oxidized WTe2 are analyzed using density functional theory calculations. It shows that the SLO layer has a significant effect on the optical and electronic properties, which is instructive for future wavelength-modulated device optoelectronic logic operations.

Tungsten disulfide (WS2) has recently attracted considerable attention owing to its excellent physical, chemical, electronic, and optical properties, leading to increased research into its applications in electronic and optoelectronic devices. However, the oxidation of 2D material affects significantly its optical and electronic properties during storage or processing. This study employs density functional theory (DFT) to analyze the effects of natural and thermal oxidation on the optical and electronic properties of WS2 monolayer. First, the climbing-image nudged elastic band (cNEB) method is applied to analyze transitional states and the potential barriers of WS2 oxidation. It reveals that primarily involves the bonding of oxygen atoms with sulfur atoms, whereas thermal oxidation introduces both oxygen substitutions and generates oxygen vacancies. Second, the electron band structures after natural and thermal oxidation are comparably analyzed, which reveals that natural and thermal oxidation both can narrow the bandgap. Lastly, we investigate the optical properties of WS2 monolayer under different oxidation conditions. The results demonstrate that natural oxidation results in weakened light absorption and a blue shift relative to the pristine WS2, whereas thermal oxidation enhances absorption and induces a red shift. These findings underscore the importance of carefully managing oxidation conditions to effectively modulate the optoelectronic properties of WS2.