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.

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.