High-performance 2D WS₂ photodetector enhanced by charge-transfer doping through NH₃ annealing

Transition metal dichalcogenides (TMDs) are potential candidates towards the next-generation photodetector, owing to their tunable energy bandgap and strong light–matter interaction. However, the low charge-carrier mobility and insufficient quantum efficiency of TMDs-based devices restrain their optoelectronic performances. Therefore, an effective and facile doping method needs to be developed for overcoming their poor optoelectronics properties. Here, we demonstrate a controllable nondegenerate n-doping technique for 2D TMDs materials by annealing under NH₃ flow. The on/off current ratio and field-effect mobility of the device after annealing treatment increases about 2 orders of magnitude and 23 times, respectively. We attribute this remarkable doping effect to the physical adsorption and chemical adsorption of NH₃ as well as the associated formation of isolated sulfur vacancies, which is dynamically activated during the annealing treatment, and further verified by the atomic-scale characterization and density functional theory calculations. The annealing temperature and time present a controllable modulation on the electron doping levels of the WS₂ channel. The fabricated WS₂ photodetector can operate in a broad range of visible light at room temperature. At 532 nm wavelength, the responsivity of 2.97 A/W, external quantum efficiency of 699% and specific detectivity of over 10¹⁰ Jones indicate its great potential in sensitive and power-efficient photodetectors. Our results provide an effective method to realize controllable n-doping of 2D materials, aiming for fabricating high-performance 2D photodetectors.