Quantum Multibody Interactions in Halide-Assisted Vapor-Synthesized Monolayer WSe₂ and Its Integration in a High Responsivity Photodetector with Low-Interface Trap Density

Among the two-dimensional (2D) transitional-metal dichalcogenides, monolayer (1L) tungsten diselenide (WSe2) has recently attracted a great deal of interest because of its direct band gap and tunable charge transport behavior, making it attractive for a variety of electronic and optoelectronic applications. Controlled and efficient synthesis of 1L WSe2 using chemical vapor deposition (CVD) is often challenging because of the high temperatures required to generate a steady flux of tungsten atoms in the vapor phase from the oxide precursors. Here, the use of halide-assisted low-pressure CVD with NaCl helps to reduce the growth temperature to ∼750 °C, which is lower than the typical temperatures needed with conventional CVD for realizing 1L WSe2. Moreover, we experimentally probed the quantum multibody interactions in 1L WSe2 ascribed to excitons, trions, and other localized states by analyzing the temperature-dependent photoluminescence spectra, where such multibody interactions govern the intrinsic electronic and optoelectronic properties of 1L WSe2 for device platforms. The role of the metal–2D semiconductor interface is also critical to realize high-performance devices. In this study, a 1L WSe2-based photodetector was fabricated using Al contacts, which shows a high photoresponsivity, and the interface-state density Dit of the Al/WSe2 junction was computed to be the lowest reported to date ∼3.45 × 1012 cm–2 eV–1. Our work demonstrates the tremendous potential of WSe2 to open avenues for state-of-the-art electronic, optoelectronic, and quantum-optoelectronic devices using scalable synthesis routes.