Electrode‐Induced Self‐Healed Monolayer MoS₂ for High Performance Transistors and Phototransistors

Abstract Contact engineering for monolayered transition metal dichalcogenides (TMDCs) is considered to be of fundamental challenge for realizing high‐performance TMDCs‐based (opto) electronic devices. Here, an innovative concept is established for a device configuration with metallic copper monosulfide (CuS) electrodes that induces sulfur vacancy healing in the monolayer molybdenum disulfide (MoS₂) channel. Excess sulfur adatoms from the metallic CuS electrodes are donated to heal sulfur vacancy defects in MoS₂ that surprisingly improve the overall performance of its devices. The electrode‐induced self‐healing mechanism is demonstrated and analyzed systematically using various spectroscopic analyses, density functional theory (DFT) calculations, and electrical measurements. Without any passivation layers, the self‐healed MoS₂ (photo)transistor with the CuS contact electrodes show outstanding room temperature field effect mobility of 97.6 cm² (Vs)⁻¹, On/Off ratio > 10⁸, low subthreshold swing of 120 mV per decade, high photoresponsivity of 1 × 10⁴ A W⁻¹, and detectivity of 10¹³ jones, which are the best among back‐gated transistors that employ 1L MoS₂. Using ultrathin and flexible 2D CuS and MoS₂, mechanically flexible photosensor is also demonstrated, which shows excellent durability under mechanical strain. These findings demonstrate a promising strategy in TMDCs or other 2D material for the development of high performance and functional devices including self‐healable sulfide electrodes.