High-performance and scalable metal-chalcogenide semiconductors and devices via chalco-gel routes

We report a general strategy for obtaining high-quality, large-area metal-chalcogenide semiconductor films from precursors combining chelated metal salts with chalcoureas or chalcoamides. Using conventional organic solvents, such precursors enable the expeditious formation of chalco-gels, which are easily transformed into the corresponding high-performance metal-chalcogenide thin films with large, uniform areas. Diverse metal chalcogenides and their alloys (MQ : M = Zn, Cd, In, Sb, Pb; Q = S, Se, Te) are successfully synthesized at relatively low processing temperatures (<400°C). The versatility of this scalable route is demonstrated by the fabrication of large-area thin-film transistors (TFTs), optoelectronic devices, and integrated circuits on a 4-inch Si wafer and 2.5-inch borosilicate glass substrates in ambient air using CdS, CdSe, and In₂Se₃ active layers. The CdSe TFTs exhibit a maximum field-effect mobility greater than 300 cm² V^-1 s^-1 with an on/off current ratio of >10⁷ and good operational stability (threshold voltage shift < 0.5 V at a positive gate bias stress of 10 ks). In addition, metal chalcogenide-based phototransistors with a photodetectivity of >10¹³ Jones and seven-stage ring oscillators operating at a speed of ~2.6 MHz (propagation delay of < 27 ns per stage) are demonstrated.