Molecular Doping of 2D Indium Selenide for Ultrahigh Performance and Low‐Power Consumption Broadband Photodetectors

Two-dimensional (2D) photodetecting materials have shown superior performances over traditional materials (e.g., silicon, perylenes), which demonstrate low responsivity (R) (<1 AW−1), external quantum efficiency (EQE) (<100%), and limited detection bandwidth. Recently, 2D indium selenide (InSe) emerged as high-performance active material in field-effect transistors and photodetectors, whose fabrication required expensive and complex techniques. Here, it is shown for the first time how molecular functionalization with a common surfactant molecule (didodecyldimethylammonium bromide) (DDAB) represents a powerful strategy to boost the (opto)electronic performances of InSe yielding major performance enhancements in phototransistors, Schottky junctions, and van der Waals heterostructures via a lithography-compatible fabrication route. The functionalization can controllably dope and heal vacancies in InSe, resulting in ultrahigh field-effect mobility (10^3 cm2 V−1 s−1) and photoresponsivity (10^6 A W−1), breaking the record of non-graphene-contacted 2D photodetectors. The strategy towards the molecular doping of 2D photodetecting materials is efficient, practical, up-scalable, and operable with ultra-low power input, ultimately paving the way to next-generation 2D opto-electronics.