Ternary Ta2NiSe5 Flakes for a High‐Performance Infrared Photodetector

Multielemental systems enable the use of multiple degrees of freedom for control of physical properties by means of stoichiometric variation. This has attracted extremely high interest in the field of 2D optoelectronics in recent years. Here, for the first time, multilayer 2D ternary Ta₂NiSe₅ flakes are successfully fabricated using a mechanical exfoliation method from chemical vapor transport synthesized high quality bulk and the optoelectronic properties are systematically investigated. Importantly, a high responsivity of 17.21 A W^?1 and high external quantum efficiency of 2645% are recorded from an as‐fabricated photodetector at room temperature in air; this is superior to most other 2D materials‐based photodetectors that have been reported. More intriguingly, a usual sublinear and an unusual superlinear light‐intensity‐dependent photocurrent are observed under air and vacuum, respectively. These excellent and special properties make multilayer ternary Ta₂NiSe₅ a highly competitive candidate for future infrared optoelectronic applications and an interesting platform for photophysics studies.