Two‐Dimensional Bis(dithiolene)iron(II) Self‐Powered UV Photodetectors with Ultrahigh Air Stability

Organometallic two‐dimensional (2D) nanosheets with tailorable components have recently fascinated the optoelectronic communities due to their solution‐processable nature. However, the poor stability of organic molecules may hinder their practical application in photovoltaic devices. Instead of conventional organometallic 2D nanosheets with low weatherability, an air‐stable π‐conjugated 2D bis(dithiolene)iron(II) (FeBHT) coordination nanosheet (CONASH) is synthesized via bottom‐up liquid/liquid interfacial polymerization using benzenehexathiol (BHT) and iron(II) ammonium sulfate [Fe(NH(4))(2)(SO(4))(2)] as precursors. The uncoordinated thiol groups in FeBHT are easily oxidized, but the Fe(NH(4))(2)(SO(4))(2) dissociation rate is slow, which facilitates the protection of sulfur groups by iron(II) ions. The density functional theory calculates that the resultant FeBHT network gains the oxygen‐repelling function for oxidation suppression. In air, the FeBHT CONASH exhibits self‐powered photoresponses with short response times (<40 ms) and a spectral responsivity of 6.57 mA W(−1), a specific detectivity of 3.13 × 10(11) Jones and an external quantum efficiency of 2.23% under 365 nm illumination. Interestingly, the FeBHT self‐powered photodetector reveals extremely high long‐term air stability, maintaining over 94% of its initial photocurrent after aging for 60 days without encapsulation. These results open the prospect of using organometallic 2D materials in commercialized optoelectronic fields.