Electroluminescence From a 1D Metal–Organic Chalcogenide Enabled by a Minute‐Scale Facile Synthesis

Abstract Metal–organic chalcogenides (MOCs) represent a unique materials platform promising to overcome the respective stability and structural integrity challenges of perovskites and functionalized dichalcogenides. However, their practical application is hindered by slow, multi‐day synthesis methods that produce low‐quality films. Here, these challenges are addressed with a vapor‐assisted solution process that enables the ambient‐pressure fabrication of 1D MOC, silver(I) 2‐methyl ester benzenethiolate (AgSPhCOOMe), films within 5 min. The resulting dense, pinhole‐free AgSPhCOOMe films exhibit a high photoluminescence quantum yield of 37.5%, with bright, broadband emission originating from self‐trapped excitons due to the material's strong electron‐phonon coupling. This scalable synthesis platform enables the successful integration of these MOCs into light‐emitting diodes, demonstrating electroluminescence from this material class. By engineering the charge‐transport layers to achieve balanced injection, a maximum external quantum efficiency of ≈0.1% is achieved. The in situ photoelectron spectroscopy analysis reveals that a significant electron injection barrier (0.62 eV) remains even in the optimized device, identifying this as the main efficiency bottleneck. Therefore, this work provides a foundational platform for MOC‐based devices and a clear roadmap focused on new ligands and interface engineering to realize their full potential as high‐performance, solution‐processable emitters.