Abstract
AbstractDoping Mn2+ in newly emerged lead‐free metal halides to access versatile optoelectronic applications is highly desired. However, understanding the chemical pathway of Mn2+ doping and precisely controlling it remains challenging. Here, the crucial role of the initial surface adsorption of Mn2+ in doping kinetics is demonstrated, and the adsorption step is effectively optimized by a moderate Lewis base ligand. The results show that not only the doping concentration of Mn2+ in Cs3Cu2I5 is modulated flexibly but also the produced Cs3Cu2I5:Mn2+ microcrystals exhibit tuned photoluminescence/radioluminescence properties, indicating their applicability in anti‐counterfeiting and X‐ray imaging. Systematic experimental and theoretical outcomes reveal that the moderate Lewis base ligand dually links Mn2+ (hard acid) and Cu+ (soft acid) on the matrix surface, which improves the initial surface adsorption of the dopant and further promotes the doping step. This study contributes a simple strategy for simply controlling Mn2+ doping in Cu(I)‐based halides and also opens a new avenue for understanding the fundamentals of doping dynamics in metal halide systems.
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