Abstract
Defect engineering is an exciting tool for customizing semiconductors' structural and optoelectronic properties. Elaborating programmable methodologies to circumvent energy constraints in multievent inversions expands our understanding of mechanisms governing the functionalization of nanomaterials. Herein, we introduce a novel strategy based on defect incorporation and solution rationalization, which triggers energetically unfavorable cation exchange reactions in extended solids. Using Sb2X3 + Ag (I) → Ag: Sb2X3 (X = S, Se) as a system to model, we demonstrate that incorporating chalcogen vacancies and AgSbVX complex defects into initial thin films (TFs) is crucial for activating long-range solid-state ion diffusion. Additional regulation of the Lewis acidity of auxiliary chemicals provides exceptional conversion yield of the Ag precursor into a solid-state product up to 90%, simultaneously transforming upper matrix layers into AgSbX2. The proposed strategy enables tailoring radiative recombination processes, offers efficiency to invert TFs at moderate temperatures quickly, and yields structures of large areas with substantial antibacterial activity in visible light for a particular system considered. Similar customization can be applied to most sulfides and selenides with controlled reaction yields.
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Electronic Supplementary Information with Additional Figures, Tables, and Experimental Data
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