AbstractSelf‐trapped exciton (STE) emission, typified by antimony (Sb), with broadband characteristics, represents the next generation of materials for solid‐state lighting and radiation detection. However, little is known about the multiexciton behavior of the Sb emission center. Here, we proposed a general approach for designing antimony‐centered multi‐exciton emitting materials through self‐assembly. Benefitting from controllable multiexciton behavior, dual‐band white light emission spanning the entire visible spectrum was achieved. Relying on the reduction of an effective atomic number brought by self‐assembly, excellent scintillation response to β‐rays was attained. This study offers unprecedented insight into hybrid single/triple STE emission and unveils new avenues for single‐emitter white‐light emission, as well as radiographic testing using low‐risk β‐rays as sources.
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