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Broadband emissive perovskites are next‐generation materials for solid‐state lighting and radiative detection. However, white‐emitting perovskites are generally synthesized by regulating B/X sites, while not enough attention is paid to the A‐site, which is thought to hardly affect the band‐edge structures and optoelectronic properties. Here, a series of Sb3+‐doped In‐based 0D halide perovskite derivatives are described with various organoammonium cations in A‐sites. Warm‐white light emitting across the visible spectrum (450–850 nm), large Stokes shifts, and high photoluminescence quantum yields are easily tunable by molecularly tailoring A‐site cations. These features enable a light yield up to 60976 Photons/MeV as X‐ray scintillator, and a detection limit of 90 nGyair/s that is ≈60 times lower than the medical requirement. It is proved that A‐site plays a critical role in determining the degree of distortion of polyhedra, which influences the broadband photoluminescence and self‐trapped exciton (STE) dominates the emission process. Moreover, for the first time, via the incorporation of 2,6‐dimethylpiperazine, a mixed A‐site regulating strategy produces a standard white‐light emission, which originates from the blue‐light and yellow‐light related to various STE emission centers. It is foreseen that this strategy highlights the expanded role of A‐site and the importance of rethinking A‐sites in perovskites. [ABSTRACT FROM AUTHOR]

Herein, the first study on the scintillation properties of CsCu2X3 and Cs3Cu2X5 (where X: Cl−, Br−, I−) is presented, describing their charged particle‐induced luminescence involving electrons, protons, α‐particles, and heavy ions, as well as revealing their capabilities on the timing and spectroscopic evaluation of single‐particle events. The thin layers are prepared with a simple and cost‐effective deposition procedure, without the incorporation of external dopants, exploiting the intrinsic radiative recombination observed in low‐dimensional perovskites. The combined effect of the high binding energy and localized stability of self‐trapped excitons, large Stokes shift, defect tolerance, and the high excitation density along the particle track leads to the emergence of boosted scintillation pulses. The observations demonstrate the first use of inorganic thin‐film scintillators with optical pulse characteristics and light yield competitive with doped single crystal scintillators, while also providing improved structural and functional stability under extreme environmental conditions. [ABSTRACT FROM AUTHOR]