Publication date: 15th December 2025
High-entropy alloying (HEA) has recently emerged as a powerful strategy for engineering structural stability and electronic functionality across a wide range of materials. While HEA concepts have been successfully applied to metallic alloys and oxide ceramics, their implementation in halide perovskite nanocrystals (PNCs) remains at an early stage. In particular, the potential of HEA to benefit quantum-light technologies, especially single-photon sources (SPSs) operating at room temperature (RT), has not yet been explored.
Here, we report the first demonstration that HEA engineering intrinsically enhances radiative recombination, exciton coherence, and single-photon purity in PNCs. By incorporating transition metals (Mn, Zn, Ni) onto the B-site of CsPb(Cl/Br)3 PNCs, we create a high-entropy crystal lattice that provides a fundamentally altered excitonic environment. Systematic photophysical measurements reveal that HEA-PNCs exhibit significantly faster radiative decay, suppressed trap-assisted recombination, and reduced electron-phonon coupling. In addition, we conducted ab initio molecular dynamics simulations that show that high-entropy incorporation leads to reduced phonon interactions and enhanced exciton coherence. Our HEA-PNCs achieve a single-photon emission purity of 96%, nearly complete blinking suppression, and excellent photostability at room temperature, representing the strongest intrinsic SPS performance ever reported for PNCs. Unlike previous approaches requiring plasmonic Purcell enhancement, ligand engineering, or low-temperature operation, our strategy uses a materials-intrinsic mechanism that is fully compatible with scalable colloidal synthesis. Overall, this work demonstrates that HEA is a powerful, generalizable design principle for achieving robust room-temperature quantum-light emission in perovskite nanocrystals.
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