Near-unity quantum yield hybrid antimony halide for solid-state lighting and fingerprint detection

Abstract

Zero-dimensional metal halides have emerged as a research frontier owing to their unique photoelectric properties. However, the preparation of low-dimensional materials that simultaneously exhibit high photoluminescence quantum yield (PLQY) and stability remains challenging. Herein, we successfully grow a single crystal of zero-dimensional antimony-based halide of (ATPPO)2SbCl5 (ATPPO = acetyltriphenylphosphine chloride). The crystal exhibits a broadband orange emission centered at 605 nm when excited at 387 nm, along with an additional high-energy emission peak at 482 nm when excited at 338 nm. Combined spectroscopic analysis and density functional theory calculations confirm that the dual-band luminescence originates from the radiative recombination of singlet and triplet self-trapped excitons within the [SbCl5]2 units. Notably, the material exhibits negative thermal quenching behavior with increasing temperature in the range of 80–255 K, demonstrating enhanced fluorescence intensity with increasing temperature. Moreover, it achieves up to 100% PLQY at room temperature while maintaining high thermal stability, retaining 95.8% of its luminescence intensity at 373 K compared to that at room temperature. Leveraging its exceptional luminescence efficiency and thermal stability, we fabricated white light-emitting diodes with an average color rendering index (CRI) of 92.6 (R9 = 91) using this phosphor, highlighting its potential in solid-state lighting applications. Additionally, the material effectively reveals multi-level fingerprint structures and latent fingerprints on various common evidence substrates upon 365 nm UV excitation, strongly demonstrating its practical value in forensic evidence detection.