Regulating Exciton Diffusion in Antimony‐Based Perovskite‐Like Single Crystals toward Highly Efficient and Stable Luminescence

Abstract

Organic‐inorganic hybrid metal halide perovskite has played an important role in optoelectronics and photonics due to their extremely high photoluminescence quantum yield (PLQY). However, considering the strong nonmetallic property of antimony (Sb), the excitons in antimony‐based single crystals are usually dissipated in the form of non‐radiative recombination under organic‐inductive effect, which leads to the low PLQY. Herein, two kinds of perovskite‐like single crystals, i.e., (8‐HQ)2SbCl3 and (8‐HQH)SbCl4, are innovatively grown. The density functional theory (DFT) calculations reveal that the unique luminescence characteristics are associated with the inductive effect of organic coordination and exciton effect in the metal octahedral skeleton. When Cl− replaces the organic ligand in (8‐HQ)2SbCl3, the inductive effect is reduced while the self‐trapped exciton effect in the metal octahedron is enhanced. Besides, the theoretical research on electron transmission in a modeling device reveals that the hydrogen bond of organic A‐site in the single crystal promotes the transition of electrons. Based on the luminescent properties of (8‐HQH)SbCl4, the white LED devices are obtained by coating (8‐HQH)SbCl4 and red phosphor on 450 nm LED chips.

A universal supramolecular assembly strategy for achieving efficient tunable white emission and anti-counterfeiting in antimony doped tin(iv)-based vacancy-ordered double perovskites

“…All results illustrate that the dual-emission in pure (AC) 2 SnCl 6 may stem from defect-related emissions, as observed in the previously obtained Sn-based compounds. 32–35 The low emission intensity is not conducive to applying (AC) 2 SnCl 6 practically.…”

“…Therefore, there should be charge transfer between the organic component and inorganic [SnCl 6 ] 2− cluster in pure (AC) 2 SnCl 6 . 50 Generally, the significant contribution of organic ligands to the VBM and CBM in low dimensional metal halides will generate energy level defects and efficient non-radiative recombination, 35 thus eliminating the possibility of PL observed in exciton transitions under photo-absorption. Moreover, Sn 4+ with 4d 10 5s 0 outer-shell electron configuration exhibits a rigid crystal structure and is stereochemically inactive, which is not conducive to yielding efficient emission of the corresponding compounds.…”