Abstract
Lead-free halide double perovskites (DPs) [A2B(I)B(III)X6] (A: monovalent cation, B(I): monovalent cation, B(II): trivalent cation, X: halide anion) has drawn tremendous attention because of their environmental-friendliness and high stability compared to traditional lead-based perovskites ABX3 (A: monovalent cation; B: Pb2+; X: halide anion). The optoelectronic properties of DPs are, however, compromised. This work provides a methodology for improving the photophysical properties of DPs and achieving high-efficiency warm white light emission. First principles density functional theory (DFT) was used in material design and the ligand-free synthesis of halide DP Cs2Ag1−xKxIn0.875Bi0.125Cl6 (x ≤ 0.60) via a facile recrystallization process was demonstrated. The compositional tuning of K+ to Ag+ resulted in an improvement in photophysical properties. Independent of K+ content, all the samples exhibit strong absorption at a wavelength of λmax ∼ 375 nm with a direct bandgap which is consistent with our DFT calculation results. Broadband photoluminescence (PL) emission profiles covering the spectra from blue to deep red (405–820 nm at λmax ∼ 629 nm) were observed. Besides, with an optimized K+ alloying content of 0.20, the optical performance of these halide DPs was impressively regulated, demonstrating improved photoluminescence quantum yield (PLQY) of host Cs2AgInCl6 crystals from ∼ 2.70 % (x = 0) to ∼15.96 % (x = 0.20), due to increased radiative recombination of self-trapped excitons. the highest report for such structures. It also shows high stability over 180 days. Furthermore, the use of blue-emitting CsPbBr3 and DP Cs2Ag0.80K0.20In0.875Bi0.125Cl6 as color conversion layers in white light-emitting diodes (LEDs) demonstrates that high-quality white light emission with the CIE color coordinate of (0.387, 0.385) and a correlated color temperature (CCT) of 3878 K, color rendering index (CRI) of 85, and luminous efficacy of radiation (LER) of 214 lm/W. Hence, the research work provides insight into realizing environmentally friendly and high-efficiency white light emission with high color quality by using earth-abundant elements and the low-cost synthesis method.
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