Tin (Sn)-based perovskite light-emitting diodes (LEDs), featuring environmental friendliness and low toxicity, have attracted growing interest as light sources for high-definition displays, medical and health monitoring applications. However, the widespread existing defects arising from the rapid crystallization and the undesirable oxidation of Sn2+ markedly limit the efficiency and brightness of current Sn-based perovskite LEDs. Herein, we develop an 0D-2D heterophasic transition strategy to promote the performance of PEA2SnI4 perovskite films. The results demonstrate that the formation of heterophase extends the processing time window of perovskites, thereby enabling effective modulation and optimization of films crystallization process by regulating initial nucleation. Finally, the fabricated device based on the optimized PEA2SnI4 films achieves a maximum external quantum efficiency (EQE) of 9% and a luminance of 1253.3 cd/m2, representing one of the highest performances reported to date for PEA2SnI4-based perovskite LEDs. Furthermore, the fabricated device was successfully employed as light sources for human cardiac pulse detection, achieving performances comparable to that of commercial detectors, representing the first demonstration of such functionality in lead-free perovskite systems.
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The vacancy-ordered quadruple perovskite Cs4CdBi2Cl12, as a newly-emerging lead-free perovskite system, has attracted great research interest due to its excellent stability and direct band gap. However, the poor luminescence performance limits its application in light-emitting diodes (LEDs) and other fields. Herein, for the first time, an Ag+ ion doping strategy was proposed to greatly improve the emission performance of Cs4CdBi2Cl12 synthesized by hydrothermal method. Density functional theory calculations combined with experimental results evidence that the weak orange emission from Cs4CdBi2Cl12 is attributed to the phonon scattering and energy level crossing due to the large lattice distortion under excited states. Fortunately, Ag+ ion doping breaks the intrinsic crystal field environment of Cs4CdBi2Cl12, suppresses the crossover between ground and excited states, and reduces the energy loss in the form of nonradiative recombination. At a critical doping amount of 0.8%, the emission intensity of Cs4CdBi2Cl12:Ag+ reaches the maximum, about eight times that of the pristine sample. Moreover, the doped Cs4CdBi2Cl12 still maintains excellent stability against heat, ultraviolet irradiation, and environmental oxygen/moisture. The above advantages make it possible for this material to be used as solid-state phosphors for white LEDs applications, and the Commission International de I’Eclairage color coordinates of (0.31, 0.34) and high color rendering index of 90.6 were achieved. More importantly, the white LED demonstrates remarkable operation stability in air ambient, showing almost no emission decay after a long working time for 48 h. We believe that this study puts forward an effective ion-doping strategy for emission enhancement of vacancy-ordered quadruple perovskite Cs4CdBi2Cl12, highlighting its great potential as efficient emitter compatible for practical applications.
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