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Sci Adv ; 6(4): eaay4045, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-32042900


Achieving perovskite-based high-color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high-color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate temperature-induced device degradation by investigating the crystal structural and spectral evolution dynamics via in situ temperature-dependent single-crystal x-ray diffraction, photoluminescence (PL) characterization, and density functional theory calculation. The PL peak becomes asymmetrically broadened with a marked intensity decay, as temperature increases owing to [PbBr6]4- octahedra tilting and the organic chain disordering, which results in bandgap decrease. This study indicates that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.

Proc Natl Acad Sci U S A ; 116(47): 23404-23409, 2019 Nov 19.
Artigo em Inglês | MEDLINE | ID: mdl-31685626


Phase transitions in halide perovskites triggered by external stimuli generate significantly different material properties, providing a great opportunity for broad applications. Here, we demonstrate an In-based, charge-ordered (In+/In3+) inorganic halide perovskite with the composition of Cs2In(I)In(III)Cl6 in which a pressure-driven semiconductor-to-metal phase transition exists. The single crystals, synthesized via a solid-state reaction method, crystallize in a distorted perovskite structure with space group I4/m with a = 17.2604(12) Å, c = 11.0113(16) Å if both the strong reflections and superstructures are considered. The supercell was further confirmed by rotation electron diffraction measurement. The pressure-induced semiconductor-to-metal phase transition was demonstrated by high-pressure Raman and absorbance spectroscopies and was consistent with theoretical modeling. This type of charge-ordered inorganic halide perovskite with a pressure-induced semiconductor-to-metal phase transition may inspire a range of potential applications.

Proc Natl Acad Sci U S A ; 116(26): 12648-12653, 2019 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-31189607


Ion exchange, as a postsynthetic transformation strategy, offers more flexibilities in controlling material compositions and structures beyond direct synthetic methodology. Observation of such transformation kinetics on the single-particle level with rich spatial and spectroscopic information has never been achieved. We report the quantitative imaging of anion exchange kinetics in individual single-crystalline halide perovskite nanoplates using confocal photoluminescence microscopy. We have systematically observed a symmetrical anion exchange pathway on the nanoplates with dependence on reaction time and plate thickness, which is governed by the crystal structure and the diffusion-limited transformation mechanism. Based on a reaction-diffusion model, the halide diffusion coefficient was estimated to be on the order of [Formula: see text] This diffusion-controlled mechanism leads to the formation of 2D perovskite heterostructures with spatially resolved coherent interface through the precisely controlled anion exchange reaction, offering a design protocol for tailoring functionalities of semiconductors at the nano-/microscale.

Nano Lett ; 18(11): 6967-6973, 2018 11 14.
Artigo em Inglês | MEDLINE | ID: mdl-30265549


Surface condition plays an important role in the optical performance of semiconductor materials. As new types of semiconductors, the emerging metal-halide perovskites are promising for next-generation optoelectronic devices. We discover significantly improved light-emission efficiencies in lead halide perovskites due to surface oxygen passivation. The enhancement manifests close to 3 orders of magnitude as the perovskite dimensions decrease to the nanoscale, improving external quantum efficiencies from <0.02% to over 12%. Along with about a 4-fold increase in spontaneous carrier recombination lifetimes, we show that oxygen exposure enhances light emission by reducing the nonradiative recombination channel. Supported by X-ray surface characterization and theoretical modeling, we propose that excess lead atoms on the perovskite surface create deep-level trap states that can be passivated by oxygen adsorption.