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1.
Nano Lett ; 24(21): 6410-6416, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38767286

RESUMO

CsPbI3 perovskite quantum dots (QDs) could achieve pure-red emission by reducing their size, but the increased exciton binding energy (EB) and surface defects for the small-sized QDs (SQDs) cause severe Auger and trap recombinations, thus worsening their electroluminescence (EL) performance. Herein, we utilize the dangling bonds of the SQDs as a driving force to accelerate KI dissolution to solve its low solubility in nonpolar solvents, thereby allowing K+ and I- to bond to the surface of SQDs. The EB of the SQDs was decreased from 305 to 51 meV because of the attraction of K+ to electrons, meanwhile surface vacancies were passivated by K+ and I-. The Auger and trap recombinations were simultaneously suppressed by this difunctional ligand. The SQD-based light-emitting diode showed a stable pure-red EL peak of 639 nm, an external quantum efficiency of 25.1% with low roll-off, and a brightness of 5934 cd m-2.

2.
J Am Chem Soc ; 146(20): 13934-13948, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38741463

RESUMO

Double perovskite films have been extensively studied for ferroelectric order, ferromagnetic order, and photovoltaic effects. The customized ion combinations and ordered ionic arrangements provide unique opportunities for bandgap engineering. Here, a synergistic strategy to induce chemical strain and charge compensation through inequivalent element substitution is proposed. A-site substitution of the barium ion is used to modify the chemical valence and defect density of the two B-site elements in Bi2FeMnO6 double perovskite epitaxial thin films. We dramatically increased the ferroelectric photovoltaic effect to ∼135.67 µA/cm2 from 30.62 µA/cm2, which is the highest in ferroelectric thin films with a thickness of less than 100 nm under white-light LED irradiation. More importantly, the ferroelectric polarization can effectively improve the photovoltaic efficiency of more than 5 times. High-resolution HAADF-STEM, synchrotron-based X-ray diffraction and absorption spectroscopy, and DFT calculations collectively demonstrate that inequivalent ion plays a dual role of chemical strain (+1.92 and -1.04 GPa) and charge balance, thereby introducing lattice distortion effects. The reduction of the oxygen vacancy density and the competing Jahn-Teller distortion of the oxygen octahedron are the main phenomena of the change in electron-orbital hybridization, which also leads to enhanced ferroelectric polarization values and optical absorption. The inequivalent strategy can be extended to other double perovskite systems and applied to other functional materials, such as photocatalysis for efficient defect control.

3.
Mater Horiz ; 10(10): 4389-4397, 2023 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-37465904

RESUMO

Polarization rotation caused by various strains, such as substrate and/or chemical strain, is essential to control the electronic structure and properties of ferroelectric materials. This study proposes anion-induced polarization rotation with chemical strain, which effectively improves ferroelectricity. A method for the sulfurization of BiFeO3 thin films by introducing sulfur anions is presented. The sulfurized films exhibited substantial enhancement in room-temperature ferroelectric polarization through polarization rotation and distortion, with a 170% increase in the remnant polarization from 58 to 100.7 µC cm-2. According to first-principles calculations and the results of X-ray absorption spectroscopy and high-angle annular dark-field scanning transmission electron microscopy, this enhancement arose from the introduction of S atoms driving the re-distribution of the lone-pair electrons of Bi, resulting in the rotation of the polarization state from the [001] direction to the [110] or [111] one. The presented method of anion-driven polarization rotation might enable the improvement of the properties of oxide materials.

4.
Materials (Basel) ; 13(20)2020 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-33066396

RESUMO

The microwave sintering of glass-ceramics, non-thermal microwave effect, and crystal growth mechanism remain important challenges in materials science. In this study, we focus on developing approaches to affect crystal growth in the glass network of glass-ceramics by microwave heating, rather than performing a single study on the crystal structure and type. Raman spectroscopy is used to detect the structure of the glass network. We demonstrated that the non-thermal microwave effect promoted the diffusion of metal ions, which promoted the aggregation and precipitation of metal ions in the glass network to form crystals. The samples produced by microwave heating contain more non-bridging oxygen bonds than conventional sintered samples; therefore, the non-thermal microwave effect has a depolymerization effect on the glass network of the sample. Under the influence of microwave field, many metal ions precipitate, which precipitates many crystal nuclei. In addition, many active metal ions are captured during the crystal nucleus growth, which shortens the sintering process of glass-ceramics.

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