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用于光电器件的高效稳定CsNaInCl:Sb@PVDF复合薄膜的原位制备

In Situ Fabrication of Highly Efficient and Stable CsNaInCl: Sb@PVDF Composite Films for Optoelectronic Devices.

作者信息

Li Wen, Dong Yongrun, Xie Ting, Li Tongzhou, Ning Chuang, Huang Tao, Li Zequan, Gao Wei, Zou Bingsuo

机构信息

Guangxi Key Lab of Processing for Non-ferrous Metals and Featured Materials and Key Lab of New Processing Technology for Nonferrous Metals and Materials, Ministry of Education; School of Resources, Environmental and Materials, Guangxi University, Nanning 530004, China.

School of Resources, Environment and Materials, Guangxi University, Nanning, Guangxi 530004, China.

出版信息

ACS Appl Mater Interfaces. 2024 Oct 2;16(39):52921-52931. doi: 10.1021/acsami.4c10918. Epub 2024 Sep 22.

DOI:10.1021/acsami.4c10918
PMID:39307968
Abstract

Lead-free double perovskites (DPs) have superior phase stability and optical properties, which make them competitive for future applications in illumination and displays. However, the preparation of DPs was mainly based on high-temperature heating and hydrochloric acid as a solvent to form powders, which increased the risk and cost of the preparation process and limited its further application. In this study, the growth of CsNaInCl: Sb DPs in polyvinylidene difluoride (PVDF) films was achieved using an in situ fabrication strategy with DMSO as the solvent. The prepared CsNaInCl: Sb@PVDF composite films (CFs) can achieve a bright blue emission under 302 nm irradiation. To achieve the optimal luminescent performance of CFs, the photoluminescence (PL) intensity of CsNaInCl: Sb@PVDF CFs under various in situ preparation conditions was compared. In addition, the photoluminescence quantum yield (PLQY) of CFs was increased from 0.72% to 83.77% by adjusting the doping amount of Sb, and the fluorescence lifetimes and were 131.08 and 1048.52 ns, respectively. Temperature-dependent PL spectroscopy and density functional theory (DFT) calculations indicate that these excellent optical properties are derived from the self-trapped excitons (STEs) at the [SbCl] octahedron and [InCl] octahedron connected via Cl-Na-Cl. The CFs also demonstrated excellent environmental stability, maintaining a relatively stable PL intensity even under conditions of water immersion, high temperatures, and ultraviolet (UV) radiation. Finally, we used the CFs to assemble a blue light-emitting device (LED), which showed good and stable blue emission performance at different currents. This work can provide a new idea for preparing DPs, which is conducive to promoting their commercial application in high-performance optoelectronic devices.

摘要

无铅双钙钛矿(DPs)具有优异的相稳定性和光学性能,这使其在未来的照明和显示应用中具有竞争力。然而,DPs的制备主要基于高温加热并以盐酸为溶剂形成粉末,这增加了制备过程的风险和成本,并限制了其进一步应用。在本研究中,使用以二甲基亚砜(DMSO)为溶剂的原位制备策略实现了CsNaInCl:Sb DPs在聚偏二氟乙烯(PVDF)薄膜中的生长。制备的CsNaInCl:Sb@PVDF复合薄膜(CFs)在302nm照射下可实现亮蓝色发射。为了实现CFs的最佳发光性能,比较了CsNaInCl:Sb@PVDF CFs在各种原位制备条件下的光致发光(PL)强度。此外,通过调整Sb的掺杂量,CFs的光致发光量子产率(PLQY)从0.72%提高到了83.77%,荧光寿命分别为131.08和1048.52ns。温度相关的PL光谱和密度泛函理论(DFT)计算表明,这些优异的光学性能源自通过Cl-Na-Cl连接的[SbCl]八面体和[InCl]八面体处的自陷激子(STEs)。CFs还表现出优异的环境稳定性,即使在水浸、高温和紫外线(UV)辐射条件下也能保持相对稳定的PL强度。最后,我们使用CFs组装了一个蓝色发光器件(LED),其在不同电流下均表现出良好且稳定的蓝色发光性能。这项工作可为制备DPs提供新思路,有助于推动其在高性能光电器件中的商业应用。

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