单粒子光致发光将热处理与铯-溴化铅纳米晶体阱分布的非均质性联系起来

IF 9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Dong Wang, Jie Chen, Dongyan Zhang, Dariusz M. Niedzwiedzki, Richard A. Loomis, Bryce Sadtler
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引用次数: 0

摘要

了解卤化铅钙钛矿纳米晶体的降解机制对其未来在光电器件中的应用至关重要。我们报告了单粒子测量的光致发光铯-溴化铅纳米晶体包覆二氧化硅外壳(CsPbBr3@SiO2)。通过相关成像,我们量化了相同纳米晶体在不同温度下退火前后荧光强度轨迹的变化。我们观察到,在70°C和100°C退火后,几乎相同数量的CsPbBr3@SiO2纳米晶体在发射状态下花费的时间增加而减少。另一方面,在120℃下退火会使大多数纳米晶体的导通分数降低,相应地,在该温度下退火的薄膜的光致发光强度也会大幅降低。我们将单个纳米晶体之间的行为差异归因于最初存在的陷阱态分布的异质性。对CsPbBr3@SiO2纳米晶体薄膜进行的x射线光电子、时间分辨光致发光和瞬态吸收光谱分析表明,热退火通过钝化表面Pb离子来修复电子陷阱,同时通过形成Pb和Cs空位来产生空穴陷阱。这些平行过程的相对速率取决于退火温度,这对于在高温下工作的光电器件中开发卤化铅钙钛矿纳米晶体的钝化策略非常重要。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Single-particle photoluminescence connects thermal processing with heterogeneity in the trap distribution of cesium lead bromide nanocrystals

Understanding the mechanisms of degradation in lead halide perovskite nanocrystals is critical for their future application in optoelectronic devices. We report single-particle measurements of the photoluminescence from cesium lead bromide nanocrystals coated with a silica shell (CsPbBr3@SiO2). Through correlative imaging, we quantified changes in the fluorescence intensity trajectories of the same nanocrystals before and after annealing them at different temperatures. We observe that nearly equal numbers of CsPbBr3@SiO2 nanocrystals exhibit an increase versus decrease in the amount of time they spend in an emissive state after annealing at temperatures of 70 and 100 °C. On the other hand, annealing at 120 °C produces a decrease in the on-fraction for most nanocrystals and, correspondingly, a substantial decrease in the photoluminescence intensity for a thin film annealed at this temperature. We attribute the differences in behavior among individual nanocrystals to heterogeneity in the distribution of trap states that are initially present. X-ray photoelectron, time-resolved photoluminescence, and transient absorption spectroscopies performed on thin films of CsPbBr3@SiO2 nanocrystals indicate that thermal annealing heals electron traps by passivating surface Pb ions and simultaneously creates hole traps through the formation of Pb and Cs vacancies. The relative rates of these parallel processes depend on the annealing temperature, which are important to account for when developing passivation strategies for lead halide perovskite nanocrystals in optoelectronic devices that will operate at elevated temperatures.

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来源期刊
Nano Research
Nano Research 化学-材料科学:综合
CiteScore
14.30
自引率
11.10%
发文量
2574
审稿时长
1.7 months
期刊介绍: Nano Research is a peer-reviewed, international and interdisciplinary research journal that focuses on all aspects of nanoscience and nanotechnology. It solicits submissions in various topical areas, from basic aspects of nanoscale materials to practical applications. The journal publishes articles on synthesis, characterization, and manipulation of nanomaterials; nanoscale physics, electrical transport, and quantum physics; scanning probe microscopy and spectroscopy; nanofluidics; nanosensors; nanoelectronics and molecular electronics; nano-optics, nano-optoelectronics, and nano-photonics; nanomagnetics; nanobiotechnology and nanomedicine; and nanoscale modeling and simulations. Nano Research offers readers a combination of authoritative and comprehensive Reviews, original cutting-edge research in Communication and Full Paper formats. The journal also prioritizes rapid review to ensure prompt publication.
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