Real-Time Structural Dynamics at the 3D/2D Perovskite Interface in CsPbBr3/PEA2PbBr4 Nano-heterostructures

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters Pub Date : 2024-12-18 DOI:10.1021/acs.nanolett.4c05021

Xiayan Wu, Nithin Pathoor, Xin Xu, Shun Omagari, Toranosuke Takagi, Martin Vacha

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Abstract

Three-dimensional (3D) and two-dimensional (2D) perovskite hybrid systems, known for their exceptional optoelectronic properties and stability, are revolutionizing optoelectronic materials research. However, fundamental physics of the 3D/2D interfaces and their dynamics remain poorly understood. We use fluorescence microspectroscopy to study the photoluminescence (PL) properties of 3D/2D nano-heterostructures of CsPbBr₃/PEA₂PbBr₄ formed by postgrowth self-assembly. The in situ PL spectra uncover the presence of new structural phases, quasi-2D PEA₂Cs_n–1Pb_nBr_3n+1 layers of varying n, at the 3D/2D interface and demonstrate their reversible restructuring under light excitation at room temperature. The restructuring is a result of layer-by-layer cation diffusion at the epitaxial interfaces, manifested as reversible spectral shifts occurring on a time scale of seconds. Such dynamics ultimately leads to optimized distribution of the quasi-2D phases in the system for efficient energy transfer from the 2D to the 3D phases. Our findings provide new insights into controlling energy flow in 3D/2D perovskites for next-generation optoelectronic devices.

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CsPbBr3/PEA2PbBr4 纳米异质结构中三维/二维过氧化物界面的实时结构动态变化

三维（3D）和二维（2D）包晶石杂化系统以其卓越的光电特性和稳定性而著称，正在为光电材料研究带来革命性的变化。然而，人们对三维/二维界面的基本物理学及其动力学仍然知之甚少。我们利用荧光微光谱技术研究了由生长后自组装形成的铯铋硼3/PEA2PbBr4三维/二维纳米异质结构的光致发光（PL）特性。原位聚光光谱揭示了在三维/二维界面上存在新的结构相，即不同 n 的准二维 PEA2Csn-1PbnBr3n+1 层，并证明了它们在室温光激发下的可逆重组。这种重组是阳离子在外延界面逐层扩散的结果，表现为以秒为单位的可逆光谱移动。这种动态变化最终导致系统中准二维相的优化分布，从而实现从二维相到三维相的高效能量转移。我们的发现为控制三维/二维包晶中的能量流以实现下一代光电器件提供了新的见解。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.