Releasing trapped excitons in 2D perovskites via pressure annealing: a cooperative interplay between lattice strain and the electronic structure†

IF 6.4 2区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Materials Chemistry Frontiers Pub Date : 2024-12-11 DOI:10.1039/D4QM00780H

Andre L. M. Freitas, Naidel A. M. S. Caturello, Aryane Tofanello, Ulisses F. Kaneko, Lucas E. Correa, Ricardo D. dos Reis, Fabio F. Ferreira, Gustavo M. Dalpian and Jose A. Souza

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Abstract

Characteristic photon emissions in low-dimensional hybrid perovskites are strongly related to inherent distortions in the crystal lattice. These cooperative distortions, influenced by organic spacers and the confined BX₆ octahedral arrangement, allow for the manipulation and control of the emitted photon energy and its nature. Herein, we observed a complex dynamic where photon emissions at both low and high energies emerge, depending on octahedral distortion and the application of hydrostatic pressure. Our results demonstrated that samples featuring different octahedral sizes and distortions but having a common organic spacer (BA₂MAPb₂Br₇ and BA₂MAPb₂I₇) showed low-energy photon emission attributed to self-trapped excitons (STEs), which can be tuned towards free exciton (FE) states through pressure annealing. Experimental and theoretical results revealed that octahedral distortions in 2D perovskites played a crucial role in controlling emission, disclosing their complex structure and electronic relationship.

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通过压力退火释放二维钙钛矿中的捕获激子：晶格应变与电子结构之间的协同相互作用†

低维杂化钙钛矿中的特征光子发射与晶格中的固有畸变密切相关。受有机间隔层和受限的BX6八面体排列的影响，这些协同畸变允许操纵和控制发射的光子能量及其性质。在这里，我们观察到一个复杂的动态，其中低能和高能光子发射都出现，这取决于八面体畸变和静水压力的应用。研究结果表明，具有不同八面体尺寸和畸变但具有共同有机间隔层（BA2MAPb2Br7和BA2MAPb2I7）的样品显示出由自捕获激子（STEs）引起的低能光子发射，可以通过压力退火将其调谐到自由激子（FE）状态。实验和理论结果表明，二维钙钛矿的八面体畸变在控制发射中起着至关重要的作用，揭示了它们复杂的结构和电子关系。

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来源期刊

Materials Chemistry Frontiers Materials Science-Materials Chemistry

CiteScore

12.00

自引率

2.90%

发文量

313

期刊介绍： Materials Chemistry Frontiers focuses on the synthesis and chemistry of exciting new materials, and the development of improved fabrication techniques. Characterisation and fundamental studies that are of broad appeal are also welcome. This is the ideal home for studies of a significant nature that further the development of organic, inorganic, composite and nano-materials.