Conformational Disorder of Organic Cations Induces Charge Localization in 3D Lead Iodide Perovskitoids toward Sensitive Photodetectors

IF 8.7 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-08-15 DOI:10.1021/acsmaterialslett.5c00995

Biqi He, Kuan Kuang, Mingkai Li, Jie Yang, Lei Zhang*, Yunbin He* and Junnian Chen*,

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Abstract

Three-dimensional (3D) hybrid halide perovskitoids have drawn intense attention in the optoelectronic fields. Therefore, understanding the structural effects on the charge carrier behavior is essential for device optimization. Herein, we establish the correlation between the conformational disorder of cations and the charge carrier property in 3D perovskitoids using computational and experimental investigations. It is shown that the conformational disorder of N,N′-dimethyl-1,3-propane diammonium (M₂PDA) cations induces great distortion of the [Pb₂I₁₀]^6– inorganic framework in 3D (M₂PDA)Pb₂I₆, leading to distinct charge localization. Moreover, the cation configuration disorder suppresses defect formation, thereby reducing lattice microstrain. These modifications effectively elongate the carrier lifetime and diminish carrier scattering to facilitate charge carrier transport. As a result, a photodetector assembled from (M₂PDA)Pb₂I₆ single crystals achieves a satisfying on/off current ratio of 1.42 × 10⁴ and responsivity of 0.55 A W^–1, ranking among the highest-performing devices based on 3D perovskitoids. Moreover, the (M₂PDA)Pb₂I₆ single crystals display superior stability in 100% isopropanol.

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有机阳离子的构象紊乱诱导三维碘化铅钙钛矿向敏感光电探测器的电荷定位

三维（3D）杂化卤化物钙钛矿在光电领域引起了广泛的关注。因此，了解结构对载流子行为的影响对器件优化至关重要。本文通过计算和实验研究，建立了三维类钙钛矿中阳离子的构象紊乱与载流子性质之间的关系。结果表明，N,N ' -二甲基-1,3-丙烷二铵（M2PDA）阳离子的构象紊乱导致[Pb2I10]6 -无机骨架在三维（M2PDA）Pb2I6中发生了很大的畸变，导致了明显的电荷定位。此外，阳离子构型紊乱抑制了缺陷的形成，从而降低了晶格微应变。这些修饰有效地延长了载流子寿命，减少了载流子散射，有利于电荷载流子的输运。结果表明，由（M2PDA）Pb2I6单晶组装的光电探测器实现了1.42 × 104的通断电流比和0.55 a W-1的响应率，是基于三维钙钛矿的器件中性能最高的器件之一。此外，（M2PDA）Pb2I6单晶在100%异丙醇中表现出优异的稳定性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.