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Engineering the Exciton Dissociation in Quantum-Confined 2D CsPbBr_3 Nanosheet Films

机译:工程量子受限的二维CsPbBr_3纳米片薄膜中的激子离解。

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摘要

Recent years have witnessed a rapid development of all-inorganic halide perovskite in optoelectronic devices. Ultrathin 2D CsPbBr3 nanosheets (NSs) with large lateral dimensions have demonstrated exceptional photophysical properties because of their analogous exciton electronic structure to quantum wells. Despite the incredible progress on device performance, the photophysics and carrier transportation parameters of quantum-confined CsPbBr3 NSs are lacking, and the fundamental understanding of the exciton dissociation mechanism is far less developed. Here, a ligands rearrangement mechanism is proposed to explain why annealed NS films have an increased charge transfer rate and a decreased exciton binding energy and lifetime, prompting tunneling as a dominant way of exciton dissociation to separate photogenerated excitons between neighboring NSs. This facile but efficient method provides a new insight to manipulate perovskite nanocrystals coupling. Moreover, ultrathin 2D CsPbBr3 NS film is demonstrated to have a enhanced absorption cross section and high carrier mobility of 77.9 cm(2) V-1 s(-1), contributing to its high responsivity of 0.53 A W-1. The photodetector has a long-term stability up to three months, which are responsible for reliable perovskite-based device performance.
机译:近年来,光电器件中的全无机卤化物钙钛矿发展迅速。具有大横向尺寸的超薄二维CsPbBr3纳米片(NSs)由于其与量子阱的激子电子结构相似,因此具有出色的光物理特性。尽管在器件性能上取得了令人难以置信的进步,但仍缺乏量子限制的CsPbBr3 NS的光物理和载流子输运参数,并且对激子离解机理的基本了解还远远不够。在这里,提出了配体重排机制来解释为什么退火的NS膜具有增加的电荷转移速率和降低的激子结合能和寿命,从而促使隧穿成为激子解离的主要方式,以分离相邻NS之间的光生激子。这种简便而有效的方法为操纵钙钛矿纳米晶体的耦合提供了新的见识。此外,超薄的2D CsPbBr3 NS薄膜被证明具有增强的吸收截面和77.9 cm(2)V-1 s(-1)的高载流子迁移率,有助于其0.53 A W-1的高响应度。光电探测器具有长达三个月的长期稳定性,可确保基于钙钛矿的可靠设备性能。

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  • 来源
    《Advanced Functional Materials》 |2018年第14期|1705908.1-1705908.10|共10页
  • 作者单位

    Xi An Jiao Tong Univ, Key Lab Educ Minist, EMRL, ICDR,Shaanxi Engn Res Ctr Adv Energy Mat & Device, Xian 710049, Shaanxi, Peoples R China;

    Xi An Jiao Tong Univ, Key Lab Educ Minist, EMRL, ICDR,Shaanxi Engn Res Ctr Adv Energy Mat & Device, Xian 710049, Shaanxi, Peoples R China;

    Xi An Jiao Tong Univ, Key Lab Educ Minist, EMRL, ICDR,Shaanxi Engn Res Ctr Adv Energy Mat & Device, Xian 710049, Shaanxi, Peoples R China;

    Xi An Jiao Tong Univ, Key Lab Educ Minist, EMRL, ICDR,Shaanxi Engn Res Ctr Adv Energy Mat & Device, Xian 710049, Shaanxi, Peoples R China;

    Univ Hong Kong, Dept Phys, Pokfulam Rd, Hong Kong, Hong Kong, Peoples R China;

    Shandong Business & Technol Univ, Key Lab Intelligent Informat Proc Univ Shandong, Yantai 264005, Peoples R China;

    Univ Connecticut, Dept Chem & Biomol Engn, Storrs, CT 06269 USA;

    Xi An Jiao Tong Univ, State Key Lab Mfg Syst Engn, Xian 710049, Shaanxi, Peoples R China;

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  • 正文语种 eng
  • 中图分类
  • 关键词

    all-inorganic halide perovskites; binding energy; charge transfer rates; exciton dissociation; nanosheets;

    机译:全无机卤化物钙钛矿;结合能;电荷转移速率;激子离解;纳米片;

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