Charge Carrier Dynamics at the Interface of 2D Metal–Organic Frameworks and Hybrid Perovskites for Solar Energy Harvesting,Nano Letters

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Charge Carrier Dynamics at the Interface of 2D Metal–Organic Frameworks and Hybrid Perovskites for Solar Energy Harvesting
Nano Letters ( IF 9.6 ) Pub Date : 2023-12-15 , DOI: 10.1021/acs.nanolett.3c04054
Robert Stanton ₁ , Dhara J Trivedi ₁

Affiliation

Interfacing perovskites with two-dimensional materials such as metal–organic frameworks (MOFs) for improved stability and electron or hole extraction has emerged as a promising path forward for the generation of highly efficient and stable solar cells. In this work, we examine the structural properties and excitation dynamics of two MOF–perovskite systems: UMCM309-a@MAPbI₃ and ZrL3@MAPbI₃. We find that precise band alignment and electronegativity of the MOF-linkers are necessary to facilitate the capture of excited charge carriers. Furthermore, we demonstrate that intraband relaxation of hot electrons to the MOF subsystem results in optically disallowed transitions across the band gap, suppressing radiative recombination. Furthermore, we elucidate the key mechanisms associated with improved structural stability afforded to the perovskites by the two-dimensional MOFs, highlighting the necessity of broad surface coverage and strong MOF–perovskite interaction.

中文翻译：

用于太阳能收集的二维金属有机框架和混合钙钛矿界面的电荷载流子动力学

将钙钛矿与二维材料（例如金属有机框架（MOF））连接以提高稳定性和电子或空穴提取已成为生产高效和稳定太阳能电池的一条有前途的道路。在这项工作中，我们研究了两种 MOF-钙钛矿系统的结构特性和激发动力学：UMCM309-a@MAPbI ₃和 ZrL3@MAPbI ₃ 。我们发现 MOF 连接体的精确能带排列和电负性对于促进激发电荷载流子的捕获是必要的。此外，我们证明热电子到 MOF 子系统的带内弛豫会导致光学上不允许的跨越带隙的跃迁，从而抑制辐射复合。此外，我们阐明了二维 MOF 提高钙钛矿结构稳定性的关键机制，强调了广泛的表面覆盖和强 MOF-钙钛矿相互作用的必要性。

更新日期：2023-12-15

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