Abnormal spatial heterogeneity governing the charge-carrier mechanism in efficient Ruddlesden–Popper perovskite solar cells,Energy & Environmental Science

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Abnormal spatial heterogeneity governing the charge-carrier mechanism in efficient Ruddlesden–Popper perovskite solar cells
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2021-07-26 , DOI: 10.1039/d1ee00984b
Jun Xi _{1,

2} , Junseop Byeon _{1,

3} , Unsoo Kim _{1,

3} , Kijoon Bang _{1,

3} , Gi Rim Han ₄ , Ji-Young Kim ₅ , Jungjin Yoon ₆ , Hua Dong ₇ , Zhaoxin Wu ₇ , Giorgio Divitini ₈ , Kai Xi ₈ , Jinwoo Park ₉ , Tae-Woo Lee _{9,

10} , Seong Keun Kim ₄ , Mansoo Choi _{1,

3} , Jong Woo Lee ₁₁

Affiliation

Global Frontier Center for Multiscale Energy Systems, Seoul National University, Seoul 08826, Republic of Korea
Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands
Department of Mechanical and Aerospace Engineering, Seoul National University, Seoul 08826, Republic of Korea
Department of Chemistry, Seoul National University, Seoul 08826, Republic of Korea
Advanced Analysis Center, Korea Institute of Science and Technology (KIST), Hwarangno 14-gil 5, Seongbuk-gu, Seoul 02792, Republic of Korea
Materials Research Institute, Pennsylvania State University, University Park, PA 16802, USA
School of Electronic and Information Engineering, Xi’an Jiaotong University, No. 28, Xianning West Road, Xi’an, 710049, China
Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS, UK
Department of Materials Science and Engineering, Research Institute of Advanced Materials, and Institute of Engineering Research, Nano Systems Institute (NSI), Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea
School of Chemical and Biological Engineering, Seoul National University, Seoul 08826, Republic of Korea
Department of Chemistry, Myongji University, 116 Myongji Ro, Yongin, Gyeonggi-do, 17058, Republic of Korea

Layered Ruddlesden–Popper perovskite (RPP) photovoltaics have gained substantial attention owing to their excellent air stability. However, their photovoltaic performance is still limited by the unclear real-time charge-carrier mechanism of operating devices. Herein, we report the correlation between the charge-carrier mechanism and the spatially heterogeneous RPP bulks induced by distinct sublattice cations in the state-of-the-art antisolvent-driven RPP devices. In particular, abnormal heterogeneities ranging from the lateral long-range to local sub-grain scale and corresponding charge-carrier behaviours are visualized for triple-cation RPPs. We discovered that such heterogeneities with a unitary 2D/3D hybrid suppress lattice vibrations and reduce Fröhlich interactions by about 2 times, significantly promoting charge-carrier dynamics. Consequently, optimized triple-cation RPP solar cells greatly outperform their mono-cation counterparts. Furthermore, this principle can be applicable irrespective of 2D layer thickness (n > 2) and substrate type. This work provides a rationale for leveraging a disordered structure to stimulate charge-carrier motion and suggests the design principle of low-dimensional perovskites.

中文翻译：

控制高效 Ruddlesden-Popper 钙钛矿太阳能电池中电荷载流子机制的异常空间异质性

层状 Ruddlesden-Popper 钙钛矿（RPP）光伏由于其优异的空气稳定性而受到广泛关注。然而，它们的光伏性能仍然受到操作装置实时电荷载流子机制不明确的限制。在此，我们报告了在最先进的反溶剂驱动的 RPP 装置中电荷载流子机制与由不同亚晶格阳离子诱导的空间异质 RPP 体之间的相关性。特别是，从横向远程到局部亚晶粒尺度的异常异质性和相应的电荷载流子行为对于三阳离子 RPP 进行了可视化。我们发现这种具有单一 2D/3D 混合体的异质性抑制了晶格振动并将 Fröhlich 相互作用减少了约 2 倍，从而显着促进了电荷载流子动力学。因此，优化的三阳离子 RPP 太阳能电池大大优于其单阳离子对应物。此外，无论 2D 层厚度如何，该原理都适用（n > 2) 和基材类型。这项工作为利用无序结构刺激电荷载流子运动提供了基本原理，并提出了低维钙钛矿的设计原理。

更新日期：2021-08-02

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