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Spontaneous Formation of 2D/3D Heterostructures on the Edges of 2D Ruddlesden–Popper Hybrid Perovskite Crystals
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-05-21 , DOI: 10.1021/acs.chemmater.0c00419 Zhaojun Qin 1, 2 , Shenyu Dai 2, 3 , Chalapathi Charan Gajjela 2 , Chong Wang 2, 4 , Viktor G. Hadjiev 5, 6 , Guang Yang 7 , Jiabing Li 2 , Xin Zhong 5, 8 , Zhongjia Tang 5, 8 , Yan Yao 2 , Arnold M. Guloy 5, 8 , Rohith Reddy 2 , David Mayerich 2 , Liangzi Deng 5, 9 , Qingkai Yu 10 , Guoying Feng 3 , Hector A. Calderon 11 , Francisco C. Robles Hernandez 6 , Zhiming M. Wang 1 , Jiming Bao 2, 7
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-05-21 , DOI: 10.1021/acs.chemmater.0c00419 Zhaojun Qin 1, 2 , Shenyu Dai 2, 3 , Chalapathi Charan Gajjela 2 , Chong Wang 2, 4 , Viktor G. Hadjiev 5, 6 , Guang Yang 7 , Jiabing Li 2 , Xin Zhong 5, 8 , Zhongjia Tang 5, 8 , Yan Yao 2 , Arnold M. Guloy 5, 8 , Rohith Reddy 2 , David Mayerich 2 , Liangzi Deng 5, 9 , Qingkai Yu 10 , Guoying Feng 3 , Hector A. Calderon 11 , Francisco C. Robles Hernandez 6 , Zhiming M. Wang 1 , Jiming Bao 2, 7
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The observation of low-energy edge photoluminescence and its beneficial effect on the solar cell efficiency of Ruddlesden–Popper perovskites has unleashed an intensive research effort to reveal its origin. This effort, however, has been met with more challenges as the underlying material structure has still not been identified; new modelings and observations also do not seem to converge. Using two-dimensional (2D) (BA)2(MA)2Pb3Br10 as an example, we show that three-dimensional (3D) MAPbBr3 is formed due to the loss of BA on the edge. This self-formed MAPbBr3 can explain the reported edge emission under various conditions, while the reported intriguing optoelectronic properties such as fast exciton trapping from the interior 2D perovskite, rapid exciton dissociation, and long carrier lifetime can be understood via the self-formed 2D/3D lateral perovskite heterostructure. The 3D perovskite is identified by submicron infrared spectroscopy, the emergence of X-ray diffraction (XRD) signature from freezer-milled nanometer-sized 2D perovskite, and its photoluminescence response to external hydrostatic pressure. The revelation of this edge emission mystery and the identification of a self-formed 2D/3D heterostructure provide a new approach to engineering 2D perovskites for high-performance optoelectronic devices.
中文翻译：
2D Ruddlesden-Pop杂化钙钛矿晶体边缘上的2D / 3D异质结构的自发形成
低能边缘光致发光的观察及其对Ruddlesden-Popper钙钛矿的太阳能电池效率的有益影响，已经展开了深入的研究工作以揭示其起源。但是，由于尚未确定基本的材料结构，因此这项工作面临更多挑战。新的建模和观察似乎也无法融合。以二维（2D）（BA）2（MA）2 Pb 3 Br 10为例，我们表明由于边缘上BA的损失而形成了三维（3D）MAPbBr 3。这种自形成的MAPbBr 3通过自形成的2D / 3D横向钙钛矿异质结构，可以解释所报道的在各种条件下的边缘发射，而所报道的引人入胜的光电特性，例如从内部2D钙钛矿中快速捕获激子，快速激子解离和长载流子寿命。3D钙钛矿可通过亚微米红外光谱法，通过冷冻粉碎的纳米级2D钙钛矿的X射线衍射（XRD）签名以及其对外部静水压力的光致发光响应来识别。这一边缘发射之谜的启示以及对自形成的2D / 3D异质结构的鉴定为工程化高性能光电器件的2D钙钛矿提供了一种新方法。
更新日期：2020-06-23
中文翻译：
2D Ruddlesden-Pop杂化钙钛矿晶体边缘上的2D / 3D异质结构的自发形成
低能边缘光致发光的观察及其对Ruddlesden-Popper钙钛矿的太阳能电池效率的有益影响，已经展开了深入的研究工作以揭示其起源。但是，由于尚未确定基本的材料结构，因此这项工作面临更多挑战。新的建模和观察似乎也无法融合。以二维（2D）（BA）2（MA）2 Pb 3 Br 10为例，我们表明由于边缘上BA的损失而形成了三维（3D）MAPbBr 3。这种自形成的MAPbBr 3通过自形成的2D / 3D横向钙钛矿异质结构，可以解释所报道的在各种条件下的边缘发射，而所报道的引人入胜的光电特性，例如从内部2D钙钛矿中快速捕获激子，快速激子解离和长载流子寿命。3D钙钛矿可通过亚微米红外光谱法，通过冷冻粉碎的纳米级2D钙钛矿的X射线衍射（XRD）签名以及其对外部静水压力的光致发光响应来识别。这一边缘发射之谜的启示以及对自形成的2D / 3D异质结构的鉴定为工程化高性能光电器件的2D钙钛矿提供了一种新方法。
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