TY - JOUR
T1 - Spontaneous Formation of 2D/3D Heterostructures on the Edges of 2D Ruddlesden-Popper Hybrid Perovskite Crystals
AU - Qin, Zhaojun
AU - Qin, Zhaojun
AU - Dai, Shenyu
AU - Dai, Shenyu
AU - Gajjela, Chalapathi Charan
AU - Wang, Chong
AU - Wang, Chong
AU - Hadjiev, Viktor G.
AU - Hadjiev, Viktor G.
AU - Yang, Guang
AU - Li, Jiabing
AU - Zhong, Xin
AU - Zhong, Xin
AU - Tang, Zhongjia
AU - Tang, Zhongjia
AU - Yao, Yan
AU - Guloy, Arnold M.
AU - Guloy, Arnold M.
AU - Reddy, Rohith
AU - Mayerich, David
AU - Deng, Liangzi
AU - Deng, Liangzi
AU - Yu, Qingkai
AU - Feng, Guoying
AU - Calderon, Hector A.
AU - Robles Hernandez, Francisco C.
AU - Wang, Zhiming M.
AU - Bao, Jiming
N1 - Publisher Copyright:
© 2020 American Chemical Society.
PY - 2020/6/23
Y1 - 2020/6/23
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85087404307&partnerID=8YFLogxK
U2 - 10.1021/acs.chemmater.0c00419
DO - 10.1021/acs.chemmater.0c00419
M3 - Artículo
SN - 0897-4756
VL - 32
SP - 5009
EP - 5015
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 12
ER -