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Ultrafast Broadband Charge Collection from Clean Graphene/CH3NH3PbI3 Interface Hao Hong, Jincan Zhang, Jin Zhang, Ruixi Qiao, Fengrui Yao, Yang Cheng, Chunchun Wu, Li Lin, Kaicheng Jia, Yicheng Zhao, Qing Zhao, Peng Gao, Jie Xiong, Kebin Shi, Dapeng Yu, Zhongfan Liu, Sheng Meng, Hailin Peng, and Kaihui Liu J. Am. Chem. Soc., Just Accepted Manuscript • DOI: 10.1021/jacs.8b09353 • Publication Date (Web): 15 Oct 2018 Downloaded from http://pubs.acs.org on October 15, 2018
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Journal of the American Chemical Society
Ultrafast Broadband Charge Collection from Clean Graphene/CH3NH3PbI3 Interface Hao Hong1#, Jincan Zhang2#, Jin Zhang3#, Ruixi Qiao1, Fengrui Yao1, Yang Cheng1, Chunchun Wu4, Li Lin2, Kaicheng Jia2, Yicheng Zhao1, Qing Zhao1, Peng Gao5, Jie Xiong4, Kebin Shi1, Dapeng Yu6,7, Zhongfan Liu2, Sheng Meng3*, Hailin Peng2*, Kaihui Liu1* 1
State Key Laboratory for Mesoscopic Physics, Collaborative Innovation Centre of Quantum Matter, School of Physics, Peking University, Beijing 100871, China
2
Center for Nanochemistry, College of Chemistry and Molecular Engineering, Academy for Advanced Interdisciplinary Studies, Peking University, Beijing 100871, China
3
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
4 State
Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic
Science and Technology of China, Chengdu 610054, China 5
International Centre for Quantum Materials, Peking University, Beijing 100871, China
6
Institute for Quantum Science and Engineering and Department of Physics, South University of Science and Technology of China, Shenzhen 518055, China
7
Shenzhen Key Laboratory of Quantum Science and Engineering, Shenzhen 518055, China
# These authors contributed equally to this work * Correspondence:
[email protected];
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[email protected] ACS Paragon1Plus / 21Environment
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Abstract Photocarrier generation in a material, transportation to the material surface, and collection at the electrode interface are of paramount importance in any optoelectronic and photovoltaic device. In the last collection process, ideal performance comprises ultrafast charge collection to enhance current conversion efficiency and broadband collection to enhance energy conversion efficiency. Here, for the first time, we demonstrate ultrafast broadband charge collection achieved simultaneously at the clean graphene/organicinorganic halide perovskite interface. The clean interface is realized by directly growing perovskite on graphene surface without polymer contamination. The tunable two-color pump-probe spectroscopy, time-resolved photoluminescence spectroscopy and timedependent density functional theory all reveal that the clean-interfacial graphene collects band-edge photocarriers of perovskite in an ultrashort time of ~100 fs, with a current collection efficiency close to 99%. In addition, graphene can extract deep-band hot carriers of perovskite within only ~50 fs, several orders faster than hot carrier relaxation and cooling in perovskite itself, due to the unique Dirac linear band structure of graphene, indicating a potential high energy conversion efficiency exceeding Shockley−Queisser limit. Adding other graphene superiority of good transparency, high carrier mobility and extreme flexibility, clean-interfacial graphene provides an ideal charge collection layer and electrode candidate for future optoelectronic and photovoltaic applications in two dimensions.
ACS Paragon2Plus / 21Environment
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Journal of the American Chemical Society
Introduction In all optoelectronic and photovoltaic devices, three essential processes are involved to accomplish photocurrent generation or photoenergy harvesting: light absorption in a material to generate photocarriers, photocarrier transportation to the material surface, and charge collection to the electrode. The engineering and optimization of these three processes lie at the center of improving the photoelectric device performance. The emergent absorber materials of organicinorganic halide perovskites (e.g. CH3NH3PbI3) shed bright light on optimizing the first two key photoelectric processes, as this family of materials have a tunable bandgap from visible to near infrared with high absorption coefficient (over 104 cm-1 above bandgap) to ensure high photocarrier generation efficiency1, strong dielectric screening with negligible exciton binding energy (
