Regulating off-centering distortion maximizes photoluminescence in halide perovskites.
Xujie Lü,Constantinos C. Stoumpos,Qingyang Hu,Xuedan Ma,Dongzhou Zhang,Songhao Guo,Justin M. Hoffman,Kejun Bu,Xiaofeng Guo,Yingqi Wang,Cheng Ji,Haijie Chen,Hongwu Xu,Quanxi Jia,Wenge Yang,Mercouri G. Kanatzidis,Ho-kwang Mao +16 more
TLDR
This work demonstrates a quantitative relationship between structural distortion and PL property of the halide perovskites but also illustrates the use of knowledge gained from high-pressure research to achieve the desired properties by ambient methods.Abstract:
Metal halide perovskites possess unique atomic and electronic configurations that endow them with high defect tolerance and enable high-performance photovoltaics and optoelectronics. Perovskite light-emitting diodes have achieved an external quantum efficiency of over 20%. Despite tremendous progress, fundamental questions remain, such as how structural distortion affects the optical properties. Addressing their relationships is considerably challenging due to the scarcity of effective diagnostic tools during structural and property tuning as well as the limited tunability achievable by conventional methods. Here, using pressure and chemical methods to regulate the metal off-centering distortion, we demonstrate the giant tunability of photoluminescence (PL) in both the intensity (>20 times) and wavelength (>180 nm/GPa) in the highly distorted halide perovskites [CH3NH3GeI3, HC(NH2)2GeI3, and CsGeI3]. Using advanced in situ high-pressure probes and first-principles calculations, we quantitatively reveal a universal relationship whereby regulating the level of off-centering distortion towards 0.2 leads to the best PL performance in the halide perovskites. By applying this principle, intense PL can still be induced by substituting CH3NH3+ with Cs+ to control the distortion in (CH3NH3)1-xCsxGeI3, where the chemical substitution plays a similar role as external pressure. The compression of a fully substituted sample of CsGeI3 further tunes the distortion to the optimal value at 0.7 GPa, which maximizes the emission with a 10-fold enhancement. This work not only demonstrates a quantitative relationship between structural distortion and PL property of the halide perovskites but also illustrates the use of knowledge gained from high-pressure research to achieve the desired properties by ambient methods.read more
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Screening in crystalline liquids protects energetic carriers in hybrid perovskites
Haiming Zhu,Kiyoshi Miyata,Yongping Fu,Jue Wang,Prakriti P. Joshi,Daniel Niesner,Kristopher W. Williams,Song Jin,Xiaoyang Zhu +8 more
TL;DR: The hot fluorescence is correlated with liquid-like molecular reorientational motions, suggesting that dynamic screening protects energetic carriers via solvation or large polaron formation on time scales competitive with that of ultrafast cooling.
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Local polar fluctuations in lead halide perovskite crystals
Yinsheng Guo,Omer Yaffe,Liang Tan,David Egger,Trevor D. Hull,Constantinos C. Stoumpos,Fan Zheng,Tony F. Heinz,Leeor Kronik,Mercouri G. Kanatzidis,Jonathan S. Owen,Andrew M. Rappe,Marcos A. Pimenta,Louis E. Brus +13 more
TL;DR: Observations of a strong central peak in the cubic phase of both hybrid and all-inorganic lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead- Halide Perovskite structure, and not unique to the dipolar organic cation.
Journal ArticleDOI
Enhanced Photocurrent of All-Inorganic Two-Dimensional Perovskite Cs2PbI2Cl2 via Pressure-Regulated Excitonic Features.
Songhao Guo,Kejun Bu,Jiangwei Li,Qingyang Hu,Hui Luo,Yihui He,Yanhui Wu,Dongzhou Zhang,Yongsheng Zhao,Wenge Yang,Mercouri G. Kanatzidis,Xujie Lü +11 more
TL;DR: In this article, the 2D perovskite Cs2PbI2Cl2 was shown to achieve a 3 orders of magnitude increase in photoresponse under pressure tuning.
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Enhanced Photoluminescence and Photoresponsiveness of Eu3+ Ions-Doped CsPbCl3 Perovskite Quantum Dots under High Pressure
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Regulating Exciton-Phonon Coupling to Achieve a Near-Unity Photoluminescence Quantum Yield in One-Dimensional Hybrid Metal Halides.
Hui Luo,Songhao Guo,Yubo Zhang,Kejun Bu,Haoran Lin,Yingqi Wang,Yanfeng Yin,Dongzhou Zhang,Shengye Jin,Wenqing Zhang,Wenge Yang,Biwu Ma,Xujie Lü +12 more
TL;DR: In this paper, a near 100% photoluminescence quantum yield (PLQY) of broadband emission was achieved in a corrugated 1D hybrid metal halide C5 N2 H16 Pb2 Br6, which possesses a highly distorted structure with an initial PLQY of 10%.
References
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Journal ArticleDOI
Semiconducting tin and lead iodide perovskites with organic cations: phase transitions, high mobilities, and near-infrared photoluminescent properties.
TL;DR: It is found that the chemical and physical properties of these materials strongly depend on the preparation method, and the properties of the title hybrid materials with those of the "all-inorganic" CsSnI3 and CsPbI3 prepared using identical synthetic methods.
Journal ArticleDOI
Organic–Inorganic Perovskites: Structural Versatility for Functional Materials Design
TL;DR: This review will explore beyond the current focus on three-dimensional (3-D) lead(II) halide perovskites, to highlight the great chemical flexibility and outstanding potential of the broader class of 3-D and lower dimensional organic-based perovSKite family for electronic, optical, and energy-based applications as well as fundamental research.
Journal ArticleDOI
Unique Properties of Halide Perovskites as Possible Origins of the Superior Solar Cell Performance
TL;DR: Halide perovskites solar cells have the potential to exhibit higher energy conversion efficiencies with ultrathin films than conventional thin-film solar cells based on CdTe, CuInSe2 , and Cu2 ZnSnSe4.
Journal ArticleDOI
Properties and potential optoelectronic applications of lead halide perovskite nanocrystals
Maksym V. Kovalenko,Maksym V. Kovalenko,Loredana Protesescu,Loredana Protesescu,Maryna I. Bodnarchuk +4 more
TL;DR: The prospects of LHP NCs for optoelectronic applications such as in television displays, light-emitting devices, and solar cells are surveyed, emphasizing the practical hurdles that remain to be overcome.
Journal ArticleDOI
Perovskite light-emitting diodes based on spontaneously formed submicrometre-scale structures
Yu Cao,Nana Wang,He Tian,Jingshu Guo,Yingqiang Wei,Hong Chen,Yanfeng Miao,Wei Zou,Kang Pan,Yarong He,Hui Cao,You Ke,Mengmeng Xu,Ying Wang,Ming Yang,Kai Du,Zewu Fu,Decheng Kong,Daoxin Dai,Yizheng Jin,Gongqiang Li,Hai Li,Qiming Peng,Jianpu Wang,Wei Huang,Wei Huang,Wei Huang +26 more
TL;DR: The formation of submicrometre-scale structure in perovskite light-emitting diodes can raise their external quantum efficiency beyond 20%, suggesting the possibility of both high efficiency and high brightness.