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1.
Despite the exciting progress on power conversion efficiencies, the commercialization of the emerging lead (Pb) halide perovskite solar cell technology still faces significant challenges, one of which is the inclusion of toxic Pb. Searching for Pb‐free perovskite solar cell absorbers is currently an attractive research direction. The approaches used for and the consequences of Pb replacement are reviewed herein. Reviews on the theoretical understanding of the electronic, optical, and defect properties of Pb and Pb‐free halide perovskites and perovskite derivatives are provided, as well as the experimental results available in the literature. The theoretical understanding explains well why Pb halide perovskites exhibit superior photovoltaic properties, but Pb‐free perovskites and perovskite derivatives do not. 相似文献
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Yizhou Zhao Siyu Zhang Yue Lu Shangui Lan Cheng Zhu Jiawen Xiao Huachao Zai Manling Sui Dehui Li Huanping Zhou Yujing Li Qi Chen 《Small (Weinheim an der Bergstrasse, Germany)》2019,15(6)
The low‐dimensional halide perovskites have received enormous attention due to their unique photovoltaic and optoelectronic performances. Periodic spacers are used to inhibit the growth of 3D perovskite and fabricate a 2D counterpart with layered structure, mostly based on organic/inorganic cations. Herein, by introducing organic anions (e.g., pentanedioic acid (PDA) and hexanedioic acid (HDA) simultaneously), leaf‐shaped (Cs3Pb2Br5)2(PDA–HDA) microplates with low‐dimensional structure are synthesized. They also exhibit significant photoluminescence (PL) centered at 540 nm with a narrow emission peak. The synthesis of single crystals of Pb(PDA) and Pb(HDA) allows to further clarify the crystal structure of (Cs3Pb2Br5)2(PDA–HDA) perovskite and its structural evolution mechanism. Moreover, the cooperative introduction of dicarboxylic acid pairs with appropriate lengths is thermodynamically favored for the low‐dimensional perovskite crystallization. The temperature‐dependent PL indicates a V‐shaped Stokes shift with elevated temperature that could be associated with the localization of excitons in the inorganic layers between organic dicarboxylic acid molecules. This work demonstrates low‐dimensional halide perovskite with anionic spacers, which also opens up a new approach to the growth of low‐dimensional organic–inorganic hybrid perovskite crystals. 相似文献
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Jiancan Yu Jintao Kong Wei Hao Xintong Guo Huajun He Wan Ru Leow Zhiyuan Liu Pingqiang Cai Guodong Qian Shuzhou Li Xueyuan Chen Xiaodong Chen 《Advanced materials (Deerfield Beach, Fla.)》2019,31(7)
As emerging efficient emitters, metal‐halide perovskites offer the intriguing potential to the low‐cost light emitting devices. However, semiconductors generally suffer from severe luminescence quenching due to insufficient confinement of excitons (bound electron–hole pairs). Here, Sn‐triggered extrinsic self‐trapping of excitons in bulk 2D perovskite crystal, PEA2PbI4 (PEA = phenylethylammonium), is reported, where exciton self‐trapping never occurs in its pure state. By creating local potential wells, isoelectronic Sn dopants initiate the localization of excitons, which would further induce the large lattice deformation around the impurities to accommodate the self‐trapped excitons. With such self‐trapped states, the Sn‐doped perovskites generate broadband red‐to‐near‐infrared (NIR) emission at room temperature due to strong exciton–phonon coupling, with a remarkable quantum yield increase from 0.7% to 6.0% (8.6 folds), reaching 42.3% under a 100 mW cm?2 excitation by extrapolation. The quantum yield enhancement stems from substantial higher thermal quench activation energy of self‐trapped excitons than that of free excitons (120 vs 35 meV). It is further revealed that the fast exciton diffusion involves in the initial energy transfer step by transient absorption spectroscopy. This dopant‐induced extrinsic exciton self‐trapping approach paves the way for extending the spectral range of perovskite emitters, and may find emerging application in efficient supercontinuum sources. 相似文献
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Guozhan Xia Boyuan Huang Ying Zhang Xingyu Zhao Chen Wang Chunmei Jia Jinjin Zhao Weiqiu Chen Jiangyu Li 《Advanced materials (Deerfield Beach, Fla.)》2019,31(36)
Triple‐cation mixed‐halide perovskites of composition Csx(FAyMA1?y)1?xPb(IzBr1?z)3 (CsFAMA) have been reported to possess excellent photovoltaic efficiency with minimal hysteresis; in this work, nanoscale insight is shed into the roles of illumination‐induced polarization and ionic migration in photovoltaic hysteresis. By examining the concurrent evolution of ionic distribution and spontaneous polarization of CsFAMA under light illumination using dynamic‐strain‐based scanning probe microscopy, strong linear piezoelectricity arising from photoenhanced polarization is observed, while ionic migration is found to be not significantly increased by lightening. Nanoscale photocurrents are mapped under a series of biases using conductive atomic force microscopy, revealing negligible difference between forward and backward scans, and local IV curves reconstructed from principal component analysis show minimal hysteresis of just 1%. These observations at the nanoscale are confirmed in a macroscopic perovskite solar cell made of CsFAMA, exhibiting a high efficiency of 20.11% and with hysteresis index as small as 3%. Ionic migration, polarization, and photocurrent hysteresis are thus directly correlated at the nanoscale, and photoenhanced polarization in triple‐cation mixed‐halide perovskites is established, which does not contribute to the photovoltaic hysteresis. 相似文献
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Silvia G. Motti Daniele Meggiolaro Samuele Martani Roberto Sorrentino Alex J. Barker Filippo De Angelis Annamaria Petrozza 《Advanced materials (Deerfield Beach, Fla.)》2019,31(47)
The presence of various types of chemical interactions in metal‐halide perovskite semiconductors gives them a characteristic “soft” fluctuating structure, prone to a wide set of defects. Understanding of the nature of defects and their photochemistry is summarized, which leverages the cooperative action of density functional theory investigations and accurate experimental design. This knowledge is used to describe how defect activity determines the macroscopic properties of the material and related devices. Finally, a discussion of the open questions provides a path towards achieving an educated prediction of device operation, necessary to engineer reliable devices. 相似文献
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Metal‐Halide Perovskites for Gate Dielectrics in Field‐Effect Transistors and Photodetectors Enabled by PMMA Lift‐Off Process
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Alwin Daus Cristina Roldán‐Carmona Konrad Domanski Stefan Knobelspies Giuseppe Cantarella Christian Vogt Michael Grätzel Mohammad Khaja Nazeeruddin Gerhard Tröster 《Advanced materials (Deerfield Beach, Fla.)》2018,30(23)
Metal‐halide perovskites have emerged as promising materials for optoelectronics applications, such as photovoltaics, light‐emitting diodes, and photodetectors due to their excellent photoconversion efficiencies. However, their instability in aqueous solutions and most organic solvents has complicated their micropatterning procedures, which are needed for dense device integration, for example, in displays or cameras. In this work, a lift‐off process based on poly(methyl methacrylate) and deep ultraviolet lithography on flexible plastic foils is presented. This technique comprises simultaneous patterning of the metal‐halide perovskite with a top electrode, which results in microscale vertical device architectures with high spatial resolution and alignment properties. Hence, thin‐film transistors (TFTs) with methyl‐ammonium lead iodide (MAPbI3) gate dielectrics are demonstrated for the first time. The giant dielectric constant of MAPbI3 (>1000) leads to excellent low‐voltage TFT switching capabilities with subthreshold swings ≈80 mV decade?1 over ≈5 orders of drain current magnitude. Furthermore, vertically stacked low‐power Au‐MAPbI3‐Au photodetectors with close‐to‐ideal linear response (R2 = 0.9997) are created. The mechanical stability down to a tensile radius of 6 mm is demonstrated for the TFTs and photodetectors, simultaneously realized on the same flexible plastic substrate. These results open the way for flexible low‐power integrated (opto‐)electronic systems based on metal‐halide perovskites. 相似文献
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Seungjin Lee Da Bin Kim Jae Choul Yu Chung Hyeon Jang Jong Hyun Park Bo Ram Lee Myoung Hoon Song 《Advanced materials (Deerfield Beach, Fla.)》2019,31(20)
Metal halide perovskites (MHPs) have emerged as promising emitters because of their excellent optoelectronic properties, including high photoluminescence quantum yields (PLQYs), wide‐range color tunability, and high color purity. However, a fundamental limitation of MHPs is their low exciton binding energy, which results in a low radiative recombination rate and the dependence of PLQY on the excitation intensity. Under the operating conditions of light‐emitting diodes (LEDs), the injected current densities are typically lower than the trap density, leading to a low actual PLQY. Moreover, the defects not only initiate the decomposition of MHPs caused by extrinsic factors, but also intrinsically stimulate ion migration across the interface and lead to the corrosion of electrodes due to interaction between those electrodes, even under inert conditions. The passivation of defects has proven to be effective for mitigating the effects of defects in MHPs. Herein, the origins and theoretical calculations of the defect tolerance in MHPs and the impact of defects on both the performance and stability of perovskite LEDs are reviewed. The passivation methods and materials for MHP bulk films and nanocrystals are discussed in detail. Based on the currently reported advances, specific requirements and future research directions for display applications are suggested. 相似文献
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Photonic Nanostructures Patterned by Thermal Nanoimprint Directly into Organo‐Metal Halide Perovskites
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Neda Pourdavoud Si Wang André Mayer Ting Hu Yiwang Chen André Marianovich Wolfgang Kowalsky Ralf Heiderhoff Hella‐Christin Scheer Thomas Riedl 《Advanced materials (Deerfield Beach, Fla.)》2017,29(12)
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Ying‐Chieh Wong Wen‐Bin Wu Tian Wang Jun De Andrew Ng Khoong Hong Khoo Jie Wu Zhi‐Kuang Tan 《Advanced materials (Deerfield Beach, Fla.)》2019,31(24)
Lead halide perovskite possesses a semiconductor bandgap that is readily tunable by a variation in its halide composition. Here, a photo‐activated halide exchange process between perovskite nanocrystals and molecular haloalkanes is reported, which enables the perovskite luminescence to be controllably shifted across the entire visible spectrum. Mechanistic investigations reveal a mutual exchange of halogens between the perovskite crystal surface and a chemisorbed haloalkane, yielding nanocrystals and haloalkanes with mixed halide contents. Exchange kinetics studies involving primary, secondary, and tertiary haloalkanes show that the rate of reaction is governed by the activation barrier in the breakage of the covalent carbon–halogen (C? X) bond, which is a function of the C? X bond energy and carbon radical stability. Employing this halide exchange approach, a micrometer‐scale trichromatic patterning of perovskites is demonstrated using a light‐source‐integrated inkjet printer and tertiary haloalkanes as color‐conversion inks. The haloalkanes volatilize after halide exchange and leave no residues, thereby offering significant processing advantage over conventional salt‐based exchange techniques. Beyond the possible applications in new‐generation micro‐LED and electroluminescent quantum dot displays, this work exemplifies the rich surface and photochemistry of perovskite nanocrystals, and could lead to further opportunities in perovskite‐based photocatalysis and photochemical sensing. 相似文献
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Organolead Halid Perovskites: Organolead Halide Perovskites for Low Operating Voltage Multilevel Resistive Switching (Adv. Mater. 31/2016)
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Jaeho Choi Sunghak Park Joohee Lee Kootak Hong Do‐Hong Kim Cheon Woo Moon Gyeong Do Park Junmin Suh Jinyeon Hwang Soo Young Kim Hyun Suk Jung Nam‐Gyu Park Seungwu Han Ki Tae Nam Ho Won Jang 《Advanced materials (Deerfield Beach, Fla.)》2016,28(31):6517-6517
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Sheng Huang Peng Huang Lei Wang Junbo Han Yu Chen Haizheng Zhong 《Advanced materials (Deerfield Beach, Fla.)》2019,31(42)
3D perovskites with typical structure of ABX3 are emerging as key materials to achieve high‐performance optoelectronic devices. The variation of A‐site cation is promising to achieve enhanced properties; however, is limited to a few available choices of methylamine, formamidine, and cesium. In this work, halogenated‐methylammoniums are developed as A cation to broaden the family of hybrid perovskites. Single crystals and colloidal nanocrystals of halogenated‐methylammoniums based perovskites are successfully synthesized, showing bright future as alternatives for device exploration. In particular, the improved thermal stability and low exciton binding energy from single crystals measurements are demonstrated and bright tunable emission from blue to green for colloidal nanocrystals is achieved. 相似文献
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Mahshid Ahmadi Liam Collins Alexander Puretzky Jia Zhang Jong Kahk Keum Wei Lu Ilia Ivanov Sergei V. Kalinin Bin Hu 《Advanced materials (Deerfield Beach, Fla.)》2018,30(11)
Organometallic halide perovskites (OMHPs) have attracted broad attention as prospective materials for optoelectronic applications. Among the many anomalous properties of these materials, of special interest are the ferroelectric properties including both classical and relaxor‐like components, as a potential origin of slow dynamics, field enhancement, and anomalous mobilities. Here, ferroelectric properties of the three representative OMHPs are explored, including FAPbxSn1–xI3 (x = 0, x = 0.85) and FA0.85MA0.15PbI3 using band excitation piezoresponse force microscopy and contact mode Kelvin probe force microscopy, providing insight into long‐ and short‐range dipole and charge dynamics in these materials and probing ferroelectric density of states. Furthermore, second‐harmonic generation in thin films of OMHPs is observed, providing a direct information on the noncentrosymmetric polarization in such materials. Overall, the data provide strong evidence for the presence of ferroelectric domains in these systems; however, the domain dynamics is suppressed by fast ion dynamics. These materials hence present the limit of ferroelectric materials with spontaneous polarization dynamically screened by ionic and electronic carriers. 相似文献
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Alexey Y. Zhizhchenko Pavel Tonkaev Dmitry Gets Artem Larin Dmitry Zuev Sergey Starikov Eugeny V. Pustovalov Alexander M. Zakharenko Sergei A. Kulinich Saulius Juodkazis Aleksandr A. Kuchmizhak Sergey V. Makarov 《Small (Weinheim an der Bergstrasse, Germany)》2020,16(19)
Nanophotonics based on resonant nanostructures and metasurfaces made of halide perovskites have become a prospective direction for efficient light manipulation at the subwavelength scale in advanced photonic designs. One of the main challenges in this field is the lack of large‐scale low‐cost technique for subwavelength perovskite structures fabrication preserving highly efficient luminescence. Here, unique properties of halide perovskites addressed to their extremely low thermal conductivity (lower than that of silica glass) and high defect tolerance to apply projection femtosecond laser lithography for nanofabrication with precise spatial control in all three dimensions preserving the material luminescence efficiency are employed. Namely, with CH3NH3PbI3 perovskite highly ordered nanoholes and nanostripes of width as small as 250 nm, metasurfaces with periods less than 400 nm, and nanowire lasers as thin as 500 nm, corresponding to the state‐of‐the‐art in multistage expensive lithographical methods are created. Remarkable performance of the developed approach allows to demonstrate a number of advanced optical applications, including morphology‐controlled photoluminescence yield, structural coloring, optical‐ information encryption, and lasing. 相似文献
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Polymer‐Passivated Inorganic Cesium Lead Mixed‐Halide Perovskites for Stable and Efficient Solar Cells with High Open‐Circuit Voltage over 1.3 V
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Qingsen Zeng Xiaoyu Zhang Xiaolei Feng Siyu Lu Zhaolai Chen Xue Yong Simon A. T. Redfern Haotong Wei Haiyu Wang Huaizhong Shen Wei Zhang Weitao Zheng Hao Zhang John S. Tse Bai Yang 《Advanced materials (Deerfield Beach, Fla.)》2018,30(9)
Cesium‐based trihalide perovskites have been demonstrated as promising light absorbers for photovoltaic applications due to their superb composition stability. However, the large energy losses (Eloss) observed in inorganic perovskite solar cells has become a major hindrance impairing the ultimate efficiency. Here, an effective and reproducible method of modifying the interface between a CsPbI2Br absorber and polythiophene hole‐acceptor to minimize the Eloss is reported. It is demonstrated that polythiophene, deposited on the top of CsPbI2Br, can significantly reduce electron‐hole recombination within the perovskite, which is due to the electronic passivation of surface defect states. In addition, the interfacial properties are improved by a simple annealing process, leading to significantly reduced energy disorder in polythiophene and enhanced hole‐injection into the hole‐acceptor. Consequently, one of the highest power conversion efficiency (PCE) of 12.02% from a reverse scan in inorganic mixed‐halide perovskite solar cells is obtained. Modifying the perovskite films with annealing polythiophene enables an open‐circuit voltage (VOC) of up to 1.32 V and Eloss of down to 0.5 eV, which both are the optimal values reported among cesium‐lead mixed‐halide perovskite solar cells to date. This method provides a new route to further improve the efficiency of perovskite solar cells by minimizing the Eloss. 相似文献
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Zhizhong Chen Yuwei Guo Esther Wertz Jian Shi 《Advanced materials (Deerfield Beach, Fla.)》2019,31(1)
Following the rejuvenation of 3D organic–inorganic hybrid perovskites, like CH3NH3PbI3, (quasi)‐2D Ruddlesden–Popper soft halide perovskites R2An?1PbnX3n+1 have recently become another focus in the optoelectronic and photovoltaic device community. Although quasi‐2D perovskites were first introduced to stabilize optoelectronic/photovoltaic devices against moisture, more interesting properties and device applications, such as solar cells, light‐emitting diodes, white‐light emitters, lasers, and polaritonic emission, have followed. While delicate engineering design has pushed the performance of various devices forward remarkably, understanding of the fundamental properties, especially the charge‐transfer process, electron–phonon interactions, and the growth mechanism in (quasi)‐2D halide perovskites, remains limited and even controversial. Here, after reviewing the current understanding and the nexus between optoelectronic/photovoltaic properties of 2D and 3D halide perovskites, the growth mechanisms, charge‐transfer processes, vibrational properties, and electron–phonon interactions of soft halide perovskites, mainly in quasi‐2D systems, are discussed. It is suggested that single‐crystal‐based studies are needed to deepen the understanding of the aforementioned fundamental properties, and will eventually contribute to device performance. 相似文献
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Yuan Gao Grant Walters Ying Qin Bin Chen Yimeng Min Ali Seifitokaldani Bin Sun Petar Todorovic Makhsud I. Saidaminov Alan Lough Sefaattin Tongay Sjoerd Hoogland Edward H. Sargent 《Advanced materials (Deerfield Beach, Fla.)》2019,31(16)
Rapid and efficient conversion of electrical signals to optical signals is needed in telecommunications and data network interconnection. The linear electro‐optic (EO) effect in noncentrosymmetric materials offers a pathway to such conversion. Conventional inorganic EO materials make on‐chip integration challenging, while organic nonlinear molecules suffer from thermodynamic molecular disordering that decreases the EO coefficient of the material. It has been posited that hybrid metal halide perovskites could potentially combine the advantages of inorganic materials (stable crystal orientation) with those of organic materials (solution processing). Here, layered metal halide perovskites are reported and investigated for in‐plane birefringence and linear electro‐optic response. Phenylmethylammonium lead chloride (PMA2PbCl4) crystals are grown that exhibit a noncentrosymmetric space group. Birefringence measurements and Raman spectroscopy confirm optical and structural anisotropy in the material. By applying an electric field on the crystal surface, the linear EO effect in PMA2PbCl4 is reported and its EO coefficient is determined to be 1.40 pm V?1. This is the first demonstration of this effect in hybrid metal halide perovskites, materials that feature both highly ordered crystalline structures and solution processability. The in‐plane birefringence and electro‐optic response reveal that layered perovskite crystals could be further explored for potential applications in polarizing optics and EO modulation. 相似文献