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Showing papers on "Perovskite (structure) published in 2017"


Journal ArticleDOI
30 Jun 2017-Science
TL;DR: The introduction of additional iodide ions into the organic cation solution, which is used to form the perovskite layers through an intramolecular exchanging process, decreases the concentration of deep-level defects, enabling the fabrication of PSCs with a certified power conversion efficiency.
Abstract: The formation of a dense and uniform thin layer on the substrates is crucial for the fabrication of high-performance perovskite solar cells (PSCs) containing formamidinium with multiple cations and mixed halide anions. The concentration of defect states, which reduce a cell’s performance by decreasing the open-circuit voltage and short-circuit current density, needs to be as low as possible. We show that the introduction of additional iodide ions into the organic cation solution, which are used to form the perovskite layers through an intramolecular exchanging process, decreases the concentration of deep-level defects. The defect-engineered thin perovskite layers enable the fabrication of PSCs with a certified power conversion efficiency of 22.1% in small cells and 19.7% in 1-square-centimeter cells.

4,603 citations


Journal ArticleDOI
TL;DR: Zheng et al. as discussed by the authors showed that quaternary ammonium halides can effectively passivate ionic defects in several different types of hybrid perovskite with their negative-and positive-charged components.
Abstract: The ionic defects at the surfaces and grain boundaries of organic–inorganic halide perovskite films are detrimental to both the efficiency and stability of perovskite solar cells. Here, we show that quaternary ammonium halides can effectively passivate ionic defects in several different types of hybrid perovskite with their negative- and positive-charged components. The efficient defect passivation reduces the charge trap density and elongates the carrier recombination lifetime, which is supported by density-function-theory calculation. The defect passivation reduces the open-circuit-voltage deficit of the p–i–n-structured device to 0.39 V, and boosts the efficiency to a certified value of 20.59 ± 0.45%. Moreover, the defect healing also significantly enhances the stability of films in ambient conditions. Our findings provide an avenue for defect passivation to further improve both the efficiency and stability of solar cells. Losses in solar cells can be caused by material defects in the bulk or at interfaces. Here, Zheng et al. use quaternary ammonium halides to passivate various perovskite absorbers and prepare solar cells with certified efficiency above 20%, suggesting that both anionic and cation defects are affected.

1,536 citations


Journal ArticleDOI
TL;DR: One-year stable perovskite devices are shown by engineering an ultra-stable 2D/3D (HOOC(CH2)4NH3)2PbI4/CH3NH3Pb mezzanine junction, which will enable the timely commercialization of perovSKite solar cells.
Abstract: Despite the impressive photovoltaic performances with power conversion efficiency beyond 22%, perovskite solar cells are poorly stable under operation, failing by far the market requirements. Various technological approaches have been proposed to overcome the instability problem, which, while delivering appreciable incremental improvements, are still far from a market-proof solution. Here we show one-year stable perovskite devices by engineering an ultra-stable 2D/3D (HOOC(CH2)4NH3)2PbI4/CH3NH3PbI3 perovskite junction. The 2D/3D forms an exceptional gradually-organized multi-dimensional interface that yields up to 12.9% efficiency in a carbon-based architecture, and 14.6% in standard mesoporous solar cells. To demonstrate the up-scale potential of our technology, we fabricate 10 × 10 cm2 solar modules by a fully printable industrial-scale process, delivering 11.2% efficiency stable for >10,000 h with zero loss in performances measured under controlled standard conditions. This innovative stable and low-cost architecture will enable the timely commercialization of perovskite solar cells. Up-scaling represents a key challenge for photovoltaics based on metal halide perovskites. Using a composite of 2D and 3D perovskites in combination with a printable carbon black/graphite counter electrode; Granciniet al., report 11.2% efficient modules stable over 10,000 hours.

1,531 citations


Journal ArticleDOI
TL;DR: Jiang et al. as mentioned in this paper proposed a low-temperature solution-processed SnO2 nanoparticles as an efficient electron transport layer for perovskite solar cells.
Abstract: Planar structures for halide perovskite solar cells have recently garnered attention, due to their simple and low-temperature device fabrication processing. Unfortunately, planar structures typically show I–V hysteresis and lower stable device efficiency compared with mesoporous structures, especially for TiO2-based n-i-p devices. SnO2, which has a deeper conduction band and higher electron mobility compared with traditional TiO2, could enhance charge transfer from perovskite to electron transport layers, and reduce charge accumulation at the interface. Here we report low-temperature solution-processed SnO2 nanoparticles as an efficient electron transport layer for perovskite solar cells. Our SnO2-based devices are almost free of hysteresis, which we propose is due to the enhancement of electron extraction. By introducing a PbI2 passivation phase in the perovskite layer, we obtain a 19.9 ± 0.6% certified efficiency. The devices can be easily processed under low temperature (150 ∘C), offering an efficient method for the large-scale production of perovskite solar cells. Planar structured perovskite solar cells often show hysteresis and lower efficiency than mesoporous ones. Jiang et al. show that using a SnO2 electron transport layer improves the performance of planar devices, reporting a certified efficiency of 19.9%, and enables a lower processing temperature.

1,500 citations


Journal ArticleDOI
TL;DR: In this paper, the authors improved the efficiency of monolithic, two-terminal, 1-cm2 perovskite/silicon tandems to 23.6% by combining an infrared-tuned silicon heterojunction bottom cell with the recently developed caesium formamidinium lead halide pervskite.
Abstract: As the record single-junction efficiencies of perovskite solar cells now rival those of copper indium gallium selenide, cadmium telluride and multicrystalline silicon, they are becoming increasingly attractive for use in tandem solar cells due to their wide, tunable bandgap and solution processability. Previously, perovskite/silicon tandems were limited by significant parasitic absorption and poor environmental stability. Here, we improve the efficiency of monolithic, two-terminal, 1-cm2 perovskite/silicon tandems to 23.6% by combining an infrared-tuned silicon heterojunction bottom cell with the recently developed caesium formamidinium lead halide perovskite. This more-stable perovskite tolerates deposition of a tin oxide buffer layer via atomic layer deposition that prevents shunts, has negligible parasitic absorption, and allows for the sputter deposition of a transparent top electrode. Furthermore, the window layer doubles as a diffusion barrier, increasing the thermal and environmental stability to enable perovskite devices that withstand a 1,000-hour damp heat test at 85 ∘C and 85% relative humidity. Perovskite solar cells can complement silicon photovoltaics in multijunction devices. Here, the authors optimize light harvesting in monolithic perovskite-on-silicon devices and fabricate a certified 23.6% efficient, 1 cm2 tandem solar cell with a perovskite device that withstands damp heat tests.

1,163 citations


Journal ArticleDOI
TL;DR: In this article, the authors report highly efficient perovskite LEDs enabled through the formation of self-assembled, nanometre-sized crystallites, with external quantum efficiencies of 10.4% for methylammonium lead iodide system and 9.3% for lead bromide system with significantly improved shelf and operational stability.
Abstract: Organic–inorganic hybrid perovskite materials are emerging as highly attractive semiconductors for use in optoelectronics. In addition to their use in photovoltaics, perovskites are promising for realizing light-emitting diodes (LEDs) due to their high colour purity, low non-radiative recombination rates and tunable bandgap. Here, we report highly efficient perovskite LEDs enabled through the formation of self-assembled, nanometre-sized crystallites. Large-group ammonium halides added to the perovskite precursor solution act as a surfactant that dramatically constrains the growth of 3D perovskite grains during film forming, producing crystallites with dimensions as small as 10 nm and film roughness of less than 1 nm. Coating these nanometre-sized perovskite grains with longer-chain organic cations yields highly efficient emitters, resulting in LEDs that operate with external quantum efficiencies of 10.4% for the methylammonium lead iodide system and 9.3% for the methylammonium lead bromide system, with significantly improved shelf and operational stability. Perovskite nanocrystal LEDs featuring long-chain ammonium cations offer improved stability and efficiency.

1,094 citations


Journal ArticleDOI
TL;DR: Wang et al. as mentioned in this paper introduced n-butylammonium cations into a mixed-cation lead mixed-halide FA0.83Cs0.17Pb(IyBr1−y)3 3D perovskite.
Abstract: Perovskite solar cells are remarkably efficient; however, they are prone to degradation in water, oxygen and ultraviolet light. Cation engineering in 3D perovskite absorbers has led to reduced degradation. Alternatively, 2D Ruddlesden–Popper layered perovskites exhibit improved stability, but have not delivered efficient solar cells so far. Here, we introduce n-butylammonium cations into a mixed-cation lead mixed-halide FA0.83Cs0.17Pb(IyBr1−y)3 3D perovskite. We observe the formation of 2D perovskite platelets, interspersed between highly orientated 3D perovskite grains, which suppress non-radiative charge recombination. We investigate the relationship between thin-film composition, crystal alignment and device performance. Solar cells with an optimal butylammonium content exhibit average stabilized power conversion efficiency of 17.5 ± 1.3% with a 1.61-eV-bandgap perovskite and 15.8 ± 0.8% with a 1.72-eV-bandgap perovskite. The stability under simulated sunlight is also enhanced. Cells sustain 80% of their ‘post burn-in’ efficiency after 1,000 h in air, and close to 4,000 h when encapsulated. Various strategies are developed to combine high efficiency and stability in perovskite solar cells. Here, Wang et al. mix 2D and 3D mixed-cation and mixed-halide perovskite phases in solar cells with stabilized efficiencies up to 19.5% and improved stability under full illumination and ambient air.

1,079 citations


Journal ArticleDOI
14 Apr 2017-Science
TL;DR: Ultraviolet damage in perovskite photovoltaics induced by TiO2 in the electron-transporting layer can be avoided with La-doped BaSnO3, and a low-temperature colloidal method for depositing La- doped Ba SnO3 films as a replacement forTiO2 is reported to reduce such ultraviolet-induced damage.
Abstract: Perovskite solar cells (PSCs) exceeding a power conversion efficiency (PCE) of 20% have mainly been demonstrated by using mesoporous titanium dioxide (mp-TiO2) as an electron-transporting layer. However, TiO2 can reduce the stability of PSCs under illumination (including ultraviolet light). Lanthanum (La)–doped BaSnO3 (LBSO) perovskite would be an ideal replacement given its electron mobility and electronic structure, but LBSO cannot be synthesized as well-dispersible fine particles or crystallized below 500°C. We report a superoxide colloidal solution route for preparing a LBSO electrode under very mild conditions (below 300°C). The PSCs fabricated with LBSO and methylammonium lead iodide (MAPbI3) show a steady-state power conversion efficiency of 21.2%, versus 19.7% for a mp-TiO2 device. The LBSO-based PSCs could retain 93% of their initial performance after 1000 hours of full-Sun illumination.

1,016 citations


Journal ArticleDOI
10 Nov 2017-Science
TL;DR: The perovskite oxide family is presented as a basis for developing such catalysts for (electro)chemical conversions spanning carbon, nitrogen, and oxygen chemistries and how these insights open experimental and computational opportunities to expand the compositional and chemical reaction space for next-generation perovkite catalysts.
Abstract: Catalysts for chemical and electrochemical reactions underpin many aspects of modern technology and industry, from energy storage and conversion to toxic emissions abatement to chemical and materials synthesis. This role necessitates the design of highly active, stable, yet earth-abundant heterogeneous catalysts. In this Review, we present the perovskite oxide family as a basis for developing such catalysts for (electro)chemical conversions spanning carbon, nitrogen, and oxygen chemistries. A framework for rationalizing activity trends and guiding perovskite oxide catalyst design is described, followed by illustrations of how a robust understanding of perovskite electronic structure provides fundamental insights into activity, stability, and mechanism in oxygen electrocatalysis. We conclude by outlining how these insights open experimental and computational opportunities to expand the compositional and chemical reaction space for next-generation perovskite catalysts.

963 citations


Journal ArticleDOI
TL;DR: This study finds that a moderate residual of PbI2 can deliver stable and high efficiency of solar cells without hysteresis, while too much residual Pbi2 will lead to serious hysteResis and poor transit stability.
Abstract: Low temperature solution processed planar-structure perovskite solar cells gain great attention recently, while their power conversions are still lower than that of high temperature mesoporous counterpart. Previous reports are mainly focused on perovskite morphology control and interface engineering to improve performance. Here, this study systematically investigates the effect of precise stoichiometry, especially the PbI2 contents on device performance including efficiency, hysteresis and stability. This study finds that a moderate residual of PbI2 can deliver stable and high efficiency of solar cells without hysteresis, while too much residual PbI2 will lead to serious hysteresis and poor transit stability. Solar cells with the efficiencies of 21.6% in small size (0.0737 cm2 ) and 20.1% in large size (1 cm2 ) with moderate residual PbI2 in perovskite layer are obtained. The certificated efficiency for small size shows the efficiency of 20.9%, which is the highest efficiency ever recorded in planar-structure perovskite solar cells, showing the planar-structure perovskite solar cells are very promising.

926 citations


Journal ArticleDOI
TL;DR: Mechanistic insights into oxygen-induced photodegradation of perovskite films are reported, finding fast oxygen diffusion into CH3NH3PbI3 films is accompanied by photo-induced formation of highly reactive superoxide species from oxygen.
Abstract: Methylammonium lead halide perovskites are attracting intense interest as promising materials for next-generation solar cells, but serious issues related to long-term stability need to be addressed. Perovskite films based on CH3NH3PbI3 undergo rapid degradation when exposed to oxygen and light. Here, we report mechanistic insights into this oxygen-induced photodegradation from a range of experimental and computational techniques. We find fast oxygen diffusion into CH3NH3PbI3 films is accompanied by photo-induced formation of highly reactive superoxide species. Perovskite films composed of small crystallites show higher yields of superoxide and lower stability. Ab initio simulations indicate that iodide vacancies are the preferred sites in mediating the photo-induced formation of superoxide species from oxygen. Thin-film passivation with iodide salts is shown to enhance film and device stability. The understanding of degradation phenomena gained from this study is important for the future design and optimization of stable perovskite solar cells.

Journal ArticleDOI
TL;DR: The use of CsPbBr3 QDs as novel photocatalysts to convert CO2 into solar fuels in nonaqueous media and the rate of electron consumption increased 25.5% because of improved electron extraction and transport.
Abstract: Halide perovskite quantum dots (QDs), primarily regarded as optoelectronic materials for LED and photovoltaic devices, have not been applied for photochemical conversion (e.g., water splitting or CO2 reduction) applications because of their insufficient stability in the presence of moisture or polar solvents. Herein, we report the use of CsPbBr3 QDs as novel photocatalysts to convert CO2 into solar fuels in nonaqueous media. Under AM 1.5G simulated illumination, the CsPbBr3 QDs steadily generated and injected electrons into CO2, catalyzing CO2 reduction at a rate of 23.7 μmol/g h with a selectivity over 99.3%. Additionally, through the construction of a CsPbBr3 QD/graphene oxide (CsPbBr3 QD/GO) composite, the rate of electron consumption increased 25.5% because of improved electron extraction and transport. This study is anticipated to provide new opportunities to utilize halide perovskite QD materials in photocatalytic applications.

Journal ArticleDOI
TL;DR: The origins of the significantly blue-shifted emission from CsPbBr3 nanocrystals and the synthetic strategies toward fabrication of stable perovskite nanocrystal materials with emission in the red and infrared parts of the optical spectrum are discussed, related to fabrication of mixed cation compounds guided by Goldschmidt tolerance factor considerations.
Abstract: This Perspective outlines basic structural and optical properties of lead halide perovskite colloidal nanocrystals, highlighting differences and similarities between them and conventional II–VI and III–V semiconductor quantum dots. A detailed insight into two important issues inherent to lead halide perovskite nanocrystals then follows, namely, the advantages of defect tolerance and the necessity to improve their stability in environmental conditions. The defect tolerance of lead halide perovskites offers an impetus to search for similar attributes in other related heavy metal-free compounds. We discuss the origins of the significantly blue-shifted emission from CsPbBr3 nanocrystals and the synthetic strategies toward fabrication of stable perovskite nanocrystal materials with emission in the red and infrared parts of the optical spectrum, which are related to fabrication of mixed cation compounds guided by Goldschmidt tolerance factor considerations. We conclude with the view on perspectives of use of th...

Journal ArticleDOI
24 Mar 2017-Science
TL;DR: It is reported that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovkite-crystal units is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovSKite layers.
Abstract: Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) Ruddlesden-Popper perovskites are solution-processed quantum wells wherein the band gap can be tuned by varying the perovskite-layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite-crystal units (>1.3 nanometers) is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovskite layers. These states provide a direct pathway for dissociating excitons into longer-lived free carriers that substantially improve the performance of optoelectronic devices.

Journal ArticleDOI
TL;DR: It is shown that charge carrier mobility within perovskite QD films is dictated by the chemical conditions at the QD-QD junctions, and the AX treatments presented here double the film mobility, enabling increased photocurrent, and lead to a record certified QD solar cell efficiency of 13.43%.
Abstract: We developed lead halide perovskite quantum dot (QD) films with tuned surface chemistry based on A-site cation halide salt (AX) treatments. QD perovskites offer colloidal synthesis and processing using industrially friendly solvents, which decouples grain growth from film deposition, and at present produce larger open-circuit voltages (VOC’s) than thin-film perovskites. CsPbI3 QDs, with a tunable bandgap between 1.75 and 2.13 eV, are an ideal top cell candidate for all-perovskite multijunction solar cells because of their demonstrated small VOC deficit. We show that charge carrier mobility within perovskite QD films is dictated by the chemical conditions at the QD-QD junctions. The AX treatments provide a method for tuning the coupling between perovskite QDs, which is exploited for improved charge transport for fabricating high-quality QD films and devices. The AX treatments presented here double the film mobility, enabling increased photocurrent, and lead to a record certified QD solar cell efficiency of 13.43%.

Journal ArticleDOI
TL;DR: A direct correlation is found between the density of traps, thedensity of mobile ionic defects, and the degree of hysteresis observed in the current–voltage (J–V) characteristics of perovskite solar cells.
Abstract: Trap-assisted recombination, despite being lower as compared with traditional inorganic solar cells, is still the dominant recombination mechanism in perovskite solar cells (PSCs) and limits their efficiency. We investigate the attributes of the primary trap-assisted recombination channels (grain boundaries and interfaces) and their correlation to defect ions in PSCs. We achieve this by using a validated device model to fit the simulations to the experimental data of efficient vacuum-deposited p–i–n and n–i–p CH3NH3PbI3 solar cells, including the light intensity dependence of the open-circuit voltage and fill factor. We find that, despite the presence of traps at interfaces and grain boundaries (GBs), their neutral (when filled with photogenerated charges) disposition along with the long-lived nature of holes leads to the high performance of PSCs. The sign of the traps (when filled) is of little importance in efficient solar cells with compact morphologies (fused GBs, low trap density). On the other hand,...

Journal ArticleDOI
19 Sep 2017-ACS Nano
TL;DR: It is shown that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects.
Abstract: Perovskite quantum dots (QDs) as a new type of colloidal nanocrystals have gained significant attention for both fundamental research and commercial applications owing to their appealing optoelectronic properties and excellent chemical processability. For their wide range of potential applications, synthesizing colloidal QDs with high crystal quality is of crucial importance. However, like most common QD systems such as CdSe and PbS, those reported perovskite QDs still suffer from a certain density of trapping defects, giving rise to detrimental nonradiative recombination centers and thus quenching luminescence. In this paper, we show that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects. This is realized with our improved synthetic protocol that involves introducing organolead compound trioctylphosphine–PbI2 (TOP–PbI2) as the reactive precursor, which also leads...

Journal ArticleDOI
04 Oct 2017-Nature
TL;DR: An all-solution-based perovskite detector could enable low-dose X-ray imaging, and could also be used in photoconductive devices for radiation imaging, sensing and energy harvesting.
Abstract: Medical X-ray imaging procedures require digital flat detectors operating at low doses to reduce radiation health risks. Solution-processed organic-inorganic hybrid perovskites have characteristics that make them good candidates for the photoconductive layer of such sensitive detectors. However, such detectors have not yet been built on thin-film transistor arrays because it has been difficult to prepare thick perovskite films (more than a few hundred micrometres) over large areas (a detector is typically 50 centimetres by 50 centimetres). We report here an all-solution-based (in contrast to conventional vacuum processing) synthetic route to producing printable polycrystalline perovskites with sharply faceted large grains having morphologies and optoelectronic properties comparable to those of single crystals. High sensitivities of up to 11 microcoulombs per air KERMA of milligray per square centimetre (μC mGyair-1 cm-2) are achieved under irradiation with a 100-kilovolt bremsstrahlung source, which are at least one order of magnitude higher than the sensitivities achieved with currently used amorphous selenium or thallium-doped cesium iodide detectors. We demonstrate X-ray imaging in a conventional thin-film transistor substrate by embedding an 830-micrometre-thick perovskite film and an additional two interlayers of polymer/perovskite composites to provide conformal interfaces between perovskite films and electrodes that control dark currents and temporal charge carrier transportation. Such an all-solution-based perovskite detector could enable low-dose X-ray imaging, and could also be used in photoconductive devices for radiation imaging, sensing and energy harvesting.

Journal ArticleDOI
TL;DR: In this paper, a scaling behavior of moisture-induced grain degradation in polycrystalline CH3NH3PbI3 films was reported, which can be explained by the degradation along the inplane direction, which is initiated at the grain boundary.
Abstract: The stability of perovskite solar cells has shown a huge variation with respect to the film process and film morphology, while the underlining mechanism for the morphology-dependent degradation of the perovskite film has remained elusive. Herein, we report a scaling behavior of moisture-induced grain degradation in polycrystalline CH3NH3PbI3 films. The degradation rates of CH3NH3PbI3 films in moisture were shown to be sensitive to the grain sizes. The duration that was needed for different films to degrade by the same percent showed a linear relationship with the grain size, despite the fact that the films were formed by five different deposition methods. This scaling behavior can be explained by the degradation along the in-plane direction, which is initiated at the grain boundary (GB). The GBs of CH3NH3PbI3 films consist of an amorphous intergranular layer, which allows quick diffusion of moisture into the perovskite films. It was found that thermal annealing induced surface self-passivation plays a critical role in stabilizing the surfaces of thin films and single crystals by reducing the moisture-sensitive methylammonium ions at the surface. The determination of the scaling behavior of grain degradation highlights the importance of stabilizing the GBs to improve the stability of perovskite solar cells.

Journal ArticleDOI
TL;DR: Low-dimensional Sn perovskite films in solar cells are reported that exhibit markedly enhanced air stability in comparison with their 3D counterparts, raising the prospects of pure Snperovskites for solar cells application.
Abstract: The low toxicity and a near-ideal choice of bandgap make tin perovskite an attractive alternative to lead perovskite in low cost solar cells. However, the development of Sn perovskite solar cells has been impeded by their extremely poor stability when exposed to oxygen. We report low-dimensional Sn perovskites that exhibit markedly enhanced air stability in comparison with their 3D counterparts. The reduced degradation under air exposure is attributed to the improved thermodynamic stability after dimensional reduction, the encapsulating organic ligands, and the compact perovskite film preventing oxygen ingress. We then explore these highly oriented low-dimensional Sn perovskite films in solar cells. The perpendicular growth of the perovskite domains between electrodes allows efficient charge carrier transport, leading to power conversion efficiencies of 5.94% without the requirement of further device structure engineering. We tracked the performance of unencapsulated devices over 100 h and found no apprec...

Journal ArticleDOI
TL;DR: This work incorporated a small amount of methylammonium organic cation into the CsPbBr3 lattice and by depositing a hydrophilic and insulating polyvinyl pyrrolidine polymer atop the ZnO electron-injection layer obtained light-emitting diodes exhibiting a high brightness and high external quantum efficiency.
Abstract: Inorganic perovskites such as CsPbX3 (X=Cl, Br, I) have attracted attention due to their excellent thermal stability and high photoluminescence quantum efficiency. However, the electroluminescence quantum efficiency of their light-emitting diodes was <1%. We posited that this low efficiency was a result of high leakage current caused by poor perovskite morphology, high non-radiative recombination at interfaces and perovskite grain boundaries, and also charge injection imbalance. Here, we incorporated a small amount of methylammonium organic cation into the CsPbBr3 lattice and by depositing a hydrophilic and insulating polyvinyl pyrrolidine polymer atop the ZnO electron-injection layer to overcome these issues. As a result, we obtained light-emitting diodes exhibiting a high brightness of 91,000 cd m−2 and a high external quantum efficiency of 10.4% using a mixed-cation perovskite Cs0.87MA0.13PbBr3 as the emitting layer. To the best of our knowledge, this is the brightest and most-efficient green perovskite light-emitting diodes reported to date. Hybrid organic-inorganic perovskites are garnering attention for light emitting diode (LED) applications. Employing a thin hydrophilic insulating polymer, Zhanget al. report LEDs exhibiting a brightness of 91,000 cd m−2and external quantum efficiency of 10.4% using a mixed-cation perovskite.

Journal ArticleDOI
21 Jul 2017-Science
TL;DR: Trimethylchloromethyl ammonium trichloromanganese(II), an organic-inorganic perovskite ferroelectric crystal processed from aqueous solution, has a large d33 of 185 picocoulombs per newton and a high phase-transition temperature of 406 kelvin (K) (16 K above that of BTO), which makes it a competitive candidate for medical, micromechanical, and biomechanical applications.
Abstract: Molecular piezoelectrics are highly desirable for their easy and environment-friendly processing, light weight, low processing temperature, and mechanical flexibility. However, although 136 years have passed since the discovery in 1880 of the piezoelectric effect, molecular piezoelectrics with a piezoelectric coefficient d33 comparable with piezoceramics such as barium titanate (BTO; ~190 picocoulombs per newton) have not been found. We show that trimethylchloromethyl ammonium trichloromanganese(II), an organic-inorganic perovskite ferroelectric crystal processed from aqueous solution, has a large d33 of 185 picocoulombs per newton and a high phase-transition temperature of 406 kelvin (K) (16 K above that of BTO). This makes it a competitive candidate for medical, micromechanical, and biomechanical applications.

Journal ArticleDOI
TL;DR: This work indicates that the doped perovskite NCs will inherit most of the unique optical properties of lanthanide ions and deliver them to the perovkite NC host, thus endowing the family of perovSKite materials with excellent optical, electric, or magnetic properties.
Abstract: Cesium lead halide (CsPbX3) perovskite nanocrystals (NCs) have demonstrated extremely excellent optical properties and great application potentials in various optoelectronic devices. However, because of the anion exchange, it is difficult to achieve white-light and multicolor emission for practical applications. Herein, we present the successful doping of various lanthanide ions (Ce3+, Sm3+, Eu3+, Tb3+, Dy3+, Er3+, and Yb3+) into the lattices of CsPbCl3 perovskite NCs through a modified hot-injection method. For the lanthanide ions doped perovskite NCs, high photoluminescence quantum yield (QY) and stable and widely tunable multicolor emissions spanning from visible to near-infrared (NIR) regions are successfully obtained. This work indicates that the doped perovskite NCs will inherit most of the unique optical properties of lanthanide ions and deliver them to the perovskite NC host, thus endowing the family of perovskite materials with excellent optical, electric, or magnetic properties.

Journal ArticleDOI
TL;DR: Zhao et al. as mentioned in this paper presented a certified 17% efficient tin and lead perovskite solar cell, which is integrated as the lowbandgap component of a tandem device with 21% efficiency.
Abstract: Tandem solar cells using only metal-halide perovskite sub-cells are an attractive choice for next-generation solar cells. However, the progress in developing efficient all-perovskite tandem solar cells has been hindered by the lack of high-performance low-bandgap perovskite solar cells. Here, we report efficient mixed tin–lead iodide low-bandgap (∼1.25 eV) perovskite solar cells with open-circuit voltages up to 0.85 V and over 70% external quantum efficiencies in the infrared wavelength range of 700–900 nm, delivering a short-circuit current density of over 29 mA cm−2 and demonstrating suitability for bottom-cell applications in all-perovskite tandem solar cells. Our low-bandgap perovskite solar cells achieve a maximum power conversion efficiency of 17.6% and a certified efficiency of 17.01% with a negligible current–voltage hysteresis. When mechanically stacked with a ∼1.58 eV bandgap perovskite top cell, our best all-perovskite 4-terminal tandem solar cell shows a steady-state efficiency of 21.0%. All-perovskite tandem solar cells hold the promise of high efficiencies whilst safeguarding the ease of fabrication intrinsic to perovskites. Here, Zhao et al. present a certified 17% efficient tin and lead perovskite solar cell, which is integrated as the low-bandgap component of a tandem device with 21% efficiency.

Journal ArticleDOI
05 Oct 2017-Nature
TL;DR: A new deposition route for methyl ammonium lead halide perovskite films that does not rely on use of a common solvent or vacuum, and relies on the rapid conversion of amine complex precursors to perovkite films, followed by a pressure application step to overcome the substantial reduction in power conversion efficiency when a small device is scaled up.
Abstract: A new deposition method for solar-panel polycrystalline perovskite thin films enables the production of large-area uniform films and avoids the need for common solvents or vacuum. Hybrid inorganic–organic perovskites are the most likely materials to replace silicon as absorber layers for solar cells, but issues with stability and scaling-up thin films mean that large-scale production is not yet possible. Liyuan Han and colleagues have developed a new deposition method for polycrystalline thin films that does not rely on spin- or drip-coating precursors in solvent or on vacuum deposition, and is therefore more amenable to larger-area films than are previous techniques. The procedure uses gaseous precursors and application of pressure, and has enabled a device with an area of 36 square centimetres to be certified at 12.1 per cent power conversion efficiency. Recent advances in the use of organic–inorganic hybrid perovskites for optoelectronics have been rapid, with reported power conversion efficiencies of up to 22 per cent for perovskite solar cells1,2,3,4,5,6,7,8,9. Improvements in stability have also enabled testing over a timescale of thousands of hours10,11,12,13,14. However, large-scale deployment of such cells will also require the ability to produce large-area, uniformly high-quality perovskite films. A key challenge is to overcome the substantial reduction in power conversion efficiency when a small device is scaled up: a reduction from over 20 per cent to about 10 per cent is found15,16,17,18,19,20,21 when a common aperture area of about 0.1 square centimetres is increased to more than 25 square centimetres. Here we report a new deposition route for methyl ammonium lead halide perovskite films that does not rely on use of a common solvent1,2,4,5,6,7,8,9,10,11,12,13,14,15 or vacuum3: rather, it relies on the rapid conversion of amine complex precursors to perovskite films, followed by a pressure application step. The deposited perovskite films were free of pin-holes and highly uniform. Importantly, the new deposition approach can be performed in air at low temperatures, facilitating fabrication of large-area perovskite devices. We reached a certified power conversion efficiency of 12.1 per cent with an aperture area of 36.1 square centimetres for a mesoporous TiO2-based perovskite solar module architecture.

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TL;DR: It is revealed that the incorporation of Ta to the Nb site can enhance the antiferroelectricity because of the reduced polarizability of B-site cations, which is confirmed by the polarization hysteresis, dielectric tunability, and selected-area electron diffraction measurements.
Abstract: Antiferroelectric materials that display double ferroelectric hysteresis loops are receiving increasing attention for their superior energy storage density compared to their ferroelectric counterparts. Despite the good properties obtained in antiferroelectric La-doped Pb(Zr,Ti)O3 -based ceramics, lead-free alternatives are highly desired due to the environmental concerns, and AgNbO3 has been highlighted as a ferrielectric/antiferroelectric perovskite for energy storage applications. Enhanced energy storage performance, with recoverable energy density of 4.2 J cm-3 and high thermal stability of the energy storage density (with minimal variation of ≤±5%) over 20-120 °C, can be achieved in Ta-modified AgNbO3 ceramics. It is revealed that the incorporation of Ta to the Nb site can enhance the antiferroelectricity because of the reduced polarizability of B-site cations, which is confirmed by the polarization hysteresis, dielectric tunability, and selected-area electron diffraction measurements. Additionally, Ta addition in AgNbO3 leads to decreased grain size and increased bulk density, increasing the dielectric breakdown strength, up to 240 kV cm-1 versus 175 kV cm-1 for the pure counterpart, together with the enhanced antiferroelectricity, accounting for the high energy storage density.

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TL;DR: In this paper, the authors demonstrate cesium cation (Cs+) doped 2D (BA)2(MA)3Pb4I13 perovskite solar cells giving a power conversion efficiency (PCE) as high as 13.7%.
Abstract: Two-dimensional (2D) organic–inorganic perovskites have recently emerged as one of the most important thin-film solar cell materials owing to their excellent environmental stability. The remaining major pitfall is their relatively poor photovoltaic performance in contrast to 3D perovskites. In this work we demonstrate cesium cation (Cs+) doped 2D (BA)2(MA)3Pb4I13 perovskite solar cells giving a power conversion efficiency (PCE) as high as 13.7%, the highest among the reported 2D devices, with excellent humidity resistance. The enhanced efficiency from 12.3% (without Cs+) to 13.7% (with 5% Cs+) is attributed to perfectly controlled crystal orientation, an increased grain size of the 2D planes, superior surface quality, reduced trap-state density, enhanced charge-carrier mobility and charge-transfer kinetics. Surprisingly, it is found that the Cs+ doping yields superior stability for the 2D perovskite solar cells when subjected to a high humidity environment without encapsulation. The device doped using 5% Cs+ degrades only ca. 10% after 1400 hours of exposure in 30% relative humidity (RH), and exhibits significantly improved stability under heating and high moisture environments. Our results provide an important step toward air-stable and fully printable low dimensional perovskites as a next-generation renewable energy source.

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TL;DR: This work presents a method that allows partial cation exchange in colloidal CsPbBr3 NCs, whereby Pb2+ is exchanged for several isovalent cations, resulting in doped Cspb1–xMxBr3NCs, with preservation of the original NC shape.
Abstract: Colloidal CsPbX3 (X = Br, Cl, and I) perovskite nanocrystals (NCs) have emerged as promising phosphors and solar cell materials due to their remarkable optoelectronic properties. These properties can be tailored by not only controlling the size and shape of the NCs but also postsynthetic composition tuning through topotactic anion exchange. In contrast, property control by cation exchange is still underdeveloped for colloidal CsPbX3 NCs. Here, we present a method that allows partial cation exchange in colloidal CsPbBr3 NCs, whereby Pb2+ is exchanged for several isovalent cations, resulting in doped CsPb1–xMxBr3 NCs (M= Sn2+, Cd2+, and Zn2+; 0 50%), sh...

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TL;DR: The UCLA team has successfully passivated perovskite film by controlling the film growth with functional polymers as additive, which opens up a new class of chemical additives for improving perovSkite performance and should pave the way toward improving perOVskite solar cells for high efficiency and stability.
Abstract: The solution processing of polycrystalline perovskite films introduces trap states that can adversely affect their optoelectronic properties. Motivated by the use of small-molecule surfactants to improve the optoelectronic performance of perovskites, we demonstrate the use of polymers with coordinating groups to improve the performance of solution-processed semiconductor films. The use of these polymer modifiers results in a marked change in the electronic properties of the films, as measured by both carrier dynamics and overall device performance. The devices grown with the polymer poly(4-vinylpyridine) (PVP) show significantly enhanced power conversion efficiency from 16.9 ± 0.7% to 18.8 ± 0.8% (champion efficiency, 20.2%) from a reverse scan and stabilized champion efficiency from 17.5 to 19.1% [under a bias of 0.94 V and AM (air mass) 1.5-G, 1-sun illumination over 30 min] compared to controls without any passivation. Treating the perovskite film with PVP enables a VOC of up to 1.16 V, which is among the best reported for a CH3NH3PbI3 perovskite solar cell and one of the lowest voltage deficits reported for any perovskite to date. In addition, perovskite solar cells treated with PVP show a long shelf lifetime of up to 90 days (retaining 85% of the initial efficiency) and increased by a factor of more than 20 compared to those without any polymer (degrading to 85% after ~4 days). Our work opens up a new class of chemical additives for improving perovskite performance and should pave the way toward improving perovskite solar cells for high efficiency and stability.

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TL;DR: Recent progress on lead-free PSCs is reviewed in terms of the theoretical insight and experimental explorations of the crystal structure of lead- free perovskite, thin film deposition, and device performance.
Abstract: Organic-inorganic hybrid halide perovskites (e.g., MAPbI3 ) have recently emerged as novel active materials for photovoltaic applications with power conversion efficiency over 22%. Conventional perovskite solar cells (PSCs); however, suffer the issue that lead is toxic to the environment and organisms for a long time and is hard to excrete from the body. Therefore, it is imperative to find environmentally-friendly metal ions to replace lead for the further development of PSCs. Previous work has demonstrated that Sn, Ge, Cu, Bi, and Sb ions could be used as alternative ions in perovskite configurations to form a new environmentally-friendly lead-free perovskite structure. Here, we review recent progress on lead-free PSCs in terms of the theoretical insight and experimental explorations of the crystal structure of lead-free perovskite, thin film deposition, and device performance. We also discuss the importance of obtaining further understanding of the fundamental properties of lead-free hybrid perovskites, especially those related to photophysics.