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Showing papers on "Perovskite (structure) published in 2019"


Journal ArticleDOI
TL;DR: In this paper, an organic halide salt phenethylammonium iodide (PEAI) was used on HC(NH2)2-CH3NH3 mixed perovskite films for surface defect passivation.
Abstract: In recent years, the power conversion efficiency of perovskite solar cells has increased to reach over 20%. Finding an effective means of defect passivation is thought to be a promising route for bringing further increases in the power conversion efficiency and the open-circuit voltage (VOC) of perovskite solar cells. Here, we report the use of an organic halide salt phenethylammonium iodide (PEAI) on HC(NH2)2–CH3NH3 mixed perovskite films for surface defect passivation. We find that PEAI can form on the perovskite surface and results in higher-efficiency cells by reducing the defects and suppressing non-radiative recombination. As a result, planar perovskite solar cells with a certificated efficiency of 23.32% (quasi-steady state) are obtained. In addition, a VOC as high as 1.18 V is achieved at the absorption threshold of 1.53 eV, which is 94.4% of the Shockley–Queisser limit VOC (1.25 V). Planar perovskite solar cells that have been passivated using the organic halide salt phenethylammonium iodide are shown to have suppressed non-radiative recombination and operate with a certified power conversion efficiency of 23.3%.

3,064 citations


Journal ArticleDOI
TL;DR: The fundamentals, recent research progress, present status, and views on future prospects of perovskite-based photovoltaics, with discussions focused on strategies to improve both intrinsic and extrinsic (environmental) stabilities of high-efficiency devices are described.
Abstract: The photovoltaics of organic–inorganic lead halide perovskite materials have shown rapid improvements in solar cell performance, surpassing the top efficiency of semiconductor compounds such as CdTe and CIGS (copper indium gallium selenide) used in solar cells in just about a decade. Perovskite preparation via simple and inexpensive solution processes demonstrates the immense potential of this thin-film solar cell technology to become a low-cost alternative to the presently commercially available photovoltaic technologies. Significant developments in almost all aspects of perovskite solar cells and discoveries of some fascinating properties of such hybrid perovskites have been made recently. This Review describes the fundamentals, recent research progress, present status, and our views on future prospects of perovskite-based photovoltaics, with discussions focused on strategies to improve both intrinsic and extrinsic (environmental) stabilities of high-efficiency devices. Strategies and challenges regardi...

1,720 citations


Journal ArticleDOI
TL;DR: The recent advances in passivation of imperfections and suppressing ion migration to achieve improved efficiency and highly stable perovskite solar cells are reviewed.
Abstract: All highly-efficient organic–inorganic halide perovskite (OIHP) solar cells to date are made of polycrystalline perovskite films which contain a high density of defects, including point and extended imperfections. The imperfections in OIHP materials play an important role in the process of charge recombination and ion migration in perovskite solar cells (PSC), which heavily influences the resulting device energy conversion efficiency and stability. Here we review the recent advances in passivation of imperfections and suppressing ion migration to achieve improved efficiency and highly stable perovskite solar cells. Due to the ionic nature of OIHP materials, the defects in the photoactive films are inevitably electrically charged. The deep level traps induced by particular charged defects in OIHP films are major non-radiative recombination centers; passivation by coordinate bonding, ionic bonding, or chemical conversion have proven effective in mitigating the negative impacts of these deep traps. Shallow level charge traps themselves may contribute little to non-radiative recombination, but the migration of charged shallow level traps in OIHP films results in unfavorable band bending, interfacial reactions, and phase segregation, influencing the carrier extraction efficiency. Finally, the impact of defects and ion migration on the stability of perovskite solar cells is described.

1,040 citations


Journal ArticleDOI
TL;DR: Recommendations are made on how accelerated testing should be performed to rapidly develop solar cells that are both extraordinarily efficient and stable.
Abstract: This review article examines the current state of understanding in how metal halide perovskite solar cells can degrade when exposed to moisture, oxygen, heat, light, mechanical stress, and reverse bias. It also highlights strategies for improving stability, such as tuning the composition of the perovskite, introducing hydrophobic coatings, replacing metal electrodes with carbon or transparent conducting oxides, and packaging. The article concludes with recommendations on how accelerated testing should be performed to rapidly develop solar cells that are both extraordinarily efficient and stable.

962 citations


Journal ArticleDOI
01 Jul 2019-Nature
TL;DR: Addition of an ionic liquid, BMIMBF4, to metal halide perovskite solar cells improves their efficiency and long-term operation under accelerated aging conditions of high temperature and full-spectrum sunlight.
Abstract: Solar cells based on metal halide perovskites are one of the most promising photovoltaic technologies(1-4). Over the past few years, the long-term operational stability of such devices has been gre ...

939 citations


Journal ArticleDOI
09 Aug 2019-Science
TL;DR: High crystalline β-CsPbI3 films are obtained with an extended spectral response and enhanced phase stability and made from the treated material have highly reproducible and stable efficiencies reaching 18.4% under 45 ± 5°C ambient conditions.
Abstract: Although β-CsPbI3 has a bandgap favorable for application in tandem solar cells, depositing and stabilizing β-CsPbI3 experimentally has remained a challenge. We obtained highly crystalline β-CsPbI3 films with an extended spectral response and enhanced phase stability. Synchrotron-based x-ray scattering revealed the presence of highly oriented β-CsPbI3 grains, and sensitive elemental analyses-including inductively coupled plasma mass spectrometry and time-of-flight secondary ion mass spectrometry-confirmed their all-inorganic composition. We further mitigated the effects of cracks and pinholes in the perovskite layer by surface treating with choline iodide, which increased the charge-carrier lifetime and improved the energy-level alignment between the β-CsPbI3 absorber layer and carrier-selective contacts. The perovskite solar cells made from the treated material have highly reproducible and stable efficiencies reaching 18.4% under 45 ± 5°C ambient conditions.

852 citations


Journal ArticleDOI
TL;DR: A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses as mentioned in this paper.
Abstract: A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses. Defect passivation using organic molecul ...

849 citations


Journal ArticleDOI
TL;DR: Li et al. as discussed by the authors employed fluoride to simultaneously passivate both anion and cation vacancies, by taking advantage of the extremely high electronegativity of fluoride, and obtained a power conversion efficiency of 21.46% (and a certified 21.3%-efficient cell) in a device based on the caesium, methylammonium (MA), and formamidinium (FA) triple-cation perovskite (Cs0.05FA0.41)Pb(I0.98Br0.02)3 treated with sodium
Abstract: Defects play an important role in the degradation processes of hybrid halide perovskite absorbers, impeding their application for solar cells. Among all defects, halide anion and organic cation vacancies are ubiquitous, promoting ion diffusion and leading to thin-film decomposition at surfaces and grain boundaries. Here, we employ fluoride to simultaneously passivate both anion and cation vacancies, by taking advantage of the extremely high electronegativity of fluoride. We obtain a power conversion efficiency of 21.46% (and a certified 21.3%-efficient cell) in a device based on the caesium, methylammonium (MA) and formamidinium (FA) triple-cation perovskite (Cs0.05FA0.54MA0.41)Pb(I0.98Br0.02)3 treated with sodium fluoride. The device retains 90% of its original power conversion efficiency after 1,000 h of operation at the maximum power point. With the help of first-principles density functional theory calculations, we argue that the fluoride ions suppress the formation of halide anion and organic cation vacancies, through a unique strengthening of the chemical bonds with the surrounding lead and organic cations. Defects and defect migration are detrimental for perovskite solar cell efficiency and long-term stability. Li et al. show that fluoride is able to suppress the formation of halide anion and organic cation vacancy defects by restraining the relative ions via ionic and hydrogen bonds.

723 citations


Journal ArticleDOI
29 Aug 2019-Nature
TL;DR: The observation of superconductivity in an infinite-layer nickelate that is isostructural to infinite- Layer copper oxides11–13 and the possibility of a family of nickelate superconductors analogous to Copper oxides and pnictides25 is suggested.
Abstract: The discovery of unconventional superconductivity in (La,Ba)2CuO4 (ref. 1) has motivated the study of compounds with similar crystal and electronic structure, with the aim of finding additional superconductors and understanding the origins of copper oxide superconductivity. Isostructural examples include bulk superconducting Sr2RuO4 (ref. 2) and surface-electron-doped Sr2IrO4, which exhibits spectroscopic signatures consistent with a superconducting gap3,4, although a zero-resistance state has not yet been observed. This approach has also led to the theoretical investigation of nickelates5,6, as well as thin-film heterostructures designed to host superconductivity. One such structure is the LaAlO3/LaNiO3 superlattice7–9, which has been recently proposed for the creation of an artificially layered nickelate heterostructure with a singly occupied $${d}_{{x}^{2}-{y}^{2}}$$ band. The absence of superconductivity observed in previous related experiments has been attributed, at least in part, to incomplete polarization of the eg orbitals10. Here we report the observation of superconductivity in an infinite-layer nickelate that is isostructural to infinite-layer copper oxides11–13. Using soft-chemistry topotactic reduction14–20, NdNiO2 and Nd0.8Sr0.2NiO2 single-crystal thin films are synthesized by reducing the perovskite precursor phase. Whereas NdNiO2 exhibits a resistive upturn at low temperature, measurements of the resistivity, critical current density and magnetic-field response of Nd0.8Sr0.2NiO2 indicate a superconducting transition temperature of about 9 to 15 kelvin. Because this compound is a member of a series of reduced layered nickelate crystal structures21–23, these results suggest the possibility of a family of nickelate superconductors analogous to copper oxides24 and pnictides25. Superconductivity is demonstrated in an infinite-layer nickelate similar to infinite-layer copper oxides, which is synthesized using soft- chemistry topotactic reduction of the perovskite precursor phase.

690 citations


Journal ArticleDOI
03 May 2019-Science
TL;DR: The addition of guanidinium thiocyanate (GuaSCN) resulted in marked improvements in the structural and optoelectronic properties of Sn-Pb mixed, low-band gap perovskite films, enabling the demonstration of >20% efficient low–band gap PSCs.
Abstract: All-perovskite-based polycrystalline thin-film tandem solar cells have the potential to deliver efficiencies of >30%. However, the performance of all-perovskite-based tandem devices has been limited by the lack of high-efficiency, low-band gap tin-lead (Sn-Pb) mixed-perovskite solar cells (PSCs). We found that the addition of guanidinium thiocyanate (GuaSCN) resulted in marked improvements in the structural and optoelectronic properties of Sn-Pb mixed, low-band gap (~1.25 electron volt) perovskite films. The films have defect densities that are lower by a factor of 10, leading to carrier lifetimes of greater than 1 microsecond and diffusion lengths of 2.5 micrometers. These improved properties enable our demonstration of >20% efficient low-band gap PSCs. When combined with wider-band gap PSCs, we achieve 25% efficient four-terminal and 23.1% efficient two-terminal all-perovskite-based polycrystalline thin-film tandem solar cells.

672 citations


Journal ArticleDOI
TL;DR: Lin et al. as discussed by the authors used metallic tin to prevent oxidation in mixed Pb-Sn narrowbandgap perovskites to reduce the Sn4+ (an oxidation product of Sn2+) to Sn2+ via a comproportionation reaction.
Abstract: Combining wide-bandgap and narrow-bandgap perovskites to construct monolithic all-perovskite tandem solar cells offers avenues for continued increases in photovoltaic (PV) power conversion efficiencies (PCEs). However, actual efficiencies today are diminished by the subpar performance of narrow-bandgap subcells. Here we report a strategy to reduce Sn vacancies in mixed Pb–Sn narrow-bandgap perovskites that use metallic tin to reduce the Sn4+ (an oxidation product of Sn2+) to Sn2+ via a comproportionation reaction. We increase, thereby, the charge-carrier diffusion length in narrow-bandgap perovskites to 3 μm for the best materials. We obtain a PCE of 21.1% for 1.22-eV narrow-bandgap solar cells. We fabricate monolithic all-perovskite tandem cells with certified PCEs of 24.8% for small-area devices (0.049 cm2) and of 22.1% for large-area devices (1.05 cm2). The tandem cells retain 90% of their performance following 463 h of operation at the maximum power point under full 1-sun illumination. Improvements in the efficiency and stability of low-bandgap perovskite solar cells are key to enabling all-perovskite solar cells. Here, Lin et al. use metallic tin to prevent oxidation in such low-gap perovskite and demonstrate 24.8%-efficient tandems that are stable for over 400 h under operating conditions.

Journal ArticleDOI
TL;DR: In this article, a review of the state of the art in 2D perovskites is provided, providing an overview of structural and materials engineering aspects and optical and photophysical properties.
Abstract: Hybrid perovskites are currently one of the most active fields of research owing to their enormous potential for photovoltaics. The performance of 3D hybrid organic–inorganic perovskite solar cells has increased at an incredible rate, reaching power conversion efficiencies comparable to those of many established technologies. However, the commercial application of 3D hybrid perovskites is inhibited by their poor stability. Relative to 3D hybrid perovskites, low-dimensional — that is, 2D — hybrid perovskites have demonstrated higher moisture stability, offering new approaches to stabilizing perovskite-based photovoltaic devices. Furthermore, 2D hybrid perovskites have versatile structures, enabling the fine-tuning of their optoelectronic properties through compositional engineering. In this Review, we discuss the state of the art in 2D perovskites, providing an overview of structural and materials engineering aspects and optical and photophysical properties. Moreover, we discuss recent developments along with the main limitations of 3D perovskites and assess the advantages of 2D perovskites over their 3D parent structures in terms of stability. Finally, we review recent achievements in combining 3D and 2D perovskites as an approach to simultaneously boost device efficiency and stability, paving the way for mixed-dimensional perovskite solar cells for commercial applications. Combining low-dimensional and 3D perovskites is a promising approach to achieve stable and efficient solar cells. In this Review, we discuss the structural, optical and photophysical properties of low-dimensional perovskites, compare the stability and efficiency of 2D and 3D perovskite devices, and consider 2D/3D composites as a strategy to increase the stability of perovskite solar cells.

Journal ArticleDOI
TL;DR: In this article, the authors developed an accurate, physically interpretable, and one-dimensional tolerance factor, τ, that correctly predicts 92% of compounds as perovskite or nonperovskiy for an experimental dataset of 576 ABX 3 materials.
Abstract: Predicting the stability of the perovskite structure remains a long-standing challenge for the discovery of new functional materials for many applications including photovoltaics and electrocatalysts. We developed an accurate, physically interpretable, and one-dimensional tolerance factor, τ, that correctly predicts 92% of compounds as perovskite or nonperovskite for an experimental dataset of 576 ABX 3 materials ( X = O 2− , F − , Cl − , Br − , I − ) using a novel data analytics approach based on SISSO (sure independence screening and sparsifying operator). τ is shown to generalize outside the training set for 1034 experimentally realized single and double perovskites (91% accuracy) and is applied to identify 23,314 new double perovskites ( A 2 BB′X 6 ) ranked by their probability of being stable as perovskite. This work guides experimentalists and theorists toward which perovskites are most likely to be successfully synthesized and demonstrates an approach to descriptor identification that can be extended to arbitrary applications beyond perovskite stability predictions.

Journal ArticleDOI
02 Aug 2019-Science
TL;DR: Th Thin lead oxysalt layers passivate hybrid perovskite surfaces under an ambient atmosphere and enhance solar cell efficiency and formation of the lead oxYSalt layer increases the carrier recombination lifetime and boosts the efficiency of the solar cells to 21.1%.
Abstract: We show that converting the surfaces of lead halide perovskite to water-insoluble lead (II) oxysalt through reaction with sulfate or phosphate ions can effectively stabilize the perovskite surface and bulk material. These capping lead oxysalt thin layers enhance the water resistance of the perovskite films by forming strong chemical bonds. The wide-bandgap lead oxysalt layers also reduce the defect density on the perovskite surfaces by passivating undercoordinated surface lead centers, which are defect-nucleating sites. Formation of the lead oxysalt layer increases the carrier recombination lifetime and boosts the efficiency of the solar cells to 21.1%. Encapsulated devices stabilized by the lead oxysalt layers maintain 96.8% of their initial efficiency after operation at maximum power point under simulated air mass (AM) 1.5 G irradiation for 1200 hours at 65°C.

Journal ArticleDOI
TL;DR: In this article, the authors summarized recent developments in the synthesis and characterization of metal halide perovskite nanostructures with controllable compositions, dimensionality, morphologies and orientations.
Abstract: Nanostructures of inorganic semiconductors have revolutionized many areas of electronics, optoelectronics and photonics. The controlled synthesis of semiconductor nanostructures could lead to novel physical properties, improved optoelectronic device performance and new areas for exploration. Lead halide perovskites have recently excited the photovoltaic research community owing to their high solar-conversion efficiencies and ease of solution processing; they also hold great promise for optoelectronic applications, such as light-emitting diodes and lasers. In this Review, we summarize recent developments in the synthesis and characterization of metal halide perovskite nanostructures with controllable compositions, dimensionality, morphologies and orientations. We examine the advantageous optical properties, improved stability and potential optoelectronic applications of these 1D and 2D single-crystal perovskite nanostructures and compare them with those of bulk perovskites and nanostructures of conventional semiconductors. Studies in which perovskite nanostructures have been used to study the fundamental physical properties of perovskites are also highlighted. Finally, we discuss the challenges in realizing halide perovskite nanostructures for optoelectronic and photonic applications and offer our perspectives on future opportunities and research directions. Metal halide perovskite nanostructures are promising materials for optoelectronic applications. In this Review, we discuss the synthesis and properties of 1D and 2D single-crystal perovskite nanostructures, examine potential optoelectronic applications and highlight recent studies in which these nanostructures have been used to study the fundamental properties of perovskites.

Journal ArticleDOI
TL;DR: This work systematically engineer the structures of passivation molecular functional groups, including carboxyl, amine, isopropyl, phenethyl, and tert-butylphenethyl groups, and study their passivation capability to perovskites to provide guidance for future design of new passivation molecules to realize multiple facets applications in perovkite electronics.
Abstract: Passivation of electronic defects at the surface and grain boundaries of perovskite materials has become one of the most important strategies to suppress charge recombination in both polycrystalline and single-crystalline perovskite solar cells. Although many passivation molecules have been reported, it remains very unclear regarding the passivation mechanisms of various functional groups. Here, we systematically engineer the structures of passivation molecular functional groups, including carboxyl, amine, isopropyl, phenethyl, and tert-butylphenethyl groups, and study their passivation capability to perovskites. It reveals the carboxyl and amine groups would heal charged defects via electrostatic interactions, and the neutral iodine related defects can be reduced by the aromatic structures. The judicious control of the interaction between perovskite and molecules can further realize grain boundary passivation, including those that are deep toward substrates. Understanding of the underlining mechanisms allows us to design a new passivation molecule, D-4- tert-butylphenylalanine, yielding high-performance p-i-structure solar cells with a stabilized efficiency of 21.4%. The open-circuit voltage ( VOC) of a device with an optical bandgap of 1.57 eV for the perovskite layer reaches 1.23 V, corresponding to a record small VOC deficit of 0.34 V. Our findings provide a guidance for future design of new passivation molecules to realize multiple facets applications in perovskite electronics.

Journal ArticleDOI
TL;DR: Reviews on the theoretical understanding of the electronic, optical, and defect properties of Pb and Pb-free halide perovskites andperovskite derivatives are provided, as well as the experimental results available in the literature.
Abstract: 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.

Journal ArticleDOI
TL;DR: This new approach provides water- and heat-resistant operationally stable PSCs with a record-level PCE, and enhances interfacial hole extraction, suppressing nonradiative carrier recombination and enabling a power conversion efficiency (PCE) >22%, the highest reported for 3D/2D architectures.
Abstract: Preventing the degradation of metal perovskite solar cells (PSCs) by humid air poses a substantial challenge for their future deployment. We introduce here a two-dimensional (2D) A2PbI4 perovskite layer using pentafluorophenylethylammonium (FEA) as a fluoroarene cation inserted between the 3D light-harvesting perovskite film and the hole-transporting material (HTM). The perfluorinated benzene moiety confers an ultrahydrophobic character to the spacer layer, protecting the perovskite light-harvesting material from ambient moisture while mitigating ionic diffusion in the device. Unsealed 3D/2D PSCs retain 90% of their efficiency during photovoltaic operation for 1000 hours in humid air under simulated sunlight. Remarkably, the 2D layer also enhances interfacial hole extraction, suppressing nonradiative carrier recombination and enabling a power conversion efficiency (PCE) >22%, the highest reported for 3D/2D architectures. Our new approach provides water- and heat-resistant operationally stable PSCs with a record-level PCE.

Journal ArticleDOI
TL;DR: In this article, the hidden role of isopropyl alcohol (IPA) in surface treatments is demonstrated and a strategy in which the passivating agent is deposited without destabilizing the high quality perovskite underlayer.
Abstract: Stabilization of the crystal phase of inorganic/organic lead halide perovskites is critical for their high performance optoelectronic devices. However, due to the highly ionic nature of perovskite crystals, even phase stabilized polycrystalline perovskites can undergo undesirable phase transitions when exposed to a destabilizing environment. While various surface passivating agents have been developed to improve the device performance of perovskite solar cells, conventional deposition methods using a protic polar solvent, mainly isopropyl alcohol (IPA), results in a destabilization of the underlying perovskite layer and an undesirable degradation of device properties. We demonstrate the hidden role of IPA in surface treatments and develop a strategy in which the passivating agent is deposited without destabilizing the high quality perovskite underlayer. This strategy maximizes and stabilizes device performance by suppressing the formation of the perovskite δ-phase and amorphous phase during surface treatment, which is observed using conventional methods. Our strategy also effectively passivates surface and grain boundary defects, minimizing non-radiative recombination sites, and preventing carrier quenching at the perovskite interface. This results in an open-circuit-voltage loss of only ∼340 mV, a champion device with a power conversion efficiency of 23.4% from a reverse current–voltage scan, a device with a record certified stabilized PCE of 22.6%, and enhanced operational stability. In addition, our perovskite solar cell exhibits an electroluminescence external quantum efficiency up to 8.9%.

Journal ArticleDOI
TL;DR: A comprehensive review of the latest developments of the various types of perovskite piezoelectric ceramic systems is presented in this article, with special attention given to three promising families of lead-free perovsite ferroelectrics: the barium titanate, alkaline niobate and bismuth pervskites.
Abstract: High strain piezoelectric ceramics are the state-of-the-art materials for high precision, positioning devices. A comprehensive review of the latest developments of the various types of perovskite piezoelectric ceramic systems is presented herein, with special attention given to three promising families of lead-free perovskite ferroelectrics: the barium titanate, alkaline niobate and bismuth perovskites. Included in this review are details of phase transition behavior, strain enhancement approaches, material reliabilities as well as the status of some promising applications. This current review describes both compositional and structural engineering approaches that are intended to achieve enhanced strain properties in perovskite piezoelectric ceramics. The factors that affect the strain behavior of high-strain perovskite piezoelectric ceramics are addressed. The reliability characteristics of these high-strain ferroelectrics as well as the recent approaches to the long-term electrical, thermal and time-stability enhancement are summarized. Several promising applications of high-strain perovskite materials are introduced, which take advantages of their characteristics; examples include high-energy storage, pyroelectric and electro-caloric effect and luminescent properties.

Journal ArticleDOI
TL;DR: In this paper, a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes, were studied.
Abstract: Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (VOC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the VOC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the VOC of the device. Importantly, the VOC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the VOC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the VOC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces.

Journal ArticleDOI
TL;DR: The impact of the gradient in-plane strain on the carrier dynamics of the strained perovskite films and optimize the device efficiency is studied to enhance PCEs up to 20.7% (certified) in devices via rational strain engineering.
Abstract: The mixed halide perovskites have emerged as outstanding light absorbers for efficient solar cells. Unfortunately, it reveals inhomogeneity in these polycrystalline films due to composition separation, which leads to local lattice mismatches and emergent residual strains consequently. Thus far, the understanding of these residual strains and their effects on photovoltaic device performance is absent. Herein we study the evolution of residual strain over the films by depth-dependent grazing incident X-ray diffraction measurements. We identify the gradient distribution of in-plane strain component perpendicular to the substrate. Moreover, we reveal its impacts on the carrier dynamics over corresponding solar cells, which is stemmed from the strain induced energy bands bending of the perovskite absorber as indicated by first-principles calculations. Eventually, we modulate the status of residual strains in a controllable manner, which leads to enhanced PCEs up to 20.7% (certified) in devices via rational strain engineering. The residual strains in the mixed halide perovskite thin films and their effects on the solar cell devices are less understood. Here Zhu et al. study the impact of the gradient in-plane strain on the carrier dynamics of the strained perovskite films and optimize the device efficiency.

Journal ArticleDOI
TL;DR: The native-oxide passivation approach reported here represents an alternate avenue for boosting the efficiency and stability of lead-free PSCs, and develops inorganic cesium tin and germanium mixed-cation perovskites that show high operational stability and efficiency over 7%.
Abstract: There has been an urgent need to eliminate toxic lead from the prevailing halide perovskite solar cells (PSCs), but the current lead-free PSCs are still plagued with the critical issues of low efficiency and poor stability. This is primarily due to their inadequate photovoltaic properties and chemical stability. Herein we demonstrate the use of the lead-free, all-inorganic cesium tin-germanium triiodide (CsSn0.5Ge0.5I3) solid-solution perovskite as the light absorber in PSCs, delivering promising efficiency of up to 7.11%. More importantly, these PSCs show very high stability, with less than 10% decay in efficiency after 500 h of continuous operation in N2 atmosphere under one-sun illumination. The key to this striking performance of these PSCs is the formation of a full-coverage, stable native-oxide layer, which fully encapsulates and passivates the perovskite surfaces. The native-oxide passivation approach reported here represents an alternate avenue for boosting the efficiency and stability of lead-free PSCs. Replacing the toxic lead in the state-of-the-art halide perovskite solar cells is highly desired but the device performance and stability are usually compromised. Here Chen et al. develop inorganic cesium tin and germanium mixed-cation perovskites that show high operational stability and efficiency over 7%.

Journal ArticleDOI
TL;DR: The fundamental background knowledge of nucleation and crystal growth processes in solution including the LaMer model and Ostwald ripening process is described and the contemporary progress in chemical precursor composition is provided to comprehend the current research approaches to further enhance photovoltaic performance and device stability.
Abstract: Over the last several years, inorganic–organic hybrid perovskites have shown dramatic achievements in photovoltaic performance and device stability. Despite the significant progress in photovoltaic application, an in-depth understanding of the fundamentals of precursor solution chemistry is still lacking. In this review, the fundamental background knowledge of nucleation and crystal growth processes in solution including the LaMer model and Ostwald ripening process is described. This review article also highlights the recent progress in precursor-coordinating molecule interaction in solution along with the role of anti-solvent in the solvent engineering process to control nucleation and crystal growth. Moreover, chemical pathways from precursor solution to perovskite film formation are given. This represents identification of the intermediate phase induced by precursor-coordinating molecule interaction and responsible intermediate species for uniform and dense perovskite film formation. Further to the description of chemical phenomena in solution, the contemporary progress in chemical precursor composition is also provided to comprehend the current research approaches to further enhance photovoltaic performance and device stability. On the basis of the critical and comprehensive review, we provide some perspectives to further achieve high-performance perovskite solar cells with long-term device stability through precisely controlled nucleation and crystal growth in precursor solution.

Journal ArticleDOI
TL;DR: In this paper, the authors demonstrate blue perovskite LEDs (PeLEDs) with a peak external quantum efficiency of up to 9.5% at a luminance of 54'cd m−2.
Abstract: The emergence of inorganic–organic hybrid perovskites, a unique class of solution-processable crystalline semiconductors, provides new opportunities for large-area, low-cost and colour-saturated light-emitting diodes (LEDs) ideal for display and solid-state lighting applications1. However, the performance of blue perovskite LEDs (PeLEDs)2–11 is far inferior to that of their near-infrared, red and green counterparts12–19, strongly limiting the practicality of the PeLED technology. Here, we demonstrate blue PeLEDs emitting at 483 nm with colour coordinates of (0.094, 0.184) and operating with a peak external quantum efficiency of up to 9.5% at a luminance of 54 cd m–2. The devices have a T50 lifetime of 250 s for an initial brightness of 100 cd m–2. The efficient blue electroluminescence originates from a structure of quantum-confined perovskite nanoparticles embedded within quasi-two-dimensional phases with higher bandgaps, prepared by an antisolvent processing scheme. Our work paves the way towards high-performance PeLEDs in the blue region. Blue light-emitting diodes based on perovskite nanostructures embedded within quasi-two-dimensional phases show highly effective charge injection and suppressed non-radiative recombination.

Journal ArticleDOI
TL;DR: This work encapsulates low-cost CH3 NH3 PbI3 (MAPbI 3 ) perovskite QDs in the pores of earth-abundant Fe-porphyrin based metal organic framework PCN-221(Fex) by a sequential deposition route to construct a series of composite photocatalysts protected by the MOF, which exhibit much improved stability in reaction systems containing water.
Abstract: Improving the stability of lead halide perovskite quantum dots (QDs) in a system containing water is the key for their practical application in artificial photosynthesis. Herein, we encapsulate low-cost CH3 NH3 PbI3 (MAPbI3 ) perovskite QDs in the pores of earth-abundant Fe-porphyrin based metal organic framework (MOF) PCN-221(Fex ) by a sequential deposition route, to construct a series of composite photocatalysts of MAPbI3 @PCN-221(Fex ) (x=0-1). Protected by the MOF the composite photocatalysts exhibit much improved stability in reaction systems containing water. The close contact of QDs to the Fe catalytic site in the MOF, allows the photogenerated electrons in the QDs to transfer rapidly the Fe catalytic sites to enhance the photocatalytic activity for CO2 reduction. Using water as an electron source, MAPbI3 @PCN-221(Fe0.2 ) exhibits a record-high total yield of 1559 μmol g-1 for photocatalytic CO2 reduction to CO (34 %) and CH4 (66 %), 38 times higher than that of PCN-221(Fe0.2 ) in the absence of perovskite QDs.

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TL;DR: The present paper is a review of the past and present literature on both colloidal nanostructures and multilayered compounds, emphasizing that availability of accurate structural information is of dramatic importance to reach a fair understanding of quantum and dielectric confinement effects.
Abstract: Hybrid halide perovskites are now superstar materials leading the field of low-cost thin film photovoltaics technologies. Following the surge for more efficient and stable 3D bulk alloys, multilayered halide perovskites and colloidal perovskite nanostructures appeared in 2016 as viable alternative solutions to this challenge, largely exceeding the original proof of concept made in 2009 and 2014, respectively. This triggered renewed interest in lower-dimensional hybrid halide perovskites and at the same time increasingly more numerous and differentiated applications. The present paper is a review of the past and present literature on both colloidal nanostructures and multilayered compounds, emphasizing that availability of accurate structural information is of dramatic importance to reach a fair understanding of quantum and dielectric confinement effects. Layered halide perovskites occupy a special place in the history of halide perovskites, with a large number of seminal papers in the 1980s and 1990s. In ...

Journal ArticleDOI
19 Jun 2019-Joule
TL;DR: In this paper, 1,3,7-trimethylxanthine, a commodity chemical with two conjugated carboxyl groups better known by its common name caffeine, improves the performance and thermal stability of perovskite solar cells.

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TL;DR: In this paper, a twenty-micrometer-thick single-crystal methylammonium lead triiodide perovskite (MAPbI3) was grown on a charge-selective contact using a solution space-limited inverse-temperatur.
Abstract: Twenty-micrometer-thick single-crystal methylammonium lead triiodide (MAPbI3) perovskite (as an absorber layer) grown on a charge-selective contact using a solution space-limited inverse-temperatur...

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TL;DR: The focus herein is on the recombination at perovskite/electron-transporting material and perovSkite/hole-transport material interfaces in normal or inverted PSCs.
Abstract: Organic-inorganic hybrid perovskite materials are receiving increasing attention and becoming star materials on account of their unique and intriguing optical and electrical properties, such as high molar extinction coefficient, wide absorption spectrum, low excitonic binding energy, ambipolar carrier transport property, long carrier diffusion length, and high defects tolerance. Although a high power conversion efficiency (PCE) of up to 22.7% is certified for perovskite solar cells (PSCs), it is still far from the theoretical Shockley-Queisser limit efficiency (30.5%). Obviously, trap-assisted nonradiative (also called Shockley-Read-Hall, SRH) recombination in perovskite films and interface recombination should be mainly responsible for the above efficiency distance. Here, recent research advancements in suppressing bulk SRH recombination and interface recombination are systematically investigated. For reducing SRH recombination in the films, engineering perovskite composition, additives, dimensionality, grain orientation, nonstoichiometric approach, precursor solution, and post-treatment are explored. The focus herein is on the recombination at perovskite/electron-transporting material and perovskite/hole-transporting material interfaces in normal or inverted PSCs. Strategies for suppressing bulk and interface recombination are described. Additionally, the effect of trap-assisted nonradiative recombination on hysteresis and stability of PSCs is discussed. Finally, possible solutions and reasonable prospects for suppressing recombination losses are presented.