
Ligang Yuan
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[ASAP] Materials and Methods for Interface Engineering toward Stable and Efficient Perovskite Solar Cells
Synergistically Improved Molecular Doping and Carrier Mobility by Copolymerization of Donor–Acceptor and Donor–Donor Building Blocks for Thermoelectric Application
A new strategy for synergistically improving molecular doping and carrier mobility is proposed by copolymerizing donor–acceptor type and donor–donor type building blocks along polymer backbone. The copolymers show significantly improved mobilities of 1–2 cm2 V−1 s−1 at a high doping level while the structural disorder endows a high Seebeck coefficient, indicating a great potential of random copolymer for thermoelectric application.
Abstract
In this work, it is demonstrated that random copolymerization is a simple but effective strategy to obtain new conductive copolymers as high‐performance thermoelectric materials. By using a polymerizing acceptor unit diketopyrropyrrole with donor units thienothiophene and oligo ethylene glycol substituted bithiophene (g32T), it is found that strong interchain donor–acceptor interactions ensure good film crystallinity for charge transport, while donor–donor type building blocks contribute to effective charge transfers. Hall effect measurements show that the high electrical conductivity results from increased free carriers with simultaneously improved mobility reaching over 1 cm2 V−1 s−1. The synergistic effect of improved molecular doping and carrier mobility, as well as a high Seebeck coefficient ascribed to the structural disorder along polymer chains via random copolymerization, results in an impressive power factor up to 110 µW K−2 m−1 which is 10 times higher than that of solution‐processed polythiophenes.
ZnO–Ti3C2 MXene Electron Transport Layer for High External Quantum Efficiency Perovskite Nanocrystal Light‐Emitting Diodes
Adding an appropriate amount of Ti3C2 into the ZnO electron transport layer (ETL) to change the energy level structure and electron mobility of the ETL and further make the carrier transport balanced is explored. The ZnO/TiC ETL‐based red emitting perovskite nanocrystals light‐emitting diodes exhibit an external quantum efficiency of 17.4%.
Abstract
2D transition metal carbides, nitrides, and carbonitrides called MXenes show outstanding performance in many applications due to their superior physical and chemical properties. Herein, a ZnO–MXene mixture with different contents of Ti3C2 is applied as electron transport layers (ETLs) and the influence of the Ti3C2 MXene in all‐inorganic metal halide perovskite nanocrystal light‐emitting diodes (perovskite NC LEDs) is explored. The addition of Ti3C2 makes more balanced charge carrier transport in LEDs by changing the energy level structure and electron mobility of ETL. Moreover, lower surface roughness is obtained for the ETL, thus guaranteeing uniform distribution of the perovskite NCs layer and further reducing leakage current. As a result, a 17.4% external quantum efficiency (EQE) with low efficiency roll‐off is achieved with 10% Ti3C2, which is a 22.5% improvement compared to LEDs without Ti3C2.
[ASAP] Co-Evaporated p-i-n Perovskite Solar Cells beyond 20% Efficiency: Impact of Substrate Temperature and Hole-Transport Layer

Efficient and stable perovskite solar cell with suppressed defects by employing lead indicator—dithizone
The defect in perovskite film is one of the most non‐negligible factors that can attenuate the performances of perovskite solar cell. This work fabricates defects‐reduced perovskite film by using the lead indicator (dithizone) as an additive of perovskite functional layer. The dithizone can retard the crystallization rate of perovskite films, passivate the defects, and enhance the structure stability of perovskite by coordinating with lead atoms. As a result, the device doped with dithizone yields outstanding power conversion efficiency and stability.
Full Defects Passivation Enables 21% Efficiency Perovskite Solar Cells Operating in Air
A full defects passivation strategy for superior carrier dynamics is demonstrated, which enables highly efficient perovskite solar cells operating in air.
Abstract
The lattice defects in the bulk and on the surface of the halide perovskite layer serve as trap sites and recombination centers to annihilate photogenerated carriers, determining the performance and stability of perovskite optoelectronic devices. Herein, the previously reported surface defects passivation engineering is extended to a full defects passivation strategy through stereoscopically introducing the cysteamine hydrochloride (CSA‐Cl) in the bulk and on the surface of perovskites. First‐principle density functional theory (DFT) calculations are employed to theoretically verify the multiple defects passivation effect of the CAS‐Cl on the perovskite. The perovskite layer with full defects passivation exhibits superior carrier dynamics as revealed by femtosecond transient absorption due to the reduced defect density determined by a highly sensitive photothermal deflection spectroscopy technique. Consequently, a high efficiency approaching 21% is achieved for the inverted planar perovskite solar cells (PVSCs). More importantly, the CAS‐Cl passivated PVSCs exhibit operation in air, which will be beneficial for the in situ device test for understanding the photophysics involved. This work provides a promising strategy to reduce the defects in both the perovskite bulk and surface for superior optoelectronic properties, facilitating the development of highly efficient and stable PVSCs and other optoelectronic devices.
Revealing the A‐Site Effect of Lead‐Free A3Sb2Br9 Perovskite in Photocatalytic C(sp3)−H Bond Activation
A3Sb2Br9 nanoparticles (NPs) with different ratios of Cs and CH3NH3 (MA) were employed in photocatalytic C(sp3)−H bond activation with high conversion rates. It was demonstrated that the octahedron distortion by A‐site cations could affect the electronic properties of A3Sb2Br9 and further influence the photocatalytic activities.
Abstract
The lead‐free halide perovskite A3Sb2Br9 is utilized as a photocatalyst for the first time for C(sp3)−H bond activation. A3Sb2Br9 nanoparticles (A3Sb2Br9 NPs) with different ratios of Cs and CH3NH3 (MA) show different photocatalytic activities for toluene oxidation and the photocatalytic performance is enhanced when increasing the amount of Cs. The octahedron distortion caused by A‐site cations can change the electronic properties of X‐site ions and further affect the electron transfer from toluene molecules to Br sites. After the regulation of A‐site cations, the photocatalytic activity is higher with A3Sb2Br9 NPs than that with classic photocatalysts (TiO2, WO3, and CdS). The main active species involved in photocatalytic oxidation of toluene are photogenerated holes (h+) and superoxide anions (.O2 −). The octahedron distortion by A‐site cations affecting photocatalytic activity remains unique and is also a step forward for understanding more about halide‐perovskite‐based photocatalysis. The relationship between octahedron distortion and photocatalysis can also guide the design of new photocatalytic systems involving other halide perovskites.
Perovskite and Organic Solar Cells on a Rocket Flight
Publication date: 16 September 2020
Source: Joule, Volume 4, Issue 9
Author(s): Lennart K. Reb, Michael Böhmer, Benjamin Predeschly, Sebastian Grott, Christian L. Weindl, Goran I. Ivandekic, Renjun Guo, Christoph Dreißigacker, Roman Gernhäuser, Andreas Meyer, Peter Müller-Buschbaum
Compositional Engineering of Chloride Ion‐Doped CsPbBr3 Halides for Highly Efficient and Stable All‐Inorganic Perovskite Solar Cells
A large‐grained CsPbBr3 perovskite film with improved energy‐level alignment and hole mobility is fabricated by compositional engineering of Cl ion doping, which suppresses charge recombination thus affording a champion power conversion efficiency (PCE) as high as 9.73% for carbon‐based all‐inorganic CsPbBr2.98Cl0.02 PSC free of encapsulation with excellent operational stability.
Carbon‐based CsPbBr3 perovskite solar cells (PSCs) without hole‐transporting layers (HTLs) have aroused extensive attention due to their low manufacturing cost and prominent ambient stability. However, the defects of perovskite film and the poor charge extraction within PSCs result in severe charge recombination, which restricts the further enhancement of device efficiency. In view of this critical point, a compositional engineering of CsPbBr3 perovskite via doping with Cl− ions is presented herein to decrease the trap states and enhance the charge extraction. It is revealed that the doping of Cl− ions not only enlarges the grain size and thereby reduces the trap‐state density, but also optimizes the energy‐level alignment and improves the hole mobility of the perovskite film, leading to an evidently suppressed charge recombination and improved charge extraction and transportation. As a result, a champion power conversion efficiency (PCE) of 9.73% is achieved for carbon‐based HTL‐free CsPbBr2.98Cl0.02 PSC, yielding a marked enhancement in comparison with 6.69% efficiency for the control. Meanwhile, the thermal and moisture stabilities of unencapsulated CsPbBr2.98Cl0.02 PSC are improved, maintaining 93% and 95% of the initial PCE after expose to air atmosphere with 80% relative humidity (RH) and at 80 °C over 60 days, respectively.
Effect of Additives AX (A = FA, MA, Cs, Rb, NH4, X = Cl, Br, I) in FAPbI3 on Photovoltaic Parameters of Perovskite Solar Cells
Studies on effect of additives of FAX (X = Cl, Br, and I, FA = formamidinium) and ACl (A = MA, Cs, Rb, and NH4) in FAPbI3‐based perovskite solar cells reveal that the FACl additive shows best performance over other additives due to passivating the grain boundary effectively without altering bandgap of pristine perovskite.
Herein, the dependence of photovoltaic performance on the additives of FAX (X = Cl, Br, and I, FA = formamidinium) and ACl [A = methylammonium (MA), Cs, Rb, and NH4] in FAPbI3‐based perovskite solar cells (PSCs) is reported. Effect of concentration on photovoltaic parameters is first screened for each additive, from which optimal concentration is determined with respect to the pristine without additive. Power conversion efficiency (PCE) is significantly improved from 16.55% to 22.51% after adding 20 mol% FACl in the perovskite precursor solution, whereas moderate increase in PCE to 20.08% and 19.97% is observed for FABr and FAI, respectively, indicating an important role of chloride. MACl and CsCl improved PCE to 20.81% and 20.59%, respectively, which is, however, inferior to FACl. A significantly increased carrier lifetime by treating FACl is responsible for the best performance. Energy dispersive X‐ray spectroscopy shows that chloride in the additive FACl is not incorporated in grain but placed on the grain boundary, which plays an important role in passivating iodide‐deficient grain boundary. The FACl additive has benefits over other additives because it cannot change the bandgap of FAPbI3.
The Stabilization of Formamidinium Lead Tri‐Iodide Perovskite through a Methylammonium‐Based Additive for High‐Efficiency Solar Cells
A methylammonium chloride (MACl) additive is used to synthesize FA1–x MA x PbI3 films. The best molar fraction of this additive is determined. The MA content in thin films actually used in solar cells is x = 0.06. This amount is thermodynamically the best for the stabilization of this highly efficient perovskite. The perovskite solar cell achieves a stabilized power conversion efficiency as high as 22.06%.
Nowadays, complex chemistry and precursor solution compositions are developed to stabilize hybrid perovskite films and boost the efficiency of perovskite solar cells (PSCs). In this context, determining the actual composition of these layers, especially in organic cations, and understanding the chemistry behind is challenging. Herein, the introduction of methylammonium (MA+) in formamidinium lead iodide (FAPbI3) 3D perovskite is considered to stabilize the α‐phase, whose quantity must be minimized to reduce the material hydrophilicity and its possible destabilization by degassing. The key effects of methylammonium chloride (MACl) additive on the growth of FA1–x MA x PbI3 perovskite layers are studied. Liquid nuclear magnetic resonance (NMR) is used to analyze the photovoltaic layers. NMR peaks and their origin are identified. The MA and FA content in films actually used in PSCs is reliably measured and prepared over a large additive molar concentration ratio. x is quantified at 0.06 ± 0.01 for pure films, which corresponds to the best entropic compound stabilization. It results in PSCs with a stabilized power conversion efficiency as high as 22.06%. These PSCs are shown to be highly stable under solar irradiation and high moisture.
Enhanced Charge Transfer in Atom‐Thick 2H–WS2 Nanosheets’ Electron Transport Layers of Perovskite Solar Cells
Atom‐thick 2D WS2 nanosheets’ electron‐transport layers (ETLs) facilitate enhanced coupling with the perovskite absorber layer, promoting a highly active interfacial charge transfer dynamic. The single‐crystalline nature of the WS2 ETL also provides the facile transportation of photogenerated electrons to the electrode for a high‐performance and high‐stability perovskite solar cell.
The structure and the electronic properties of the electron‐transport layer (ETL) of perovskite solar cells (PSCs) govern the interfacial charge transfer and charge transportation to the electrode. The ETLs of two dimensions, that are atom thick, and have a planar structure that possesses special electronic properties, such as the surface collective motion of excitons or charge transfer–driven defect state relief, that is 2D transition metal dichalcogenide, allow a highly energetic carrier dynamic process for enhanced photovoltaic effect. Herein, it is discovered that planar, few‐atom‐thick 2H–WS2 nanosheets' ETLs drive ultrafast charge transfer and transportation along the ETL during the photovoltaic process. Time‐resolved photoluminescence and electrochemical impedance spectroscopy analysis results indicate that the charge transfer from the perovskite to the ETL occurs as fast as 5.9 ns with charge transfer resistance as low as 25.6 Ω. This allows the PSC device to produce a power conversion efficiency of 18.21% with short‐circuit current density, open‐circuit voltage, and fill factor as high as 22.24 mA cm2, 1.12 V, and 0.731, respectively. The PSC retains 96.87% of its performance when being aged in nitrogen atmosphere for 33 days. Atom‐thick planar WS2 ETL nanosheets can be the basis for the development of high‐performance PSC devices.
Numerical Analysis of Pb‐Free Perovskite Absorber Materials: Prospects and Challenges
Pb and Pb‐free perovskite absorbers are analyzed using a 1D simulator for n‐i‐p devices. SCAPS‐1D simulations suggest: 1) theoretically determined efficiency limit of Cs2PtI6 perovskites is comparable with (FA,MA,Cs)Pb(I,Br)3, 2) FA4GeSbCl12 is a promising photoabsorber; and 3) for efficient photoconversion with Sn‐, Ge‐, Ti‐, or Ag‐based perovskite absorbers, reduction in defect density and increase in absorption coefficient is needed.
Optoelectronic properties of organic–inorganic halide perovskites are exceptional with solar cells showing efficiency comparable with conventional photovoltaic technologies. However, with issues of material stability and toxicity of Pb, it is important to understand if Pb can be replaced while maintaining the high power conversion efficiencies of (FA,MA,Cs)Pb(I,Br)3. Herein, practical efficiency limits of Pb and Pb‐free perovskite absorbers are analyzed using a 1D simulator for n‐i‐p or p‐i‐n device structures. SCAPS‐1D baseline models for perovskite absorber materials with and without Pb are developed to numerically reproduce the experimental current density–voltage (JV) and external quantum efficiency (EQE) of champion devices from literature. From these baseline models, the efficiency limits are determined based on optimizing the interface band alignments, reduction in midgap defect density, increased absorption coefficient, and no parasitic losses. SCAPS‐1D simulations suggest that 1) theoretically determined efficiency limit of Cs2PtI6 perovskites is comparable with (FA,MA,Cs)Pb(I,Br)3 perovskites, 2) FA4GeSbCl12 is a promising photoabsorber; and 3) for efficient photoconversion with Sn‐, Ge‐, Ti‐, or Ag‐based compounds, a reduction of defect density and increase in absorption coefficient is needed.
[ASAP] The Possible Side Reaction in the Annealing Process of Perovskite Layers

Toward All Slot‐Die Fabricated High Efficiency Large Area Perovskite Solar Cell Using Rapid Near Infrared Heating in Ambient Air
An industry compatible slot‐die coating process combined with near‐infrared irradiation heating enables rapid manufacture of large‐area and uniform perovskite solar cells in air. The highest power conversion efficiency for a device, which is fabricated using the slot‐die coated four layer, is nearly 11%.
Abstract
Currently, high‐efficiency perovskite solar cells are mainly fabricated by the spin‐coating process, which limits the possibility of commercial mass‐production of perovskite solar cells. In this work, the slot‐die coating process is combined with near‐infrared irradiation heating to quickly manufacture perovskite solar cells in air. The composition of the perovskite precursor solution is tuned by adding n‐butanol, with its low boiling point and low surface tension, to increase the near‐infrared energy absorption, facilitate the evaporation of the solvent system and film formation, and accelerate the crystallization of perovskite. High‐quality uniform perovskite film can be prepared within 18 s. Moreover, the all slot‐die coating process is demonstrated to prepare over an area of 12 cm × 12 cm, four layers of uniform film overlay on top of each other for the devices except electrode in ambient air. A power conversion efficiency of ≈11% is achieved when this all slot‐die coated film is used to fabricate device. This facile process can greatly reduce the cost, time and bypass post‐annealing to fabricate high‐efficiency large‐area perovskite solar cells in ambient air.
Self-Elimination of Intrinsic Defects Improves the Low-Temperature Performance of Perovskite Photovoltaics
Publication date: 16 September 2020
Source: Joule, Volume 4, Issue 9
Author(s): Yihua Chen, Shunquan Tan, Nengxu Li, Bolong Huang, Xiuxiu Niu, Liang Li, Mingzi Sun, Yu Zhang, Xiao Zhang, Cheng Zhu, Ning Yang, Huachao Zai, Yiliang Wu, Sai Ma, Yang Bai, Qi Chen, Fei Xiao, Kangwen Sun, Huanping Zhou
[ASAP] Enhanced Efficiency of Air-Stable CsPbBr3 Perovskite Solar Cells by Defect Dual Passivation and Grain Size Enlargement with a Multifunctional Additive

Laser‐Generated Supranano Liquid Metal as Efficient Electron Mediator in Hybrid Perovskite Solar Cells
The technology of pulsed laser irradiation in liquid from a solid target to liquid is pioneered, yielding liquid ternary supranano‐(<10 nm) alloys with a unique core–shell structure. The decoration of such supranano‐alloys as an electron mediator at grain boundaries promotes the electron extraction and transfer of the hybrid perovskite film of a perovskite solar cell and drives the efficiency up to 22.03%.
Abstract
Creating colloids of liquid metal with tailored dimensions has been of technical significance in nano‐electronics while a challenge remains for generating supranano (<10 nm) liquid metal to unravel the mystery of their unconventional functionalities. Present study pioneers the technology of pulsed laser irradiation in liquid from a solid target to liquid, and yields liquid ternary nano‐alloys that are laborious to obtain via wet‐chemistry synthesis. Herein, the significant role of the supranano liquid metal on mediating the electrons at the grain boundaries of perovskite films, which are of significance to influence the carriers recombination and hysteresis in perovskite solar cells, is revealed. Such embedding of supranano liquid metal in perovskite films leads to a cesium‐based ternary perovskite solar cell with stabilized power output of 21.32% at maximum power point tracing. This study can pave a new way of synthesizing multinary supranano alloys for advanced optoelectronic applications.
Low‐Temperature Crystallization of CsPbIBr2 Perovskite for High Performance Solar Cells
A low‐temperature crystallization strategy of CsPbIBr2 perovskite solar cells is reported. The additive n‐butylammonium iodide (BAI) is incorporated into the perovskite precursor to improve crystallinity, optimize morphology, and passivate defects at 160 °C. As a result, a high‐level PCE of 10.78% with a high open‐circuit voltage (V OC) of 1.25 V is achieved.
Inorganic cesium lead halide perovskite solar cells (PSCs) have been widely explored due to their outstanding thermal stability and photovoltaic performance. However, the application and development of CsPbIBr2‐based PSCs is still hindered by major challenges such as high fabrication temperature and large voltage loss. To address these difficulties, additive engineering is conducted using n‐butylammonium iodide (BAI). It is found that it not only improves the crystallization and morphology of perovskite layers but also substantially decreases the annealing temperature. In addition, the BAI incorporation decreases trap state density and restrains nonradiative recombination. As such, a high power conversion efficiency (PCE) of 10.78% is achieved, 21% higher compared with that of the control sample (8.88%). It should be noted that this is particularly high for the CsPbIBr2 PSCs fabricated at low temperatures (<200 °C) that are required for flexible devices based on polymeric substrates.
Hydrolyzable Hydrophobic Molecules: Double Barriers for Moisture Degradation: Assembly of Hydrolysable Hydrophobic Molecules for Stable Perovskite Solar Cells with High Open‐Circuit Voltage (Adv. Funct. Mater. 28/2020)
In article number https://doi.org/10.1002/adfm.2020026392002639, Liang Li, Hongqiang Wang, and co‐workers demonstrate a double‐barrier strategy that not only blocks the invasion of moisture but also employs the permeated moisture to increase the moisture durability of perovskite films, which results in an n–i–p perovskite solar cell with moisture stability over 115 days (relative humidity of 70%) and a champion efficiency up to 21.34%.
Defect Passivation in Perovskite Solar Cells by Cyano‐Based π‐Conjugated Molecules for Improved Performance and Stability
Cyano‐based π‐conjugated molecules composed of indacenodithieno[3,2‐b]thiophene (IDTT) and the cyano group are used to passivate defects at the surface and grain boundaries of metal–halide perovskite films. These molecules are self‐anchored at the grain boundaries due to their strong binding to undercoordinated Pb2+ and enhance the power conversion efficiencies up to 21.2%, with improved stability of the perosvkite solar cells.
Abstract
Defects at the surface and grain boundaries of metal–halide perovskite films lead to performance losses of perovskite solar cells (PSCs). Here, organic cyano‐based π‐conjugated molecules composed of indacenodithieno[3,2‐b]thiophene (IDTT) are reported and it is found that their cyano group can effectively passivate such defects. To achieve a homogeneous distribution, these molecules are dissolved in the antisolvent, used to initiate the perovskite crystallization. It is found that these molecules are self‐anchored at the grain boundaries due to their strong binding to undercoordinated Pb2+. On a device level, this passivation scheme enhances the charge separation and transport at the grain boundaries due to the well‐matched energetic levels between the passivant and the perovskite. Consequently, these benefits contribute directly to the achievement of power conversion efficiencies as high as 21.2%, as well as the improved environmental and thermal stability of the PSCs. The surface treatment provides a new strategy to simultaneously passivate defects and enhance charge extraction/transport at the device interface by manipulating the anchoring groups of the molecules.
Overcoming Redox Reactions at Perovskite-Nickel Oxide Interfaces to Boost Voltages in Perovskite Solar Cells
Publication date: 19 August 2020
Source: Joule, Volume 4, Issue 8
Author(s): Caleb C. Boyd, R. Clayton Shallcross, Taylor Moot, Ross Kerner, Luca Bertoluzzi, Arthur Onno, Shalinee Kavadiya, Cullen Chosy, Eli J. Wolf, Jérémie Werner, James A. Raiford, Camila de Paula, Axel F. Palmstrom, Zhengshan J. Yu, Joseph J. Berry, Stacey F. Bent, Zachary C. Holman, Joseph M. Luther, Erin L. Ratcliff, Neal R. Armstrong
Pressure‐Suppressed Carrier Trapping Leads to Enhanced Emission in Two‐Dimensional Perovskite (HA)2(GA)Pb2I7
A remarkably enhanced emission (by 12‐fold) is achieved using pressure to modulate the structure of a highly distorted 2D halide perovskite (HA)2(GA)Pb2I7. In situ structural, spectroscopic, and theoretical analyses reveal that lattice compression under a mild pressure within 1.6 GPa considerably suppresses the carrier trapping, leading to the significantly improved performance.
Abstract
A remarkable PL enhancement by 12 fold is achieved using pressure to modulate the structure of a recently developed 2D perovskite (HA)2(GA)Pb2I7 (HA=n‐hexylammonium, GA=guanidinium). This structure features a previously unattainable, extremely large cage. In situ structural, spectroscopic, and theoretical analyses reveal that lattice compression under a mild pressure within 1.6 GPa considerably suppresses the carrier trapping, leading to significantly enhanced emission. Further pressurization induces a non‐luminescent amorphous yellow phase, which is retained and exhibits a continuously increasing band gap during decompression. When the pressure is released to 1.5 GPa, emission can be triggered by above‐band gap laser irradiation, accompanied by a color change from yellow to orange. The obtained orange phase could be retained at ambient conditions and exhibits two‐fold higher PL emission compared with the pristine (HA)2(GA)Pb2I7.
[ASAP] Rapid Vapor-Phase Deposition of High-Mobility p-Type Buffer Layers on Perovskite Photovoltaics for Efficient Semitransparent Devices

Aryl Diammonium Iodide Passivation for Efficient and Stable Hybrid Organ‐Inorganic Perovskite Solar Cells
An aryl diammonium iodide: PDMAI is demonstrated first to be highly promising to enhance open‐circuit voltage, short‐circuit current, and stability of FAMAPbI3 based perovskite solar cells through surface passivation. Theoretical calculation suggests a stronger energy binding between PDMAI and perovskite surface. This work provides a new passivation strategy for efficient and stable perovskite solar cells.
Abstract
Surface passivation is increasingly one of the most prominent strategies to promote the efficiency and stability of perovskite solar cells (PSCs). However, most passivation molecules hinder carrier extraction due to poorly conductive aggregation between perovskite surface and carrier transportation layer. Herein, a novel molecule: p‐phenyl dimethylammonium iodide (PDMAI) with ammonium group on both terminals is introduced, and its passivation effect is systematically investigated. It is found that PDMAI can mitigate defects at the surface and promote carrier extraction from perovskite to the hole transporting layer, leading to a lift of open‐circuit voltage of 40 mV. Profiting from superior PDMAI passivation, the average efficiency of PSCs has been elevated from 19.69% to 20.99%. As demonstrated with density functional theory calculations, PDMAI probably tends to anchor onto the perovskite surface with both NH3I tails, and enhances the adhesion and contact to perovskite layer. The exposed hydrophobic aryl core protects perovskite against detrimental environmental factors. In addition, the alkyl component between aryl and ammonium groups is demonstrated to be essentially vital in triggering passivation function, which offers the guidance for the design of passivation molecules.
In Situ Grazing‐Incidence Wide‐Angle Scattering Reveals Mechanisms for Phase Distribution and Disorientation in 2D Halide Perovskite Films
The mechanism of 2D halide perovskite film formation is resolved using in situ grazing‐incidence wide‐angle scattering (GIWAXS). The film begins as a sol–gel precursor before first forming a 3D MAPbI3‐like phase at the air/liquid interface. This acts as a template for the highly textured 2D phase with the layers perpendicular to the substrate, which grows closer to the substrate.
Abstract
2D hybrid halide perovskites with the formula (A′)2(A) n ‐1Pb n I3 n +1 have remarkable stability and promising efficiency in photovoltaic and optoelectronic devices, yet fundamental understanding of film formation, key to optimizing these devices, is lacking. Here, in situ grazing‐incidence wide‐angle X‐ray scattering (GIWAXS) is used to monitor film formation during spin‐coating. This elucidates the general film formation mechanism of 2D halide perovskites during one‐step spin‐coating. There are three stages of film formation: sol–gel, oriented 3D, and 2D. Three precursor phases form during the sol–gel stage and transform to perovskite, first giving a highly oriented 3D‐like phase at the air/liquid interface followed by subsequent nucleations forming slightly less oriented 2D perovskite. Furthermore, heating before crystallization leads to fewer nucleations and faster removal of the precursors, improving orientation. This outlines the primary causes of phase distribution and perpendicular orientation in 2D perovskite films and paves the way for rationally designed film fabrication techniques.
[ASAP] Incorporation of Vanadium(V) Oxide in Hybrid Hole Transport Layer Enables Long-term Operational Stability of Perovskite Solar Cells

The Synergism of DMSO and Diethyl Ether for Highly Reproducible and Efficient MA0.5FA0.5PbI3 Perovskite Solar Cells
By using a solvent‐mediated phase transformation process, a record certified 21.8% power conversion efficiency in pure‐iodide, alkaline‐metal‐free MA0.5FA0.5PbI3 perovskite‐based solar cells is achieved.
Abstract
Composition and film quality of perovskite are crucial for the further improvement of perovskite solar cells (PSCs), including efficiency, reproducibility, and stability. Here, it is demonstrated that by simply mixing 50% of formamidinium (FA+) into methylammonium lead iodide (MAPbI3), a highly crystalline, stable phase, and compact, polycrystalline grain morphology perovskite is formed by using a solvent‐mediated phase transformation process via the synergism of dimethyl sulfoxide and diethyl ether, which shows long carrier lifetime, low trap state density, and a record certified 21.8% power conversion efficiency (PCE) in pure‐iodide, alkaline‐metal‐free MA0.5FA0.5PbI3 perovskite‐based PSCs. These PSCs show very high operational stability, with 85% PCE retention upon 1000 h 1 Sun intensity illumination. A 17.33% PCE module (6.5 × 7 cm2) is also demonstrated, attesting to the scalability of such devices.
[ASAP] Hybrid 2D [Pb(CH3NH2)I2]n Coordination Polymer Precursor for Scalable Perovskite Deposition

Bifacial passivation towards efficient FAPbBr3-based inverted perovskite light-emitting diodes
DOI: 10.1039/D0NR02323J, Paper
PeLEDs with bifacial passivation give a maximum EQE of 9.0%, which is the highest efficiency for FAPbBr3-based inverted PeLEDs.
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