Enhanced charge carrier transport and defects mitigation of passivation layer for efficient perovskite solar cells.

Surface passivation has been developed as an effective strategy to reduce trap-state density and suppress non-radiation recombination process in perovskite solar cells. However, passivation agents usually own poor conductivity and hold negative impact on the charge carrier transport in device. Here, we report a binary and synergistical post-treatment method by blending 4-tert-butyl-benzylammonium iodide with phenylpropylammonium iodide and spin-coating on perovskite surface to form passivation layer. The binary and synergistical post-treated films show enhanced crystallinity and improved molecular packing as well as better energy band alignment, benefiting for the hole extraction and transfer. Moreover, the surface defects are further passivated compared with unary passivation. Based on the strategy, a record-certified quasi-steady power conversion efficiency of 26.0% perovskite solar cells is achieved. The devices could maintain 81% of initial efficiency after 450 h maximum power point tracking.

Efficient and stable perovskite mini-module via high-quality homogeneous perovskite crystallization and improved interconnect.

The efficiency and stability of perovskite module devices are mainly limited by the quality of scalable perovskite films and sub-cells' lateral contact. Here, firstly, we report constant low temperature substrate to regulate the growth of perovskite intermediate films to slow down the crystallization for obtaining high-quality homogeneous perovskite films in large scale size, which avoid the effect of the ambient temperature on the film quality. Secondly, a scribing step named P1.5 was added before the top function layers deposition, the diffusion barrier layer can be formed "naturally" at the interconnection interface without introducing any additional materials, which well alleviates the diffusion degradation process. As a result, our inverted perovskite devices exhibit a very small efficiency loss with area expansion comparable to other photovoltaic devices (for example, Cadmium Telluride), the perovskite module (aperture area 14.61 cm2) shows a certified quasi-steady-state power conversion efficiency of 22.73%, and the module maintaining over 90% of its initial efficiency after 1000 hours of continuous operation under illumination.

Efficient pure-red perovskite light-emitting diodes with strong passivation via ultrasmall-sized molecules.

Perovskite light-emitting diodes (PeLEDs) have attracted great attention in recent years; however, the halogen vacancy defects in perovskite notably hamper the development of high-efficiency devices. Previously, large-sized passivation agents have been usually used, while the effect of defect passivation is limited due to the weak bonding or the large space steric hindrance. Here, we predict that the ultrasmall-sized formate (Fa) and acetate (Ac) have more efficient passivation ability because of the stronger binding with the perovskite, as demonstrated by density functional theory calculation. We introduce ultrasmall-sized cesium salts (CsFa/CsAc) into buried interface, which can also diffuse into the bulk, resulting in both buried interface and bulk passivation. In addition, the improved perovskite growth has been found due to the enhanced hydrophily after introducing CsFa/CsAc as additive. According to these advantages, a pure-red PeLED with 24.2% efficiency at 639 nm has been achieved.

Homogenized NiOx nanoparticles for improved hole transport in inverted perovskite solar cells.

The power conversion efficiency (PCE) of inverted perovskite solar cells (PSCs) is still lagging behind that of conventional PSCs, in part because of inefficient carrier transport and poor morphology of hole transport layers (HTLs). We optimized self-assembly of [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) onto nickel oxide (NiOx) nanoparticles as an HTL through treatment with hydrogen peroxide, which created a more uniform dispersion of nanoparticles with high conductivity attributed to the formation of Ni3+ as well as surface hydroxyl groups for bonding. A 25.2% certified PCE for a mask size of 0.074 square centimeters was obtained. This device maintained 85.4% of the initial PCE after 1000 hours of stabilized power output operation under 1 sun light irradiation at about 50°C and 85.1% of the initial PCE after 500 hours of accelerated aging at 85°C. We obtained a PCE of 21.0% for a minimodule with an aperture area of 14.65 square centimeters.

High-Efficiency Pure-Red Perovskite Quantum-Dot Light-Emitting Diodes.

It is still challenging to achieve high-efficiency pure-red (620-650 nm wavelength) perovskite light-emitting diodes (PeLEDs). Herein, we report pure-red PeLEDs with Commission Internationale de l'Eclairage coordinates (0.703, 0.297) meeting the Rec. 2020, an external quantum efficiency of 20.8%, and a luminance of 3775 cd/m2. This design is based on the strong quantum confinement CsPbI3 quantum dots (QDs) capped by composite ligands of 3-phenyl-1-propylamine and tetrabutylammonium iodide. This strategy stabilized the structure of the strong-confined QDs and reduced the influence of the electric field-induced Stark effect on the PeLEDs. Furthermore, the exciton binding energy of the QDs was decreased by the composited ligands to suppress Auger recombination within the devices. Additionally, the valence-band maximum of the QDs was lifted to match the hole-transport layer, thus balancing charge injection in the PeLEDs. Our device also demonstrated a stable electroluminescence spectrum and a lifetime of 5.6 times longer than the control device.

Red Perovskite Light-Emitting Diodes with Efficiency Exceeding 25% Realized by Co-Spacer Cations.

Perovskite light-emitting diodes (PeLEDs) have received great attention in recent years due to their narrow emission bandwidth and tunable emission spectrum. Efficient red emission is one of most important parts for lighting and displays. Quasi-2D perovskites can deliver high emission efficiency due to the strong carrier confinement, while the external quantum efficiencies (EQE) of red quasi-2D PeLEDs are inefficient at present, which is due to the complex distribution of different n-value phases in quasi-2D perovskite films. In this work, the phase distribution of the quasi-2D perovskite is finely controlled by mixing two different large organic cations, which effectively reduces the amount of smaller n-index phases, meanwhile the passivation of lead and halide defects in perovskite films is realized. Accordingly, the PeLEDs show 25.8% EQE and 1300 cd m-2 maximum brightness at 680 nm, which exhibits the highest performance for red PeLEDs up to now.

Inactive (PbI2)2RbCl stabilizes perovskite films for efficient solar cells.

In halide perovskite solar cells the formation of secondary-phase excess lead iodide (PbI2) has some positive effects on power conversion efficiency (PCE) but can be detrimental to device stability and lead to large hysteresis effects in voltage sweeps. We converted PbI2 into an inactive (PbI2)2RbCl compound by RbCl doping, which effectively stabilizes the perovskite phase. We obtained a certified PCE of 25.6% for FAPbI3 (FA, formamidinium) perovskite solar cells on the basis of this strategy. Devices retained 96% of their original PCE values after 1000 hours of shelf storage and 80% after 500 hours of thermal stability testing at 85°C.

Broadband Photodetector Based on Inorganic Perovskite CsPbBr3 /GeSn Heterojunction.

Photodetectors with broadband response spectrum have attracted great interest in many application areas such as imaging, gas sensing, and night vision. Here, a high performance broadband photodetector is demonstrated with inorganic perovskite CsPbBr3 /GeSn heterojunction, detection range can be covered from 450 to 2200 nm. The responsivity of heterojunction device can achieve as high as 129 mA W-1 under illuminated light of 532 nm, which is 4.92 times larger than that of a GeSn based device. As the CsPbBr3 can also act as anti-reflective coating for infrared wavelength, the infrared band responsivity at wavelength of 2200 nm can also be raised by 1.42 times. In addition, the device with all inorganic components is showed good stability, while keeping in the dry environment, the device can sustain its 90% original after 550 h storage. These results show the inorganic perovskite/GeSn heterojunction device is of great potential in broadband photodetection with high responsivity.

Perovskite Light-Emitting Diodes with External Quantum Efficiency Exceeding 22% via Small-Molecule Passivation.

Perovskite light-emitting diodes (PeLEDs) are considered as particularly attractive candidates for high-quality lighting and displays, due to possessing the features of wide gamut and real color expression. However, most PeLEDs are made from polycrystalline perovskite films that contain a high concentration of defects, including point and extended imperfections. Reducing and mitigating non-radiative recombination defects in perovskite materials are still crucial prerequisites for achieving high performance in light-emitting applications. Here, ethoxylated trimethylolpropane triacrylate (ETPTA) is introduced as a functional additive dissolved in antisolvent to passivate surface and bulk defects during the spinning process. The ETPTA can effectively decrease the charge trapping states by passivation and/or suppression of defects. Eventually, the perovskite films that are sufficiently passivated by ETPTA make the devices achieve a maximum external quantum efficiency (EQE) of 22.49%. To our knowledge, these are the most efficient green PeLEDs up to now. In addition, a threefold increase in the T50 operational time of the devices was observed, compared to control samples. These findings provide a simple and effective strategy to make highly efficient perovskite polycrystalline films and their optoelectronics devices.

Stabilizing γ-CsPbI3 Perovskite via Phenylethylammonium for Efficient Solar Cells with Open-Circuit Voltage over 1.3 V.

Cesium lead iodide (CsPbI3 ) perovskite has gained great attention due to its potential thermal stability and appropriate bandgap (≈1.73 eV) for tandem cells. However, the moisture-induced thermodynamically unstable phase and large open-circuit voltage (VOC ) deficit and also the low efficiency seriously limit its further development. Herein, long chain phenylethylammonium (PEA) is utilized into CsPbI3 perovskite to stabilize the orthorhombic black perovskite phase (γ-CsPbI3 ) under ambient condition. Furthermore, the moderate lead acetate (Pb(OAc)2 ) is controlled to combine with phenylethylammonium iodide to form the 2D perovskite, which can dramatically suppress the charge recombination in CsPbI3 . Unprecedentedly, the resulted CsPbI3 solar cells achieve a 17% power conversion efficiency with a record VOC of 1.33 V, the VOC deficit is only 0.38 V, which is close to those in organic-inorganic perovskite solar cells (PSCs). Meanwhile, the PEA modified device maintains 94% of its initial efficiency after exceeding 2000 h of storage in the low-humidity controlled environment without encapsulation.

Large cation ethylammonium incorporated perovskite for efficient and spectra stable blue light-emitting diodes.

Perovskite light-emitting diodes (PeLEDs) have showed significant progress in recent years; the external quantum efficiency (EQE) of electroluminescence in green and red regions has exceeded 20%, but the efficiency in blue lags far behind. Here, a large cation CH3CH2NH2+ is added in PEA2(CsPbBr3)2PbBr4 perovskite to decrease the Pb-Br orbit coupling and increase the bandgap for blue emission. X-ray diffraction and nuclear magnetic resonance results confirmed that the EA has successfully replaced Cs+ cations to form PEA2(Cs1-xEAxPbBr3)2PbBr4. This method modulates the photoluminescence from the green region (508 nm) into blue (466 nm), and over 70% photoluminescence quantum yield in blue is obtained. In addition, the emission spectra is stable under light and thermal stress. With configuration of PeLEDs with 60% EABr, as high as 12.1% EQE of sky-blue electroluminescence located at 488 nm has been demonstrated, which will pave the way for the full color display for the PeLEDs.

Deep Ultraviolet Photodetectors Based on Carbon-Doped Two-Dimensional Hexagonal Boron Nitride.

Recently, the deep ultraviolet (DUV) photodetectors fabricated from two-dimensional (2D) hexagonal boron nitride (h-BN) layers have emerged as a hot research topic. However, the existing studies show that the h-BN-based photodetectors have relatively poor performance. In this work, C doping is utilized to modulate the properties of h-BN and improve the performance of the h-BN-based photodetectors. We synthesized the h-BN atomic layers with various C concentrations varying from 0 to 10.2 atom % by ion beam sputtering deposition through controlling the sputtering atmosphere. The h-BN phase remains stable when a small amount of C is incorporated into h-BN, whereas the introduction of a large amount of C impurities leads to the rapidly deteriorated crystallinity of h-BN. Furthermore, the DUV photodetectors based on C-doped h-BN layers were fabricated, and the h-BN-based photodetector with 7.5 atom % C exhibits the best performance with a responsivity of 9.2 mA·W-1, which is significantly higher than that of the intrinsic h-BN device. This work demonstrates that the C doping is a feasible and effective method for improving the performance of h-BN photodetectors.

Polymer hole-transport material improving thermal stability of inorganic perovskite solar cells.

Cesium-based inorganic perovskite solar cells (PSCs) are paid more attention because of their potential thermal stability. However, prevalent salt-doped 2,2',7,7'-tetrakis(N,N-dipmethoxyphenylamine)9,9'-spirobifluorene (Spiro-OMeTAD) as hole-transport materials (HTMs) for a high-efficiency inorganic device has an unfortunate defective thermal stability. In this study, we apply poly (3-hexylthiophene-2,5-diyl) (P3HT) as the HTM and design all-inorganic PSCs with an indium tin oxide (ITO)/SnO2/LiF/CsPbI3-xBrx/P3HT/Au structure. As a result, the CsPbI3-xBrx PSCs achieve an excellent performance of 15.84%. The P3HT HTM-based device exhibits good photo-stability, maintaining ∼80% of their initial power conversion efficiency over 280 h under one Sun irradiation. In addition, they also show better thermal stability compared with the traditional HTM Spiro-OMeTAD.

Cesium Lead Inorganic Solar Cell with Efficiency beyond 18% via Reduced Charge Recombination.

Cesium-based inorganic perovskite solar cells (PSCs) are promising due to their potential for improving device stability. However, the power conversion efficiency of the inorganic PSCs is still low compared with the hybrid PSCs due to the large open-circuit voltage (VOC ) loss possibly caused by charge recombination. The use of an insulated shunt-blocking layer lithium fluoride on electron transport layer SnO2 for better energy level alignment with the conduction band minimum of the CsPbI3- x Brx and also for interface defect passivation is reported. In addition, by incorporating lead chloride in CsPbI3- x Brx precursor, the perovskite film crystallinity is significantly enhanced and the charge recombination in perovksite is suppressed. As a result, optimized CsPbI3- x Brx PSCs with a band gap of 1.77 eV exhibit excellent performance with the best VOC as high as 1.25 V and an efficiency of 18.64%. Meanwhile, a high photostability with a less than 6% efficiency drop is achieved for CsPbI3- x Brx PSCs under continuous 1 sun equivalent illumination over 1000 h.

Compositional Engineering of Mixed-Cation Lead Mixed-Halide Perovskites for High-Performance Photodetectors.

The mixed-cation lead mixed-halide perovskites can combine the advantages of the constituents while avoiding their drawbacks, and they have been widely explored in solar cells. However, there are only few research studies on the mixed-cation lead mixed-halide perovskites for photodetectors. In this work, we fabricate photodetectors based on FA(1-x)CsxPb(BryI(1-y))3 perovskite and reveal the effect of the chemical composition on the crystal phase stability and device performance of mixed-cation mixed-halide perovskite photodetectors. The FA0.7Cs0.3Pb(I0.8Br0.2)3 photodetectors exhibit high specific detectivity, high responsivity, and excellent stability in ambient conditions. Especially, the flexible perovskite photodetectors fabricated on poly(ethylene terephthalate) substrates exhibit extremely high specific detectivity of 2.8 × 1013 Jones, which is the highest value to date for flexible perovskite photodetectors, as well as excellent stability and outstanding flexibility. These results indicate that mixed-cation mixed-halide perovskites are promising to be applied in high-performance photodetectors and other flexible optoelectronic devices.

Effects of Organic Cations on the Structure and Performance of Quasi-Two-Dimensional Perovskite-Based Light-Emitting Diodes.

Quasi-two-dimensional (quasi-2D) perovskites are efficient luminescent materials due to their self-assembled quantum-well structure. We found that the organic cations have a significant effect on the structure and performance of quasi-2D perovskite-based light-emitting diodes (LEDs). Two classic organic cations, formamidinium (FA) and methylammonium (MA), were chosen for investigation. The MA-based quasi-2D perovskite has the largest band-gap n = 1 phase and a photoluminescence quantum yield (PLQY) as high as 85.3%, whereas this n = 1 phase is almost absent in the FA-based quasi-2D perovskite, which shows a moderate PLQY of 73.5%. However, the FA-based perovskite shows a much higher external quantum efficiency (15.4%) than the MA-based perovskite (0.93%) in LEDs. The lower electroluminescence efficiency of the MA-based perovskite could be ascribed to the poor hole injection. These results showed the importance of rational design of the quasi-2D perovskite for efficient LEDs.

Two-dimensional hexagonal boron-carbon-nitrogen atomic layers.

Two-dimensional (2D) hexagonal boron-carbon-nitrogen (h-BCN) atomic layers are expected to possess interesting properties complementary to those of graphene and h-BN, enabling a rich variety of electronic structures, properties and applications. Herein, we demonstrate a novel method to synthesize 2D h-BCN atomic layers with a full range of compositions by ion beam sputtering deposition under a mixed Ar/CH4 atmosphere. The h-BCN layers have been thoroughly characterized by various techniques, aiming at the determination of their structure evolution and properties. We find that homogeneous h-BCN layers consisting of graphene and h-BN nanodomains can be obtained at an appropriate C content, whereas too high or too low C contents result in the segregation of large-sized graphene or h-BN islands. Furthermore, the band gap of h-BCN layers slightly decreases with the increasing C content, while their electric properties can be tuned from insulating to highly conducting. This work provides a novel approach for synthesizing 2D h-BCN atomic layers and paves the way for the development of h-BCN-based devices.

Remote heteroepitaxy of atomic layered hafnium disulfide on sapphire through hexagonal boron nitride.

Two-dimensional (2D) heterostructures have attracted a great deal of attention due to their novel phenomena arising from the complementary properties of their constituent materials, and provide an ideal platform for exploring new fundamental research and realizing technological innovation. Here, for the first time, we report the formation of high quality HfS2/h-BN heterostructures by the remote heteroepitaxy technique, in which the large-area single-crystal HfS2 layers were epitaxially grown on c-plane sapphire through a polycrystalline h-BN layer via chemical vapor deposition. It is found that c-sapphire substrates can penetrate monolayer and bilayer h-BN to remotely handle the epitaxial growth of HfS2. Benefitting from the high crystal quality of HfS2 epilayers and the weak interface scattering of HfS2 on h-BN, the HfS2 photodetectors demonstrate excellent performance with a high on/off ratio exceeding 105, an excellent photoresponsivity up to 0.135 A W-1 and a high detectivity of over 1012 Jones. Furthermore, the HfS2/h-BN heterostructures prepared by the remote epitaxy can be rapidly released and transferred to a substrate of interest, which opens a new pathway for large-area advanced wearable electronics applications.

Author Correction: Solution-processed hybrid perovskite photodetectors with high detectivity.

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