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Nickel oxide (NiOx) is a promising hole-selective contact to produce efficient inverted p-i-n structured perovskite solar cells (PSCs) due to its high carrier mobility and high transparency. However, the light-induced degradation of the NiOx–perovskite heterojunction is the main factor limiting its long-term operational lifetime. In this study, we used the time-resolved mass spectrometry technique to clarify the degradation mechanism of the NiOx-formamidinium–methylammonium iodide perovskite (a common composition for high-performance PSCs) heterojunction under operational conditions, and observed that (1) oxidation of iodide and generation of free protons under 1-sun illumination, (2) formation of volatile hydrogen cyanide, methyliodide, and ammonia at elevated temperatures, and (3) a condensation reaction between the organic components under a high vapor pressure. To eliminate these multi-step photochemical reactions, we constructed an aprotic trimethylsulfonium bromide (TMSBr) buffer layer at the NiOx/perovskite interface, which enables excellent photo-thermal stability, a matched lattice parameter with the perovskite crystal, and robust trap-passivation ability. Inverted PSCs stabilized with the TMSBr buffer layer reached the maximum efficiency of 22.1% and retained 82.8% of the initial value after continuous operation for 2000 hours under AM1.5G light illumination, which translates into a T80 lifetime of 2310 hours that is among the highest operational lifetimes for NiOx-based PSCs.

Practical lithium metal batteries (LMBs) require full and reversible utilization of limited metallic Li anodes at a solid/quasi-solid electrolyte condition. This leads to a challenging issue, i.e., how to create compatible interphases to regulate interfacial ionic transport and protect the reactive metal. Herein, to address this issue, we report a robust cellulose-based composite gel electrolyte (r-CCE) capable of stabilizing ion deposition via compositing bacterial cellulose (BC) skeleton with Li6.4La3Zr1.4Ta0.6O12 (LLZTO) particles. Benefiting from the decoupled segment structure of cellulose and additional ionic channels of LLZTO, r-CCE not only achieves high ionic conductivity (1.68×10−3 S/cm) with a remarkable Li-ion transfer number (∼0.92) and a wide window of electrochemical stability (∼5.3 V), but also helps stabilize the Li anode. Utilizing ultrathin lithium metal anodes (15 μm), ultra-stable symmetric Li/Li cells that are armed with r-CCE demonstrate a highly stable plating/stripping process. Furthermore, a high areal capacity of ∼4.2 mAh/cm2, and 100 cycles with improved stability of the full Li metal batteries with n/p ratio of ∼0.74 are achieved.

Upscalable fabrication of efficient and stable perovskite solar modules is urgently needed for commercialization. Here we introduce methylammonium chloride additives in the co-solvent system of N-methyl-2-pyrrolidone/N,N-dimethylformamide to control the formation of intermediate phases during the growth of formamidinium–caesium lead triiodide perovskite films. We achieve high-quality films upon drying without the use of anti-solvent. By implementing bulk and surface passivation, champion efficiencies of 24.02% for a small-sized solar cell and 20.5% for a 5 cm × 5 cm solar mini-module on an aperture area of 22.4 cm2 (geometric fill factor ∼ 96%) are achieved by spin-coating. The fully blade-coated perovskite solar sub-module demonstrates a champion efficiency of 15.3% on an aperture area of 205 cm2. The solar mini-module exhibits impressive operational stability with a T80 lifetime of over 1,000 h at maximum power point tracking under continuous light illumination.

CsPbCl3 nanocrystals are potential ultrapure emitters. But it is challenging to synthesize CsPbCl3 nanocrystals with sufficient stability, which impedes their application in light-emitting devices. In this work, we report a facile phosphoryl-chemistry-mediated synthesis approach to synthesizing stable CsPbCl3 nanocrystals, in which the phenylphosphonic dichloride (PhPOCl2) precursor is employed. In addition to the high reactivity of the P–Cl bond of PhPOCl2 for providing adequate Cl, the derived P=O with good proton affinity facilitates the formation of a distinct nanocrystal surface with the nonprotonated oleylamine (OLA) ligand. Accordingly, the L-type-ligand-capped CsPbCl3 nanocrystals exhibited not only bright luminance but also good stability that endured repeated purification up to 10 cycles. Based on the stable CsPbCl3 nanocrystals, we achieved violet LEDs with extremely narrow electroluminescence spectra (full width at half-maximum ≈ 10.6 nm).

Metal halide perovskites (MHPs) have become a major topic of research in thin film photovoltaics due to their advantageous optoelectronic properties. These devices typically have the MHP absorber layer sandwiched between two charge selective layers (CSLs). The interfaces between the perovskite layer and these CSLs are potential areas of higher charge recombination. Understanding the nature of these interfaces is key for device improvement. Additionally, non-stoichiometric perovskite films are expected to strongly impact the interfacial properties. In this study, the interface between CH3NH3PbI3 (MAPbI3) and copper phthalocyanine (CuPc), a hole transport layer (HTL), is studied at the atomic scale. We use scanning tunneling microscopy (STM) combined with density functional theory (DFT) predictions to show that CuPc deposited on MAPbX3 (X = I,Br) forms a self-assembled layer consistent with the α-polymorph of CuPc. Additionally, STM images show a distinctly different adsorption orientation for CuPc on non-perovskite domains of the thin film samples. These findings highlight the effect of non-stoichiometric films on the relative orientation at the MHP/HTL interface, which may affect interfacial charge transport in a device. Our work provides an atomic scale view of the MHP/CuPc interface and underscores the importance of understanding interfacial structures and the effect that the film stoichiometry can have on interfacial properties.

Tin dioxide (SnO2) has been demonstrated as one of the promising electron transport layers for high-efficiency perovskite solar cells (PSCs). However, scalable fabrication of SnO2 films with uniform coverage, desirable thickness and a low defect density in perovskite solar modules (PSMs) is still challenging. Here, we report preparation of high-quality large-area SnO2 films by chemical bath deposition (CBD) with the addition of KMnO4. The strong oxidizing nature of KMnO4 promotes the conversion from Sn(II) to Sn(VI), leading to reduced trap defects and a higher carrier mobility of SnO2. In addition, K ions diffuse into the perovskite film resulting in larger grain sizes, passivated grain boundaries, and reduced hysteresis of PSCs. Furthermore, Mn ion doping improves both the crystallinity and the phase stability of the perovskite film. Such a multifunctional interface engineering strategy enabled us to achieve a power conversion efficiency (PCE) of 21.70% with less hysteresis for lab-scale PSCs. Using this method, we also fabricated 5 × 5 and 10 × 10 cm2 PSMs, which showed PCEs of 15.62% and 11.80% (active area PCEs are 17.26% and 13.72%), respectively. For the encapsulated 5 × 5 cm2 PSM, we obtained a T80 operation lifetime (the lifespan during which the solar module PCE drops to 80% of its initial value) exceeding 1000 h in ambient condition.

Suppressing nucleation over large areas Although formamidinium-based lead iodide (PbI 2 ) perovskites have a favorable bandgap and good thermal stability, the difficulty in controlling nucleation makes it difficult to grow high-quality, large-area films compared with methylammonium counterparts. Bu et al. show that adding N -methyl-2-pyrrolidone to the perovskite precursors forms an adduct with PbI 2 that promotes the formation of the desired black α-phase at room temperature. The addition of potassium hexafluorophosphate eliminated hysteresis by passivating interfacial defects and promoted long-term thermal stability at 85°C in unencapsulated devices. Large-area modules (17 square centimeters) achieved power conversion efficiencies of 20.4%. Science , abh1035, this issue p. 1327

A comparative investigation of the post-electroplating treatment influence on the gas detecting performances of single ZnO nanorod/nanowire (NR/NW), as grown by electrochemical deposition (ECD) and integrated into nanosensor devices, is presented. In this work, hydrothermal treatment (HT) in a H2O steam and conventional thermal annealing (CTA) in a furnace at 150 °C in ambient were used as post-growth treatments to improve the material properties. Herein, the morphological, optical, chemical, structural, vibrational, and gas sensing performances of the as-electrodeposited and treated specimens are investigated and presented in detail. By varying the growth temperature and type of post-growth treatment, the morphology is maintained, whereas the optical and structural properties show increased sample crystallization. It is shown that HT in H2O vapors affects the optical and vibrational properties of the material. After investigation of nanodevices based on single ZnO NR/NWs, it was observed that higher temperature during the synthesis results in a higher gas response to H2 gas within the investigated operating temperature range from 25 to 150 °C. CTA and HT or autoclave treatment showed the capability of a further increase in gas response of the prepared sensors by a factor of ∼8. Density functional theory calculations reveal structural and electronic band changes in ZnO surfaces as a result of strong interaction with H2 gas molecules. Our results demonstrate that high-performance devices can be obtained with high-crystallinity NWs/NRs after HT. The obtained devices could be the key element for flexible nanoelectronics and wearable electronics and have attracted great interest due to their unique specifications.

Two-dimensional Ruddlesden–Popper (RP) and Dion–Jacobson (DJ) phase perovskites are promising alternatives to fabricate blue perovskite light-emitting diodes (PeLEDs) due to their strong quantum/dielectric confinement. While the RP phase perovskites have been widely used as emitter layers in blue PeLEDs, the DJ phase perovskites, possessing better structural stability and charge transfer property, have received little attention. Here, we report the use of DJ phase perovskites for fabricating efficient sky-blue PeLEDs. Organic diamine propane-1,3-diammonium cations were first incorporated into CsPbBr3 to prepare DJ phase perovskites. RbBr was further incorporated as a passivation agent to eliminate traps. It is found that diamine cations and RbBr are interdependent in terms of increasing the utilization of charges. Radiative recombination was enhanced, effectively benefiting from the synergetic confinement and passivation effects. The photoluminescence quantum yield approached 70%. Finally, the fabricated PeLEDs achieved an external quantum efficiency of 8.5% with an emission peak at 490 nm.

The incorporation of a certain amount of Cl ions into methylammonium lead iodide (MAPbI3) perovskite films and how these incorporated Cl ions affect the structural and electronic properties of these films have been an intensively studied topic. In this study, we comprehensively investigated Cl incorporation in MAPbI3 at the atomic scale by a combined study of scanning tunneling microscopy, X-ray photoelectron spectroscopy, ultraviolet and inverse photoemission spectroscopy, density functional theory and molecular dynamics calculations. At a Cl concentration of 14.8 ± 0.6%, scanning tunneling microscopy images confirm the incorporation of Cl ions on the MAPbI3 surface, which also corresponds to the highest surface stability of MAPbI3 found from the viewpoint of both thermodynamics and kinetics by density functional theory and molecular dynamics calculations. Our results show that the Cl concentration is crucial to the surface bandgap and stability of MAPbI3.

All-inorganic α-CsPbBrxI3-x perovskites featuring nano-sized crystallites show great potential for pure-red light-emitting diode (LED) applications. Currently, the CsPbBrxI3–x LEDs based on nano-sized α-CsPbBrxI3-x crystallites have been fabricated mainly via the classical colloidal route including a tedious procedure of nanocrystal synthesis, purification, ligand or anion exchange, film casting, etc. With the usually adopted conventional LED device structure, only high turn-on voltages (> 2.7) have been achieved for CsPbBrxI3-x LEDs. Moreover, this mix-halide system may suffer from severe spectra-shift under bias. In this report, CsPbBrxI3-x thin films featuring nano-sized crystallites are prepared by incorporating multiple ammonium ligands in a one-step spin-coating route. The multiple ammonium ligands constrain the growth of CsPbBrxI3-x nanograins. Such CsPbBrxI3-x thin films benefit from quantum confinement. The corresponding CsPbBrxI3-x LEDs, adopting a conventional LED structure of indium-doped tin oxide (ITO)/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)/CsPbBrxI3-x/[6, 6]-phenyl C61 butyric acid methyl ester (PCBM)/bathocuproine (BCP)/Al, emit pure-red color at Commission Internationale de l’eclairage (CIE) coordinates of (0.709, 0.290), (0.711, 0.289), etc., which represent the highest color-purity for reported pure-red perovskite LEDs and meet the Rec. 2020 requirement at CIE (0.708, 0.292) very well. The CsPbBrxI3-x LED shows a low turn-on voltage of 1.6 V, maximum external quantum efficiency of 8.94%, high luminance of 2,859 cdm−2, and good color stability under bias.

The upscaling of perovskite solar cells to module scale and long-term stability have been recognized as the most important challenges for the commercialization of this emerging photovoltaic technology. In a perovskite solar module, each interface within the device contributes to the efficiency and stability of the module. Here, we employed a holistic interface stabilization strategy by modifying all the relevant layers and interfaces, namely the perovskite layer, charge transporting layers and device encapsulation, to improve the efficiency and stability of perovskite solar modules. The treatments were selected for their compatibility with low-temperature scalable processing and the module scribing steps. Our unencapsulated perovskite solar modules achieved a reverse-scan efficiency of 16.6% for a designated area of 22.4 cm2. The encapsulated perovskite solar modules, which show efficiencies similar to the unencapsulated one, retained approximately 86% of the initial performance after continuous operation for 2,000 h under AM1.5G light illumination, which translates into a T90 lifetime (the time over which the device efficiency reduces to 90% of its initial value) of 1,570 h and an estimated T80 lifetime (the time over which the device efficiency reduces to 80% of its initial value) of 2,680 h. The upscaling of layer treatments and processing that afford high efficiency and stability in small-area perovskite solar cells remains challenging. Liu et al. show how the efficiency and stability of perovskite modules can be improved using an integrated approach to interface and layer engineering.

The booming growth of organic-inorganic hybrid lead halide perovskite solar cells have made this promising photovoltaic technology to leap towards commercialization. One of the most important issues for the evolution from research to practical application of this technology is to achieve high-throughput manufacturing of large-scale perovskite solar modules. In particular, realization of scalable fabrication of large-area perovskite films is one of the essential steps. During the past ten years, a great number of approaches have been developed to deposit high quality perovskite films, to which additives are introduced during the fabrication process of perovskite layers in terms of the perovskite grain growth control, defect reduction, stability enhancement, etc. Herein, we first review the recent progress on additives during the fabrication of large area perovskite films for large scale perovskite solar cells and modules. We then focus on a comprehensive and in-depth understanding of the roles of additives for perovskite grain growth control, defects reduction, and stability enhancement. Further advancement of the scalable fabrication of high-quality perovskite films and solar cells using additives to further develop large area, stable perovskite solar cells are discussed.

Control of forward and inverse reactions between perovskites and precursor materials is key to attaining high-quality perovskite materials. Many techniques focus on synthesizing nanostructured CsPbX3 materials (e.g., nanowires) via a forward reaction (CsX + PbX2 → CsPbX3). However, low solubility of inorganic perovskites and complex phase transition make it difficult to realize the precise control of composition and length of nanowires using the conventional forward approach. Herein, we report the self-assembly inverse growth of CsPbBr3 micronanowires (MWs) (CsPb2Br5 → CsPbBr3 + PbBr2↑) by controlling phase transition from CsPb2Br5 to CsPbBr3. The two-dimensional (2D) structure of CsPb2Br5 serves as nucleation sites to induce initial CsPbBr3 MW growth. Also, phase transition allows crystal rearrangement and slows down crystal growth, which facilitates the MW growth of CsPbBr3 crystals along the 2D planes of CsPb2Br5. A CsPbBr3 MW photodetector constructed based on the inverse growth shows a high responsivity of 6.44 A W–1 and detectivity of ∼1012 Jones. Large grain size, high crystallinity, and large thickness can effectively alleviate decomposition/degradation of perovskites, which leads to storage stability for over 60 days in humid environment (relative humidity = 45%) and operational stability for over 3000 min under illumination (wavelength = 400 nm, light intensity = 20.06 mW cm–2).

Perovskite materials with excellent optical and electrical properties are promising for light‐emitting diodes. In the field of perovskite light‐emitting diodes (PeLEDs), organic materials additive engineering has been proved to be an effective scheme for enhancing efficiency and stability in PeLEDs. Most impressively, the reported external quantum efficiency of PeLEDs based on perovskite‐organic composite has reached over 20%. Herein, we will review the important progress of the organic materials' additive‐modified PeLEDs and discuss the remaining problems and challenges and the key research direction in the near future.

In several photovoltaic (PV) technologies, the presence of electronic defects within the semiconductor band gap limit the efficiency, reproducibility, as well as lifetime. Metal halide perovskites (MHPs) have drawn great attention because of their excellent photovoltaic properties that can be achieved even without a very strict film‐growth control processing. Much has been done theoretically in describing the different point defects in MHPs. Herein, we discuss the experimental challenges in thoroughly characterizing the defects in MHPs such as, experimental assignment of the type of defects, defects densities, and the energy positions within the band gap induced by these defects. The second topic of this Review is passivation strategies. Based on a literature survey, the different types of defects that are important to consider and need to be minimized are examined. A complete fundamental understanding of defect nature in MHPs is needed to further improve their optoelectronic functionalities., Watching the defects: Defects play a pivotal role in the overall performance of perovskite solar cells. This Review focuses on central questions of “what defects exist in metal halide perovskites” and “how can one reduce detrimental defects towards high‐performance perovskite solar cells”.

All-inorganic halide perovskites are promising materials for optoelectronic applications. The surface or interface structure of the perovskites plays a crucial role in determining the optoelectronic conversion efficiency, as well as the material stability. A thorough understanding of surface atomic structures of the inorganic perovskites and their contributions to their optoelectronic properties and stability is lacking. Here we show a scanning tunneling microscopy investigation on the atomic and electronic structure of CsPbBr3 perovskite. Two different surface structures with a stripe and an armchair domain are identified, which originates from a complex interplay between Cs cations and Br anions. Our findings are further supported and correlated with density functional theory calculations and photoemission spectroscopy measurements. The stability evaluation of photovoltaic devices indicates a higher stability for CsPbBr3 in comparison with MAPbBr3, which is closely related to the low volatility of Cs from the perovskite surface.

Summary Tin-based perovskite solar cells (PSCs), with more consummate optical band gaps, lower exciton-binding energies, and higher charge-carrier mobility, have not attracted tremendous research efforts compared with the lead-based ones that have a record power conversion efficiency (PCE) of 24.2%. The major challenges for Sn-based research are significantly low open-circuit voltage, poor reproducibility, and environmental instability. It has been identified that the oxidation processes take place during the preparation of precursor solutions and fabrication of films, due to the low redox potential of the stannous absorption layer. Herein, we propose two strategies of crystal-resolving and recrystallization technology to reduce the oxidation process. As a result, PCEs of 8.9% (active area of 0.04 cm2) and 5.5% (active area = 1.01 cm2) are attained using the inverted p-i-n structure, which will lead to a revival of lead-free PSC research.

Lead-free double perovskite materials have attracted much interest for optoelectronic applications due to their nontoxicity and high stability. In this work, centimetre-sized Cs2AgBiBr6 single crystals were successfully grown using methylammonium bromide (MABr) as the flux by a top-seeded solution growth (TSSG) method. The low-temperature crystal structure of Cs2AgBiBr6 single crystals was determined and refined. To investigate the interface problems between Cs2AgBiBr6 single crystals and electrodes, the optical band gap, X-ray photoelectron spectroscopy (XPS), and ultraviolet photoemission spectroscopy (UPS) measurements were performed on Cs2AgBiBr6 single crystals. More importantly, we investigated the photodetectors based on Cs2AgBiBr6 single crystals with different contact electrodes (Au, Ag, and Al). It is found that a good Ohmic contact with Ag electrodes enables excellent photo-response behaviors. Furthermore, we studied the photodetectors based on Cs2AgBiBr6 single crystals using Ag electrodes under room and low temperature conditions, which underwent phase transition. Cs2AgBiBr6 single crystal photodetectors show clear differences at room and low temperatures, which is caused by the work function changes of Cs2AgBiBr6 single crystals induced by the reversible phase transition. These attractive properties may enable opportunities to apply emerging double perovskite single-crystalline materials for high-performance optoelectronic devices.

Hybrid chemical vapor deposition (HCVD) has been employed in the fabrication of perovskite solar cells (PSCs) and modules (PSMs), and it shows strong promise for upscalable fabrication. The conventional HCVD process needs a relatively long processing time (e.g., several hours) and the fabricated PSCs often exhibit salient hysteresis, which impedes utilization of this technology for mass production. Herein, we demonstrate a rapid HCVD (RHCVD) fabrication process for PSCs using a rapid thermal process, which not only significantly reduces the deposition time to less than 10 min, but also effectively suppresses hysteresis. This markedly reduced deposition time is comparable to that of solution-coating processes. Furthermore, the shorter processing time inside the furnace reduces the exposure time of the glass/ITO/SnO2 substrates under vacuum, which helps maintain the high quality of the SnO2 electron-transport layer and results in a lower density of gap states. Finally, PSMs with a designated area of 22.4 cm2 fabricated via RHCVD achieved an efficiency of 12.3%, and maintained 90% of the initial value after operation under continuous light illumination for over 800 h.

Lead-free tin perovskite solar cells (PSCs) have undergone rapid development in recent years and are regarded as a promising eco-friendly photovoltaic technology. However, a strategy to suppress charge recombination via a built-in electric field inside a tin perovskite crystal is still lacking. In the present study, a formamidinium tin iodide (FASnI

The spectral instability issue is a challenge in blue perovskite light-emitting diodes (PeLEDs). Dion–Jacobson (DJ) phase perovskites are promising alternatives to achieve high-quality blue PeLEDs. However, the current exploration of DJ phase perovskites is focused on symmetric divalent cations, and the corresponding efficiency of blue PeLEDs is still inferior to that of green and red ones. In this work, we report a new type of DJ phase CsPb(Br/Cl)3 perovskite via introduction of an asymmetric molecular configuration as the organic spacer cation in perovskites. The primary and tertiary ammonium groups on the asymmetric cations bridge with the lead halide octahedra forming the DJ phase structures. Stable photoluminescence spectra were demonstrated in perovskite films owing to the suppressed halide segregation. Meanwhile, the radiative recombination efficiency of charges is improved significantly as a result of the confinement effects and passivation of charge traps. Finally, we achieved an external quantum efficiency of 2.65% in blue PeLEDs with stable spectra emission under applied bias voltages. To our best knowledge, this is the first report of asymmetric cations used in PeLEDs, which provides a facile solution to the halide segregation issue in PeLEDs.

Metal halide perovskite materials (MHPMs) have attracted significant attention because of their superior optoelectronic properties and versatile applications. The power conversion efficiency of MHPM solar cells (PSCs) has skyrocketed to 25.5 %. Although the performance of PSCs is already competitive, several important challenges still need to be solved to realize commercial applications. A thorough understanding of surface atomic structures and structure–property relationships is at the heart of these remaining issues. Scanning tunneling microscopy (STM) and spectroscopy (STS) can be used to characterize the surface properties of MHPMs, which can offer crucial insights into MHPMs at the atomic scale. This Review summarizes recent progress in STM and STS studies on MHPMs, with a focus on the surface properties. We provide understanding from the comparative perspective of several different MHPMs. We also highlight a series of novel phenomena observed by STM and STS. Finally, we outline a few research topics of primary importance for future studies.

Metal halide perovskites (MHPs) have become a major topic of research in thin film photovoltaics due to their advantageous optoelectronic properties. These devices typically have the MHP absorber layer sandwiched between two charge selective layers (CSLs). The interfaces between the perovskite layer and these CSLs are potential areas of higher charge recombination. Understanding the nature of these interfaces is key for device improvement. Additionally, non-stoichiometric perovskite films are expected to strongly impact the interfacial properties. In this study, the interface between CH

Rational design of heterostructures opens up new opportunities as an ideal catalyst system for lithium polysulfides conversion in lithium-sulfur battery. However, its traditional fabrication process is complex, which makes it difficult to reasonably control the content and distribution of each component. In this work, to rationally design the heterostructure, the atomic layer deposition is utilized to hybridize the TiO2-TiN heterostructure with the three-dimensional carbon nanotube sponge. Through optimizing the deposited thickness of TiO2 and TiN layers and adopting the annealing post-treatment, the derived coaxial sponge with uniform TiN-TiO2 heterostructure exhibits the best catalytic ability. The corresponding lithium-sulfur battery shows enhanced electrochemical performance with high specific capacity of 1289 mAh g−1 at 1 C and capacity retention of 85% after 500 cycles at 2 C. Furthermore, benefiting from the highly porous structure and interconnected conductive pathways from the sponge, its areal capacity reaches up to 21.5 mAh cm−2., It is challenging to optimize catalytic heterostructures for lithium sulfur (Li-S) batteries. Here, authors prepare nanometer-scale TiN-TiO2 heterostructures via atomic layer deposition on carbon nanotube sponge to realize stable Li-S batteries with high areal capacity and improved rate capability.

Atomistic characterization of surface termination and the corresponding mechanical properties of single-crystal methylammonium lead tribromide (MAPbBr3) are performed using combined atomic force microscopy (AFM) measurements and density functional theory (DFT) calculations. A clean MAPbBr3 surface is obtained by in situ cleavage in ultrahigh vacuum at room temperature, and the subsequent AFM measurements of the as-cleaved MAPbBr3 exhibit the coexistence of two different surface terrace types with step height differences corresponding to about half the thickness of a PbI6 octahedron layer. Concurrent friction force microscopy measurements show that the two surfaces result in two distinct friction values. Based on DFT calculations, we attribute the higher-friction and lower-friction surfaces to MABr-terminated flat and PbBr2-terminated vacant surface terminations, respectively. The calculated electronic band structures of the various MABr- and PbBr2-terminated surfaces show that the midgap states are absent, revealing the defect-tolerant nature of the ideal single-crystal MAPbBr3 surfaces.

A series of challenging issues such as field-driven spectral drift for the CsPbClxBr3–x system and mixed phases in quasi-two-dimensional structures still exist when devising blue-emitting perovskites. In this Letter, the CsPbBr3 quantum-dot (QD) system is proposed to overcome these challenges. However, to date, the CsPbBr3 QD films with tunable colors from green to blue still cannot be achieved using existing methods. Herein, a simple one-step spin-coating route incorporated with efficient ligand passivation is developed to realize this goal. The size restriction of CsPbBr3 QDs is enabled by a diammonium ligand, propane-1,3-diammonium bromide (PDAB). A mixed-ligand system of phenethylammonium bromide (PEAB) with PDAB is further explored to enhance their optical performance. The CsPbBr3 QDs experience a second growth process upon controlled air exposure, which is utilized to realize their size control and emission wavelength tunability. The CsPbBr3 QD-based devices exhibit no spectral drift in electroluminescence under voltage bias.

Tetragonal phases for perovskite solar cells The power conversion efficiencies (PCEs) of all-inorganic perovskites are lower than those of materials with organic cations. This is in part because these materials have larger bandgaps. The cubic crystal phases of these materials also exhibit poor stability. Wang et al. synthesized the tetragonal β-phase of CsPbI 3 from HPbI 3 and CsI. The material exhibited higher stability and a more favorable bandgap, which allowed for PCEs of 15%. Passivation of the surface trap state with choline iodide boosted PCEs to 18%. Science , this issue p. 591

Perovskite photovoltaic (PV) technology toward commercialization relies on high power conversion efficiency (PCE), long lifetime, and low-toxicity in addition to development of scalable fabrication...