Multifunctional Organic Potassium Salt Additives as the Efficient Defect Passivator for High-Efficiency and Stable Perovskite Solar Cells

Despite the rapid developments are achieved for perovskite solar cells (PSCs), the existence of various defects in the devices still limits the further enhancement of the power conversion efficiency (PCE) and the long-term stability of devices. Herein, the efficient organic potassium salt (OPS) of para-halogenated phenyl trifluoroborates is presented as the precursor additives to improve the performance of PSCs. Studies have shown that the 4-chlorophenyltrifluoroborate potassium salt (4-ClPTFBK) exhibits the most effective interaction with the perovskite lattice. Strong coordination between  BF₃⁻/halogen in anion and uncoordinated Pb²⁺/halide vacancies, along with the hydrogen bond between F in  BF₃⁻ and H in FA⁺ are observed. Thus, due to the synergistic contribution of the potassium and anionic groups, the high-quality perovskite film with large grain size and low defect density is achieved. As a result, the optimal devices show an enhanced efficiency of 24.50%, much higher than that of the control device (22.63%). Furthermore, the unencapsulated devices present remarkable thermal and long-term stability, maintaining 86% of the initial PCE after thermal test at 80 °C for 1000 h and 95% after storage in the air for 2460 h.     

An Efficient One-Arrow-Two-Hawks Strategy Achieves High Efficiency and Stable Batch Variance for Benzodifuran-based Polymer Solar Cells

With the development of organic solar cells (OSCs), the high-performance and stable batch variance are becoming a new challenge for designing polymer donors. To obtain high photovoltaic performance, adopting polymers with high molecular weight as donors is an ordinary strategy. However, the high molecular weight need to subtly control the reaction time and state, inevitably caused batch-to-batch variations. Herein, a strategy of steric effect is applied to benzodifuran (BDF)-based polymer by introducing different positions of Cl atom, producing two polymers PBDFCl-1 and PBDFCl-2. The more twisted side chains conformation not only achieve the control of moderate molecular weight for PBDFCl-2, but also easily form molecular stacking through adopting BDF unit and maintain sufficient polymeric crystallinity. Due to the optimized stacking mode and good blend miscibility, PBDFCl-2-based device exhibitsa more elegant power conversion efficiency (PCE) of 17.00% compared to PBDFCl-1-based device. This is the highest efficiency record for BDF-based binary OSCs. Meanwhile, the PCE device variation of the different molecular weights for PBDFCl-2 is little, indicating the reduction of the batch variation. Therefore, smartly using steric effect of Cl atom in strong crystalline BDF unit can form efficient molecular stacking regulations and realize the coordination of high-performance and stable batch variance.     

Ultra-Stable and Sensitive Ultraviolet Photodetectors Based on Monocrystalline Perovskite Thin Films

The detection of ultraviolet (UV) radiation with effective performance and robust stability is essential to practical applications. Metal halide single-crystal perovskites (ABX₃) are promising next-generation materials for UV detection. The device performance of all-inorganic CsPbCl₃ photodetectors (PDs) is still limited by inner imperfection of crystals grown in solution. Here wafer-scale single-crystal CsPbCl₃ thin films are successfully grown by vapor-phase epitaxy method, and the as-constructed PDs under UV light illumination exhibit an ultralow dark current of 7.18 pA, ultrahigh ON/OFF ratio of ≈5.22 × 10⁵, competitive responsivity of 32.8 A W⁻¹, external quantum efficiency of 10867% and specific detectivity of 4.22 × 10¹² Jones. More importantly, they feature superb long-term stability toward moisture and oxygen within twenty-one months, good temperature tolerances at low and high temperatures. The ability of the photodetector arrays for excellent UV light imaging is further demonstrated.     

Direct Growth of Uniform Bimetallic Core-Shell or Intermetallic Nanoparticles on Carbon via a Surface-Confinement Strategy for Electrochemical Hydrogen Evolution Reaction

Due to the surface inhomogeneity of the solid supports, direct growth of uniform bimetallic nanoparticles (NPs) with controllable structure and size thereon is particularly challenging. Herein, a surface-confinement strategy is reported to directly prepare ultrafine bimetallic Pt M NPs (MFe, Cu, and Co) with structure of core-shell or intermetallic compounds on an N functionalized carbon support (NC). It is found that the N species of NC support can atomically disperse metal cations of precursors, which largely renders uniform nucleation and growth of bimetallic NPs and fine structure modulation of them. In another regard, metal transfer is confined to a narrow region on NC via N-mediation, hence greatly favoring localized particle growth and formation of ultrafine bimetallic NPs. Remarkably, the ultrafine 3.1 ± 0.7 nm intermetallic Pt₃Fe NPs on NC displayed excellent catalytic activity and durability toward electrochemical hydrogen evolution reaction.     

Electret Molecular Configuration Induced Programmable Photonic Memory for Advanced Logic Operation and Data Encryption

Nonvolatile organic photonic transistor (OPT) memories have attracted widespread attention due to their nondestructive readout, remote controllability, and robust tunability. Developing electrets with similar molecular structures but different memory behaviors and light-responsive features is crucial for light-wavelength-modulated data encryption. However, reported OPT memories have yet to meet this challenge. Here a new electret molecule (“H-PDI”) is developed via reconfiguring the linear perylene diimide molecule (“L-PDI”) to a helical shape. Respectively incorporating H-PDI and L-PDI into the floating gate layer results to H-PDI OPT and L-PDI OPT. Attributing to their remarkably different electronic structures and energy bandgaps, H-PDI OPT and L-PDI OPT preferably respond to 405 and 532 nm light irradiation, respectively. Upon electrical programming, data can be written and stored in both memories with good retention features and a high “1”/“0” state current ratio over 10⁵, though the data can only be erased by light with correct wavelengths, rather than the electrical field. Moreover, data stored in a memory array consisting of both H-PDI OPT and L-PDI OPT can only be read out by correct inputs, and wrong inputs will lead to highly deceptive outputs. This study provides a general design strategy of OPT for advanced data encryption and protection.     

Reinforced Wool Keratin Fibers via Dithiol Chain Re-bonding

Regenerated wool keratin fibers (RWKFs) have heretofore attracted tremendous interest according to environmental friendliness, ample resource, and intrinsic biocompatibility for broad applications. In this realm, both uncontrollable keratin fibril assembly procedure and resultant insufficient mechanical strength, have greatly hindered their large-scale manufacture and commercial viability. Herein, a continuous wet-spinning strategy is put forward to rebuild wool keratin into compact regenerated bio-fibers with improved strength via disulfide re-bonding. Dithiothreitol (DTT) has been introduced to renovate disulfide linkage inside keratin polypeptide chains, and bridge keratin fibrils via covalent thiol bonding to form a continuous backbone as mechanical support. A thus-derived RWKF manifests a tensile strength of 186.1 ± 7.0 MPa and Young's modulus of 7.4 ± 0.2 GPa, which exceeds those of natural wool, feathers, and regenerated wool or feather keratin fibers. The detailed wet-spinning technical parameters, such as coagulation, oxidation, and post-treatment, have been systematically optimized to guarantee the continuous preparation of high-strength regenerated keratin fibers. This work offers insight into solving the concurrent challenges for continuous manufacture of regenerated protein fibers and sustainability concerns about biomass waste.     

High-Efficiency Organic Solar Cells Enabled by Chalcogen Containing Branched Chain Engineering: Balancing Short-Circuit Current and Open-Circuit Voltage,Enhancing Fill Factor

The elaborate balance between the open-circuit voltage (V_OC) and the short-circuit current density (J_SC) is critical to ensure efficient organic solar cells (OSCs). Herein, the chalcogen containing branched chain engineering is employed to address this dilemma. Three novel nonfullerene acceptors (NFAs), named BTP-2O , BTP-O-S , and BTP-2S , featuring different peripheral chalcogen containing branched chains are synthesized. Compared with symmetric BTP-2O and BTP-2S grafting two alkoxy or alkylthio branched chains, the asymmetric BTP-O-S grafting one alkoxy and one alkylthio branched chains shows mediate absorption range, applicable miscibility, and favorable crystallinity. Benefiting from the enhanced π–π stacking and charge transport, an optimal power conversion efficiency (PCE) of 17.3% is obtained for the PM6: BTP-O-S -based devices, with a good balance between V_OC (0.912 V) and J_SC (24.5 mA cm⁻²), and a high fill factor (FF) of 0.775, which is much higher than those of BTP-2O (16.1%) and BTP-2S -based (16.4%) devices. Such a result represents one of the highest efficiencies among the binary OSCs with V_OC surpassing 0.9 V. Moreover, the BTP-O-S -based devices fabricated by using green solvent yield a satisfactory PCE of 17.1%. This work highlights the synergistic effect of alkoxy and alkylthio branched chains for high-performance OSCs by alleviating voltage loss and enhancing FF.     

Plasma Enhanced Lithium Coupled with Cobalt Fibers Arrays for Advanced Energy Storage

Construction of high efficiency and stable Li metal anodes is extremely vital to the breakthrough of Li metal batteries. In this study, for the first time, groundbreaking in situ plasma interphase engineering is reported to construct high-quality lithium halides-dominated solid electrolyte interphase layer on Li metal to stabilize & protect the anode. Typically, SF₆ plasma-induced sulfured and fluorinated interphase (SFI) is composed of LiF and Li₂S, interwoven with each other to form a consecutive solid electrolyte interphase. Simultaneously, brand-new vertical Co fibers (diameter: ≈5 µm) scaffold is designed via a facile magnetic-field-assisted hydrothermal method to collaborate with plasma-enhanced Li metal anodes (SFI@Li/Co). The Co fibers scaffold accommodates active Li with mechanical integrity and decreases local current density with good lithiophilicity and low geometric tortuosity, supported by DFT calculations and COMSOL Multiphysics simulation. Consequently, the assembled symmetric cells with SFI@Li/Co anodes exhibit superior stability over 525 h with a small voltage hysteresis (125 mV at 5 mA cm⁻²) and improved Coulombic efficiency (99.7%), much better than the counterparts. Enhanced electrochemical performance is also demonstrated in full cells with commercial cathodes and SFI@Li/Co anode. The research offers a new route to develop advanced alkali metal anodes for energy storage.     

An Intrinsically Nonflammable Electrolyte for Prominent-Safety Lithium Metal Batteries with High Energy Density and Cycling Stability

Nex-generation high-energy-density storage battery, assembled with lithium (Li)-metal anode and nickel-rich cathode, puts forward urgent demand for advanced electrolytes that simultaneously possess high security, wide electrochemical window, and good compatibility with electrode materials. Herein an intrinsically nonflammable electrolyte is designed by using 1 M lithium difluoro(oxalato)borate (LiDFOB) in triethyl phosphate (TEP) and N-methyl-N-propyl-pyrrolidinium bis(trifluoromethylsulfonyl)imide [Pyr₁₃][TFSI] ionic liquid (IL) solvents. The introduction of IL can bring plentiful organic cations and anions, which provides a cation shielding effect and regulates the Li⁺ solvation structure with plentiful Li⁺-DFOB⁻ and Li⁺-TFSI⁻ complexes. The unique Li⁺ solvation structure can induce stable anion-derived electrolyte/electrode interphases, which effectively inhibit Li dendrite growth and suppress side reactions between TEP and electrodes. Therefore, the LiNi_0.9Co_0.05Mn_0.05O₂ (NCM90)/Li coin cell with this electrolyte can deliver stable cycling even under 4.5 V and 60 °C. Moreover, a Li-metal battery with thick NCM90 cathode (≈ 15 mg cm⁻²) and thin Li-metal anode (≈ 50 µm) (N/P ≈ 3), also reveals stable cycling performance under 4.4 V. And a 2.2 Ah NCM90/Li pouch cell can simultaneously possess prominent safety with stably passing the nail penetration test, and high gravimetric energy density of 470 Wh kg⁻¹ at 4.4 V.     

Proximity-Induced Fully Ferromagnetic Order with Eightfold Magnetic Anisotropy in Heavy Transition Metal Oxide CaRuO3

Ferromagnetic materials with a strong spin-orbit coupling (SOC) have attracted much attention in recent years because of their exotic properties and potential applications in energy-efficient spintronics. However, such materials are scarce in nature. Here, a proximity-induced paramagnetic to ferromagnetic transition for the heavy transition metal oxide CaRuO₃ in (001)-(LaMnO₃/CaRuO₃) superlattices is reported. Anomalous Hall effect is observed in the temperature range up to 180 K. Maximal anomalous Hall conductivity and anomalous Hall angle are as large as ∼15 Ω⁻¹ cm⁻¹ and ∼0.93%, respectively, by one to two orders of magnitude larger than those of the typical 3d ferromagnetic oxides such as La_0.67Sr_0.33MnO₃. Density functional theory calculations indicate the existence of avoid band crossings in the electronic band structure of the ferromagnetic CRO layer, which enhances Berry curvature thus strong anomalous Hall effects. Further evidences from polarized neutron reflectometry show that the CaRuO₃ layers are in a fully ferromagnetic state (∼0.8 μ_B/Ru), in sharp contrast to the proximity-induced canted antiferromagnetic state in 5d oxides SrIrO₃ and CaIrO₃ (∼0.1 μ_B/Ir). More than that, the magnetic anisotropy of the (001)-(LaMnO₃/CaRuO₃) superlattices is eightfold symmetric, showing potential applications in the technology of multistate data storage.