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Transparent, flexible MAPbI3 perovskite microwire array passivated with ultra-hydrophobic supramolecular assembly for stable and high-performance photodetectors
摘要： The emergence of organic-inorganic hybrid perovskites (OHPs) has revolutionised the potential performance of optoelectronic devices, most perovskites are opaque and hence incompatible with transparent optoelectronics, and sensitive to environmental degradation. Here, a single-step fabrication of ultra-long MAPbI3 perovskite microwire array over a large-area using stencil lithography based on a sequential vacuum sublimation. The environmental stability of MAPbI3 is empowered a newly designed and synthesized transparent supramolecular self-assembly, based on a mixture of two tripodal L-Phe-C11H23/C7F15 molecules, which showed a contact angle of 105° and served as ultra-hydrophobic passivation layer for more than 45 days in ambient atmosphere. The MAPbI3 microwire array passivated with supramolecular self-assembly demonstrate for the first time both excellent transparency of ~89% at 550 nm and remarkable photoresponse with photo-switching ratio of ~104, responsivity of 789 A/W, detectivity of 1014 Jones, linear dynamic range of ~ 122 dB, and rise time of 432 μs. Furthermore, the photodetector fabricated on flexible PET substrate demonstrated robust mechanical flexibility even beyond 1200 bending cycles. Therefore, the scalable stencil lithography and supramolecular passivation approaches have the potential to deliver next-generation transparent, flexible, and stable optoelectronics.
关键词： transparency,stencil lithography,photodetectors,MAPbI3,supramolecular self-assembly,flexibility,organic-inorganic hybrid perovskites,environmental stability
更新于2025-09-23 15:21:01
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Gap Plasmon of Virus-Templated Biohybrid Nanostructures Uplifting the Performance of Organic Optoelectronic Devices
摘要： Plasmonic nanostructures, which exhibit prominent localized surface plasmon resonance (LSPR) properties, are highly desirable for organic solar cells (OSC) and organic light-emitting diode (OLED) devices. In the present work, novel plasmonic bio-nanostructures are successfully synthesized via the self-densification of silver (Ag) and gold (Au) metallic nanoparticles (NPs) onto a genetically engineered M13 bacteriophage template. Owing to the unique charge selectivity of the peptide receptors on the M13 bacteriophage, the metallic NPs can be directly anchored onto the bacteriophage through charge-driven interactions without binder/surfactant. The resulting Ag/AuNP-M13 bio-nanostructures display extraordinary gap-plasmon effect as well as tremendously enhanced LSPR properties than the randomly dispersed Ag/Au NPs. The incorporation of Ag/AuNP-M13 bio-nanostructures tremendously improves the performance of both OSC and OLED devices. Specifically, a power conversion efficiency increment of 15.5% is recorded for the phage-modified OSCs; whereas an external quantum efficiency increment of 22.6% is achieved for the phage-modified OLEDs. Based on this environmentally benign virus-template approach, various plasmonic/photonic bio-nanostructures can be designed for diverse device applications.
关键词： field-enhancement,optoelectronics,M13 bacteriophage,metamaterials,self-assembly,gap-plasmon effect
更新于2025-09-23 15:21:01
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Noninvasive In Situ Ratiometric Imaging of Biometals Based on Self-Assembled Peptide Nanoribbon
摘要： Development of probes for accurate sensing and imaging of biometals in situ is still a growing interest owing to their crucial roles in cellular metabolism, neurotransmission, and apoptosis. Among them, Zn2+ and Cu2+ are two important cooperative biometals closely related to Alzheimer’s disease (AD). Herein, we developed a multifunctional probe based on self-assembling peptide nanoribbon for ratiometric sensing of Zn2+, Cu2+, or Zn2+ and Cu2+ simultaneously. Uniform peptide nanoribbon (AQZ@NR) was rationally designed by coassembling a Zn2+-specific ligand AQZ-modified peptide (AQZKL-7) with peptide KL-7. The nanoribbon further combined with Cu2+-sensitive near-infrared quantum dots (NIR QDs) and Alexa Fluor 633 as an inner reference molecule, which was endowed with the capability for ratiometric Zn2+ and Cu2+ imaging at the same time. The peptide-based probe exhibited good specificity to Zn2+ and Cu2+ without interference from other ions. Importantly, the nanoprobe was successfully applied for noninvasive Zn2+ and Cu2+ monitoring in both living cells and zebrafish via multicolor fluorescence imaging. This gives insights into the dynamic Zn2+ and Cu2+ distribution in an intracellular and in vivo mode, as well as understanding the neurotoxicity of high concentration of Zn2+ and Cu2+. Therefore, the self-assembled nanoprobe shows great promise in multiplexed detection of many other biometals and biomolecules, which will benefit the diagnosis and treatment of AD in clinical applications.
关键词： fluorescence imaging,biometals,ratiometric imaging,peptide nanoribbon,Cu2+,Zn2+,self-assembly,Alzheimer’s disease
更新于2025-09-23 15:21:01
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Selfa??Assembled PMMA Porous Membranes Decorated with In Situ Synthesized ZnO Nanoparticles with UVa??Tunable Wettability
摘要： This study reports a simple approach to fabricate porous poly(methyl methacrylate) (PMMA) membranes homogeneously decorated with exposed zinc oxide (ZnO) nanoparticles (NPs). This fabrication method significantly overcomes the disadvantages of both conventional foaming processes and incorporation of inorganic NPs in polymeric matrices. In particular, the porous structure is simply self-assembled by slowly evaporating a suitable solvent. The ZnO NPs are in situ formed by a thermally activated conversion of the zinc acetate precursor, previously embedded in the polymeric matrix. Scanning and transmission electron microscopy investigations show the formation of the desired self-assembled highly porous structure and ZnO NPs with branched morphology, respectively. The wetting behavior of the membranes surface is studied as a function of the ZnO content and UV irradiation, exploiting the switchable wettability of ZnO. The obtained unexpected results are then tentatively rationalized taking into account the surface chemistry and the roughness that arises from both porous structure and the different NPs dimensions and content.
关键词： porous membranes,nanocomposites,tunable wettability,self-assembly,in situ synthesis
更新于2025-09-23 15:21:01
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Semitransparent Perovskite Solar Cells
摘要： Solar cells are one of the most attractive and nonpolluting energy sources. In this field, hybrid and inorganic perovskite, which is a semiconductor, has been shown to function efficiently in the solar cell. One of the unique properties of perovskite allows it to become semitransparent—not just by controlling its optical properties. In this review we provide the most updated methods and techniques to make semitransparent perovskite solar cells: (i) the use of thin perovskite film; (ii) the possibility to self-assemble the perovskite on a photoanode, providing an empty transparent area while not sacrificing the light harvesting efficiency; (iii) the use of the solvent properties to form islands of perovskite using de-wetting on the surface; and (iv) the possibilities to form a transparent contact that makes the solar cell fully semitransparent. Finally, the potential and future features of semitransparent perovskite solar cells are presented.
关键词： Transparent Contact,Dewetting,Solar Cells,Perovskite,Thin Films,Semitransparent,Self-assembly
更新于2025-09-23 15:21:01
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Exploiting Wavelength Orthogonality for Successive Photoinduced Polymerization-Induced Self-Assembly and Photo-Crosslinking
摘要： We report a facile benchtop process for the synthesis of cross-linked polymeric nanoparticles by exploiting wavelength-selective photochemistry to perform orthogonal photoinduced polymerization-induced self-assembly (Photo-PISA) and photo-crosslinking processes. We first established that the water-soluble photocatalyst, zinc meso-tetra(N-methyl-4-pyridyl) porphine tetrachloride (ZnTMPyP) could activate the aqueous PET-RAFT dispersion polymerization of hydroxypropyl methacrylate (HPMA). This photo-PISA process could be conducted under low energy red light (λ max = 595 nm, 10.2 mW/cm2) and without deoxygenation due to the action of the singlet oxygen quencher, biotin (vitamin B7), which allowed for the synthesis of a range of nanoparticle morphologies (spheres, worms, and vesicles) directly in 96-well plates. To perform wavelength selective nanoparticle cross-linking, we added the photoresponsive monomer, 7-[4-(trifluoromethyl)coumarin] methacrylamide (TCMAm) as a comonomer without inhibiting the evolution of the nanoparticle morphology. Importantly, under red light, exclusive activation of the photo-PISA process occurs, with no evidence of TCMAm dimerization under these conditions. Subsequent switching to a UV source (λ max = 365 nm, 10.2 mW/cm2) resulted in rapid cross-linking of the polymer chains, allowing for retention of the nanoparticle morphology in organic solvents. This facile synthesis of cross-linked spheres, worms, and vesicles demonstrates the utility of orthogonal light-mediated chemistry for performing decoupled wavelength selective chemical processes.
关键词： photoinduced polymerization-induced self-assembly,wavelength orthogonality,polymeric nanoparticles,photo-crosslinking,PET-RAFT polymerization
更新于2025-09-23 15:21:01
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The coupled dynamics of colloidal nanoparticle spreading and self-assembly at a fluid-fluid interface
摘要： We investigated the physicochemical and transport phenomena governing the self-assembly of colloidal nanoparticles at the interface of two immiscible fluids. By combining in-situ grazing incidence small-angle X-ray scattering (GISAXS) with a temporal resolution of 200 ms and electron microscopy measurements we gained new insights into the coupled effects of solvent spreading, nanoparticle assembly and recession of the vapor-liquid interface on the morphology of the self-assembled thin films. We focus on oleate-passivated PbSe nanoparticles dispersed across an ethylene glycol subphase as a model system and demonstrate how solvent parameters such as surface tension, nanoparticle solubility, aromaticity and polarity influence the mesoscale morphology of the nanoparticle superlattice. We discovered that a nanoparticle precursor monolayer film spreads in front of the bulk solution and influences the fluid spreading across the subphase. Improved understanding of the impact of kinetic phenomena (i.e., solvent spreading and evaporation) on superlattice morphology is important to describe the formation mechanism and ultimately enable assembly of high-quality superlattices with long range order.
关键词： self-assembly,interfacial phenomena,in-situ GISAXS,nanoparticle superlattice,spreading dynamics
更新于2025-09-23 15:21:01
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Binary Superlattices of Infrared Plasmonic and Excitonic Nanocrystals
摘要： Self-assembled superlattices of nanocrystals offer exceptional control over the coupling between nanocrystals, similar to how solid-state crystals tailor the bonding between atoms. By assembling nanocrystals of different properties (e.g., plasmonic, excitonic, dielectric, or magnetic), we can form a wealth of binary superlattice metamaterials with new functionalities. Here, we introduce infrared plasmonic Cu2?xS nanocrystals to the limited library of materials that have been successfully incorporated into binary superlattices. We are the first to create a variety of binary superlattices with large excitonic (PbS) nanocrystals and small plasmonic (Cu2?xS) nanocrystals, both resonant in the infrared. Then, by controlling the surface chemistry of large Cu2?xS nanocrystals, we produced structurally analogous superlattices of large Cu2?xS and small PbS nanocrystals. Transmission electron microscopy (TEM) and grazing-incidence small-angle X-ray scattering (GISAXS) were used to characterize both types of superlattices. Furthermore, our unique surface modification of the large Cu2?xS nanocrystals also prevented them from chemically quenching the photoluminescence of the PbS nanocrystals, which occurred when the PbS nanocrystals were mixed with unmodified Cu2?xS nanocrystals. These synthetic achievements create a set of binary superlattices that can be used to understand how infrared plasmonic and excitonic nanocrystals couple in a variety of symmetries and stoichiometries.
关键词： infrared quantum dots,nanocrystals,self-assembly,supracrystal,metamaterial,binary superlattice,grazing-incidence small-angle X-ray scattering (GISAXS)
更新于2025-09-23 15:21:01
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Reduced Graphene Oxide Aerogels with Uniformly Self-Assembled Polyaniline Nanosheets for Electromagnetic Absorption
摘要： Reduced Graphene Oxide (RGO)/polyaniline (PANI) composite aerogels (GPA) with uniformly distributed PANI nanosheets were prepared by a facile self-assembly way. The fabricated hybrids present a cross-linked three-dimensional(3D) porous network and RGO sheets were covered by PANI sheets with controlled content. The unique architecture efficiently reduced agglomeration of RGO and enhanced the conductive loss of the material to incident wave. Specifically, the GPA composite with 50 wt% PANI showed excellent electromagnetic wave absorption capacity, the largest reflection loss (RL) value reached -48 dB with fill loading of only 3% and the qualified bandwidth (RL ≤-10 dB) covered the entire Ku band (12-18 GHz). The study is expected to pave the way to prepare wide qualified bandwidth and lightweight graphene-based electromagnetic wave absorption hybrids with controlled microstructure.
关键词： conductive network,3D porous structure,electromagnetic wave absorption,self-assembly,light weight
更新于2025-09-23 15:21:01
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Ordered Mesoporous TiO <sub/>2</sub> Gyroids: Effects of Pore Architecture and Nb-Doping on Photocatalytic Hydrogen Evolution under UV and Visible Irradiation
摘要： Pure and Nb-doped TiO2 photocatalysts with highly ordered alternating gyroid architecture and well-controllable mesopore size of 15 nm via co-assembly of a poly(isoprene)-block-poly(styrene)-block-poly(ethylene oxide) block copolymer are synthesized. A combined effort by electron microscopy, X-ray scattering, photoluminescence, X-ray photoelectron spectroscopy, Raman spectroscopy, and density functional theory simulations reveals that the addition of small amounts of Nb results in the substitution of Ti4+ with isolated Nb5+ species that introduces inter-bandgap states, while at high concentrations, Nb prefers to cluster forming shallow trap states within the conduction band minimum of TiO2. The gyroidal photocatalysts are remarkably active toward hydrogen evolution under UV and visible light due to the open 3D network, where large mesopores ensure efficient pore diffusion and high photon harvesting. The gyroids yield unprecedented high evolution rates beyond 1000 μmol h?1 (per 10 mg catalyst), outperforming even the benchmark P25-TiO2 more than fivefold. Under UV light, the Nb-doping reduces the activity due to the introduction of charge recombination centers, while the activity in the visible triple upon incorporation is owed to a more efficient absorption due to inter-bandgap states. This unique pore architecture may further offer hitherto undiscovered optical benefits to photocatalysis, related to chiral and metamaterial-like behavior, which will stimulate further studies focusing on novel light–matter interactions.
关键词： photocatalysis,block copolymers,titanium dioxide,self-assembly
更新于2025-09-23 15:21:01