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Triplet‐Triplet Annihilation Upconversion in a MOF with Acceptor‐filled Channels
摘要： Photon upconversion enjoys an increasing interest in the last years due to its high potential for solar energy harvesting and in bio-imaging. A challenge for triplet-triplet annihilation upconversion (TTA-UC) processes is to realize these features in solid materials without undesired phase segregation and detrimental dye aggregation. To achieve this, we combine a palladium porphyrin sensitizer and a 9,10-diphenylanthracene annihilator within a crystalline mesoporous metal-organic framework using an inverted design. In this modular TTA system, the framework walls constitute the fixed sensitizer, while caprylic acid coats the channels providing a solvent-like environment for the mobile annihilator in the channel. The resulting solid material shows green-to-blue delayed upconverted emission with a luminescence lifetime of 373±5 μs, a threshold value of 329 mW cm–2 and a triplet-triplet energy transfer efficiency of 82%. The versatile design allows straightforward changing the acceptor amount and type.
关键词： triplet-triplet annihilation,porphyrins,metal-organic frameworks,upconversion,hybrid materials
更新于2025-09-11 14:15:04
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Understanding Solid-State Solvation-Enhanced Thermally Activated Delayed Fluorescence Using a Descriptor-Tuned Screened Range-Separated Functional
摘要： An efficient computational protocol suitable for both solutions and solid films can accelerate the development of efficient thermally activated delayed fluorescence (TADF) emitters aimed at practical application in organic light-emitting diodes (OLEDs). By employing the localized orbital locator (LOL), we establish an efficient descriptor-tuning methodology for the range-separated (RS) and screened range-separated (SRS) functionals with only one single-point calculation. This scheme provides good predictions for 28 charge transfer (CT)-type TADF emitters. Moreover, in comparison to the experimental data, the scheme presents a mean absolute deviation of 0.09 eV for the absorption energies of the lowest excited singlet state (EVA(S1)) in polarizable continuum model (PCM) solution and 0.10 eV for the energy difference between the lowest excited singlet and triplet states (ΔEST) under static solid-state polarization. Importantly, our results indicate that a significantly polarized S1 is key to realizing the so-called solid-state solvation-enhanced (SSSE)-TADF, which is well captured through the screened RS functionals combined with LOL-tuning (SLOL-tuning). Compared with standard ionization potential (IP)-tuning, our scheme significantly reduces the computational cost of the prediction of singlet- and triplet-transition energies for CT molecules. It also provides a reliable approach to evaluate the practical TADF character influenced by solid-state solvation in amorphous organic thin films.
关键词： Thermally Activated Delayed Fluorescence,Optical,Solid-State Solvation-Enhanced,Plasmonics,Magnetic,Hybrid Materials,TADF,Range-Separated Functional,LOL-tuning,OLEDs
更新于2025-09-11 14:15:04
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Stable Structural Phase of Potassium-Doped <i>p</i> -Terphenyl and Its Semiconducting State
摘要： The potassium-doped p-terphenyl compounds were synthesized in recent experiments and the superconductivity with high transition temperatures were reported, but the atomic structure of potassium-doped p-terphenyl is unclear. In this paper, we studied the structural and electronic properties of potassium-doped p-terphenyl with various doping levels by the first-principles simulation. We first find out the low energy position of K atom in intralayer interstitial space of the molecular layer, then examine whether two rows of K atoms can be accommodated in this one space, at last the effect of the interlayer arrangement between adjacent two molecular layers on total energy is taken into account. Our results show that the doped K atoms prefer to stay at the bridge site of single C-C bond connected two phenyls instead of locating at the site above the phenyl ring, distinct from the situation of K-doped picene and phenanthrene. Among the possible structural phases of Kx-p-terphenyl, the K2-p-terphenyl phase with P212121 group symmetry is determined to be most appropriate, which is different from the one in recent report. The stable K2-p-terphenyl phase is semiconducting with an energy gap of 0.3 eV and the bands from the lowest unoccupied molecular orbitals are just fully filled by the electrons transferred from K atoms.
关键词： Plasmonics,First-principles simulation,Semiconducting state,Magnetic,Potassium-doped p-terphenyl,Superconductivity,Optical,Hybrid Materials
更新于2025-09-10 09:29:36
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A novel strategy to modify the surface of plasma electrolysis produced inorganic coatings for fabricating organic@functional binding agents@inorganic materials
摘要： Organic@functional binding agents(FBAs)@inorganic materials are fabricated using two efficient methods. For this purpose, inorganic layer containing organically magnesium aluminate loaded with metal hydroxide, namely (Mg(OH)2 or/and Ni(OH)2), and 2-mercaptobenzimidazole (MBI) were produced on Mg-3%Al-1%Zn alloy via plasma electrolysis (PE) method and then two-step dip chemical coating (DCC) method. The presence of metal hydroxides resulted in a decrease in the porosity and microcracks and an increase in strong bonds between organic and inorganic coating. Thus, it was found that the hybrid 2-mercaptobenzimidazole and metal hydroxides materials act good corrosion inhibitors for magnesium corrosion in aqueous solutions.
关键词： Hybrid materials,Dip chemical coating,2-Mercaptobenzimidazole,Organic coating
更新于2025-09-10 09:29:36
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The Surface and Interface Engineering Multi-Layered Nanopore Films for Enhanced Fabry-Pérot Interferences
摘要： In this study, a broadly-tunable nanoporous thin film system with alternating layers of Ag/indium tin oxide (ITO)/CoFeB/ITO/Ag, which was fabricated on a porous anodic aluminum oxide (AAO) substrate, was presented, so as to achieve the flexible tailoring of the Fabry-Pérot interference. The experimental results demonstrated that the amplitude of the Fabry-Pérot interference of this system, which had only an Ag layer deposited on the AAO substrate, was 12 times higher than that of pure AAO film, aside from the tunable oscillation periods. This was mainly due to the fact that the Ag mirror greatly improved the reflectivity of the air/AAO interface, rendering the intensities of light reflected from the air/AAO and AAO/Al interfaces comparable, thereby forming an effective interference enhancement. Furthermore, the existence of the ferromagnetic CoFeB layer was capable of significantly improving the absorbance in the ultraviolet and visible spectral ranges, and, in particularly, the oscillation ranges could be extended to the near-infrared spectral range (> 2,600 nm) by utilizing an ITO with lower conductivity as a spacer layer, due to its material dispersion which was approximately equal to zero. This new nanoporous thin film system represents a powerful tool for the future development of ultrasensitive optical devices based on the Fabry-Pérot interference and investigation of many interesting physical phenomena.
关键词： Ag/ITO/CoFeB/ITO/Ag layers,Hybrid Materials,Magnetic,Plasmonics,AAO substrate,Fabry-Pérot interference,Nanoporous thin film,Optical
更新于2025-09-10 09:29:36
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Visible Light-Promoted Plasmon Resonance to Induce “Hot” Hole Transfer and Photothermal Conversion for Catalytic Oxidation
摘要： Titanium dioxide (TiO2) semiconductor photocatalysts were photosensitized to the visible spectrum with gold nanospheres (AuNSs) and gold nanorods (AuNRs) to study the ethanol photo-oxidation cycle, with an emphasis towards driving carbon-carbon (C-C) bond cleavage at low temperatures. The photocatalysts exhibited a localized surface plasmon resonance (SPR) that was harnessed to drive the complete photo-oxidation of formic acid (FA) and ethanol (EtOH) via augmented carrier generation/separation and photothermal conversion. Contributions of transverse and longitudinal localized SPR modes were decoupled by irradiating AuNSs-TiO2 and AuNRs-TiO2 with targeted wavelength ranges to probe their effects on plasmonically-assisted photocatalytic oxidation of FA and EtOH. Photocatalytic performance was assessed by monitoring the yield of gaseous products during photo-oxidation experiments using a gas chromatography-mass spectrometry-multiple headspace extraction (GC-MS-MHE) analysis method. The complete oxidation of EtOH to CO2 under visible-light irradiation was confirmed by GC-MS-MHE for both AuNSs and AuNRs on TiO2 at room temperature. Photothermal and local field enhancements were found to aid in selectively cleaving the C-C bond in EtOH to form FA, while FA was further oxidized to CO2 by plasmon-induced electron transfer mechanisms. Under visible light (>420 nm) irradiation, carrier generation/separation and photothermal conversion was achieved, resulting in the photogenerated “hot” holes driving the photo-oxidation primarily on the AuNPs. Specifically, plasmonic enhancement by AuNR-TiO2 enhances EtOH oxidation, providing a method to selectively cleave C-C bonds.
关键词： Carbon-carbon bond cleavage,Photocatalysis,Hybrid Materials,Gold nanoparticles,Ethanol oxidation,Magnetic,Formic acid oxidation,Plasmonics,TiO2,Optical
更新于2025-09-10 09:29:36
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Synthesis, Characterisation and Applications of Polymer–Silica Core–Shell Microparticle Capsules
摘要： Encapsulation is a powerful method for the targeted delivery of concentrated reagents, as well as capture of valuable materials in dilute systems. To this end, many encapsulation schemes for specific scenarios have been devised, that incorporate chemospecificity or stimulus response in terms of uptake or release. However, an encapsulation platform that enables highly tailorable surface chemistry for targeting, stimulus response, and core chemistry for capture and release of reagents remains elusive. Here we present such a system comprising composite core–shell capsule particles of hydrophilic polymers coated with thin silica layers, synthesised via straightforward one-pot syntheses. Silica is found to encapsulate a range of polymer hydrogels through a mechanism independent of the specific core chemistry. The hybrid materials possess significantly enhanced rigidity, while allowing surface modification through simple yet versatile silane coupling reactions without a reduction in the functionality of the core. They are shown to have applications as diverse as recyclable catalysis and controlled delivery vehicles for agrochemicals. The successful synthesis and utilisation of this catalogue of materials indicates the broader capability of simple composite structures in an array of high value applications.
关键词： catalysis,silica,microgel,encapsulation,Hybrid materials
更新于2025-09-10 09:29:36
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Organic and hybrid resistive switching materials and devices
摘要： The explosive increase in digital communications in the Big Data and internet of Things era spurs the development of universal memory that can run at high speed with high-density and nonvolatile storage capabilities, as well as demonstrating superior mechanical flexibility for wearable applications. Among various candidates for the next-generation information storage technology, resistive switching memories distinguish themselves with low power consumption, excellent downscaling potential, easy 3D stacking, and high CMOS compatibility, fulfilling key requirements for high-performance data storage. Employing organic and hybrid switching media in addition allows light weight and flexible integration of molecules with tunable device performance via molecular design-cum-synthesis strategy. In this review, we present a timely and comprehensive review of the recent advances in organic and hybrid resistive switching materials and devices, with particular attention on their design principles for electronic property tuning and flexible device performance. The current challenges posed with development of organic and hybrid resistive switching materials and flexible memory devices, together with their future perspectives, are also discussed.
关键词： flexible electronics,organic materials,resistive switching memories,nonvolatile storage,hybrid materials
更新于2025-09-09 09:28:46
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New organic dye/anionic clay hybrid pigments: Preparation, optical properties and structural stability
摘要： Encapsulation and subsequent stabilization of organic dye into layered double hydroxides (LDHs) are investigated. Three commercialized dye molecules such as: acid orange 6, acid yellow 50 and acid green 25, were intercalated in Zn2-Al-LDH by co-precipitation method, analyzed by ICP and UV–Visible, and characterized by XRD at di?erent temperatures. Functionalized organic molecules have been interleaved for the synthesized hybrid LDH materials. It is shown that the e?ect of encapsulation is revealed by the di?erent interactions according to the molecule size and stacking of dye molecules. Thermal behavior of hybrid materials showed a clear enhancement of the structural stability in temperature over the chloride-Zn2Al LDH, indicating that the assembly may appear as a mutual bene?t.
关键词： LDHs,Hybrid materials,Acid yellow 50,Acid orange 6,Acid green 25,Anionic dye
更新于2025-09-09 09:28:46
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Effects of Rare-Gas Matrices on the Optical Response of Silver Nanoclusters
摘要： The optical response of silver clusters, Agn with n = 8, 20, 35, 58, 92, embedded in a rare-gas matrix are calculated in the framework of the Time-Dependent Density Functional Theory (TDDFT). We present a methodology able to reproduce with unprecedented accuracy the experimental spectra measured on metal clusters embedded in neon, argon, krypton and xenon solid matrices. In our approach, the metal cluster is surrounded by explicit rare-gas atoms and embedded in a polarizable continuum medium. Interactions with the surrounding medium affects both the position and the width of the surface plasmon absorption band of metal clusters. The size dependent shift of the surface plasmon band is evaluated in the case of a neon matrix. While the band shifts to lower energies (red shift) for large clusters, it shifts to higher energies (blue shift) for very small clusters.
关键词： Silver Nanoclusters,Optical,TDDFT,Plasmonics,Magnetic,Hybrid Materials,Rare-Gas Matrices
更新于2025-09-09 09:28:46