Rich oxygen vacancies (OVs) in a semiconductor are crucial for solar-driven water purification. Herein, we report an eco-friendly and energy-efficient strategy to fabricate mesoporous black TiOC with high concentrations of both surface and bulk OVs. Our approach leverages the microenvironment-regulated decomposition of diglyceryl ether (D100)-a biomass-derived derivative of glycerol-during the low-temperature calcination of polymeric coordination gels. We demonstrate that the coordination microenvironment dictates the D100 decomposition pathway: the oxygen-rich surface facilitates complete oxidation to generate surface OVs, while the oxygen-deficient interior directs the dehydration and aromatization-condensation of D100 and yields aromatic carbon doping and the associated stable bulk OVs. The resulting TiOC-2 material exhibits broad-spectrum absorption spanning the UV-vis-NIR region and enhanced non-radiative recombination, achieving a rapid photothermal temperature rise of over 20 degrees C within only 90 seconds. When integrated into a self-floating aerogel (TiOC@SA-TiOC), the system achieves a high solar evaporation rate of 2.61 kg m(-2) h(-1) under 1 sun illumination. This work pioneers a green and scalable approach for the direct conversion of bio-based chemicals into high-performance, multifunctional semiconductors, addressing critical needs in the energy-water nexus.
The miniature sensor for volatile organic compounds (VOCs) detection has attracted considerable interest due to its wide application in chemical and biological fields. Here we propose and demonstrate a multi-core fiber-tip polymer Mach-Zehnder interferometer (MZI) fabricated via two-photon polymerization (TPP) for VOCs concentration sensing. The miniaturized MZI sensor comprises a dual-waveguide structure printed on the multi-core fiber (MCF). Light launched from one core of the MCF is split into two polymer waveguides of unequal lengths, which subsequently recombine and interfere at the output core. Our results indicate that the optimal spectral performance is achieved when the two waveguides are arranged with a specific angular separation. The sensor's performance was characterized by immersing it in different types of VOCs and a sensitivity of 2.06 pm/ppm for isopropanol detection was achieved. The MZI design implemented on the MCF enables precise control over sensor dimensions, facilitates VOCs sensing in restricted spaces and shows the potential in the field of biometrics and chemistry.
Interfacial interactions between organic molecules and inorganic substrates play an important role in ion exchange, immobilization, and adsorption, which affect contaminant removal in aquatic environments. Here, we develop a transferable model using readily accessible descriptors that can be applied across distinct organic-inorganic interfacial systems. The model was trained on density functional theory (DFT) data of three antibiotics (tetracycline, ciprofloxacin, and berberine hydrochloride) adsorbed on the modified TiO2 surface, and implemented to predict adsorption energies of antibiotics on three other kinds of clay minerals (rectorite, montmorillonite, and vermiculite) with satisfactory performance (R2 = 0.75). The uppermost Ti atoms on the TiO2 surface are the potential active sites for hosting organic molecules, whereas the surface oxygen atoms on the clay minerals act as the primary interaction sites for adsorption. Using the Sure Independence Screening and Sparsifying Operator (SISSO) algorithm, we constructed composite descriptors of interfacial charge transfer and hydrogen bonding preference to rationalize the experimental removal efficiency of tetracycline on various substrates (with versus without light illumination) as well as the dye on TiO2. Applying this framework to methylene blue on P25 TiO2, we show that surface polarization and the dye's electronic structure properties dictate adsorption and photocatalytic efficiency, which can be further enhanced through Bayesian-optimized reaction conditions. This study provides a transferable, physically interpretable framework for understanding and predicting complex organic-inorganic interfacial interactions, and offers mechanistic guidance for designing functional interfaces for contaminant removal.
Altermagnetism has recently drawn considerable attention in three- and twodimensional materials. Here, we extend this concept to quasi-one-dimensional (Q1D) monolayers assembled from single-atomic magnetic chains. Through systematically examining nine types of structures, two stacking orders, and intra-/inter-chain magnetic couplings, we identify four out of thirty promising structural prototypes for hosting altermagnetism, which yields 192 potential monolayer materials. We further confirm eight thermodynamically stable Q1D monolayers via high-throughput calculations. Using symmetry analysis and first-principles calculations, we find that the existence of altermagnetism is determined by the type of inter-chain magnetic coupling and predict three intrinsic altermagnets,CrBr_3,VBr_3,MnBr_3,due to their ferromagnetic inter-chain couplings and five extrinsic ones,CrF_3,CrCl_3,CrI_3,FeCl_3and CoTe_3, ascribed to their neglectable or antiferromagnetic inter-chain couplings. Moreover, the inter-chain magnetic coupling here is highly tunable by manipulating the inter-chain spacing, leading to experimentally feasible transitions between altermagnetic and nodal-line semiconducting states. In addition, applying external electric fields can further modulate the spin splitting. Our findings establish a highly tunable family of Q1D altermagnets, offering fundamental insights into the intricate relationship between geometry, electronic structure, and magnetism.These discoveries hold significant promises for experimental realization and future spintronic applications.
We propose and demonstrate a multicore fiber-tip polymer Mach-Zehnder interferometer manufactured by two-photon polymerization for breath monitoring. The multicore fiber-tip sensor has the characteristics of ultracompactness, fast, and flexibility, and it is promising to be a useful tool for non-contract breath monitoring.
We propose a novel 3D shape reconstruction method for multi-core optical fibers using a space curve helical extension approach. Compared with the traditional Frenet-Serret reconstruction method, this approach regards the arc-length element of the space curve as a helical segment for simultaneous bending and torsion measurement. The method performs non-uniform interpolation optimization algorithm with high curvature variation rates and abrupt curvature direction changes. Experimental results demonstrate that this approach enhances the reconstruction accuracy of 3D space curves, showing significant potential for advanced fiber optic shape sensing applications.
We propose and demonstrate a multi-core fiber-tip polymer Mach-Zehnder interferometer manufactured by two-photon polymerization for Volatile Organic Compound Concentration Sensing. As MCF have characteristics of high integration and small size, high-sensitivity gas concentration measurement can be achieved on a micro-nano scale platform.
We demonstrate an efficient method for reversely tailoring the tubes of an antiresonant hollow-core fiber (AR-HCF). Furthermore, we have achieved and characterized the tapered AR-HCF with elliptical-shaped tubes, implemented by a traditional flame brushing technique. The measured results show that the extra loss as small as 0.1 dB in the passband and the out-of-band suppression of up to 28 dB in the lossband are realized. The ability to tailor the shape and thickness of tubes of AR-HCF in a submicron-scale using a traditional flame taper rig will benefit the fabrication of in-fiber HCF devices such as the low-loss HCF bandpass filter with high out-of-band suppression.
We report a simple and effective approach to reversely tailoring the tubes of an antiresonant hollow-core fiber (AR-HCF). The AR-HCFs with elliptical-shaped shrinkage tubes, implemented by a traditional flame brushing technique, were characterized for what we believe to be the first time. We have thus achieved a 70 nm wide bandpass filter with a minimum extra loss below 0.1 dB and the out-of-band suppression up to 28 dB in the 800 nm wide spectral range via the combination of down-tapering and reverse-tapering of AR-HCFs. The elliptical-shaped tubes can reduce the deformation-induced confinement loss when tailoring the thickness of HCF. The ability to tailor the shape and thickness of tubes of AR-HCF in a submicron-scale using a traditional flame taper rig will benefit the fabrication of in-fiber HCF devices such as the low-loss HCF bandpass filter with high out-of-band suppression.
A multicore fiber-tip whispering-gallery-mode resonator was proposed and demonstrated. The resonator was manufactured by two-photon polymerization, and was used to detect the concentration of volatile organic compounds. The ultracompact probe sensor is expected to be applied in some biochemical scenarios.
In this study, a novel method is presented for enhancing second harmonic generation (SHG) by exploiting the natural Fabry‐Pérot cavity effect within PCN‐250 metal‐organic framework (MOF) microplates. PCN‐250, recognized for its chemical stability and moisture resistance, exhibits strong anisotropic second‐order nonlinear susceptibility, making it an excellent candidate for SHG applications. By harnessing the cavity‐controlled SHG emission, a significant enhancement in SHG efficiency under 1030 nm femtosecond laser excitation is achieved. The study involved eight single‐crystalline microplates with varying thicknesses, demonstrating a tenfold increase in SHG signal strength when the detuning (Δ) between the cavity mode and SHG signal is approximately zero. Simulations using a nonlinear transfer matrix method (TMM) confirms that resonance‐driven SHG enhancement occurred only at 1030 nm, with a selective nonlinear optical filtering effect. This approach introduces a cost‐effective technique for developing highly efficient SHG materials, with broad applications in telecommunications, sensing, and quantum optics.
Organometallic halide perovskites have attracted attention due to their excellent optical properties. However, the inherent instability limits their wide application in the field of optoelectronics. In this study, a distribution...
Individual superatoms are assembled into more complicated nanostructures to diversify their physical properties. Magnetism of assembled superatoms remains, however, ambiguous, particularly in terms of its distance dependence. Here, we report density functional theory calculations on the distance-dependent magnetism of transition metal embedded Au6Te8Se12 (ATS) superatomic dimers. Among the four considered transition metals, which include V, Cr, Mn and Fe, the Cr-embedded Au6Te12Se8 (Cr@ATS) is identified as the most suitable for exploring the inter-superatomic distance-dependent magnetism. We thus focused on Cr@ATS superatomic dimers and found an inter-superatomic magnetization-distance oscillation where three transitions occur for magnetic ordering and/or anisotropy at different inter-superatomic distances. As the inter-superatomic distance elongates, a ferromagnetism (FM)-to-antiferromagnetic (AFM) transition and a sequential AFM-to-FM transition occur, ascribed to competitions among Pauli repulsion and kinetic-energy-gains in formed inter-superatomic Cr-Au-Au-Cr covalent bonds and Te-Te quasi-covalent bonds. For the third transition, in-plane electronic hybridization contributes to the stabilization of the AFM configuration. This work unveils two mechanisms for tuning magnetism through non-covalent interactions and provides a strategy for manipulating magnetism in superatomic assemblies.
Many intriguing quantum states of matter, such as unconventional superconductivity, magnetic phases and fractional quantum Hall physics, emergent from the spatially-correlated localized electrons in the flat band of solid materials. By using scanning tunneling microscopy and spectroscopy (STM/STS), we report the real-space investigation of correlated electrons in the flat band of superlattice 4Hb-TaSexS2-x. In contrast with the pristine 4Hb-TaS2, the selenium (Se) substitutions significantly affect the interfacial transfer of correlated electrons between the CDW states of 1T- and 1H-TaS2 layers, and contribute a real-space fractional electron-filling configurations with the distributed electron-filled and -void SoD clusters of 1T-layer. The site-specific STS spectra directly reveal their respective prominent spectra weight above EF and symmetric Mott-like spectra. In addition, the spatial distributions of these electron-filled SoDs in the 1T-layer of 4Hb-TaSe0.7S1.3 demonstrate different local short-range patterning, clearly indicating the complex neighboring interactions among the localized electrons in the flat band of 1T-layer. Our results not only provide an in-depth insight of correlated electrons in the flat CDW band, and provide a simple platform to manipulate the electron-correlation-related quantum states.
Optical fiber force sensing has attracted considerable interest in biological, materials science, micromanipulation, and medical applications owing to its compact and cost-efficient configuration. However, the glass fiber has an intrinsic high Young's modulus, resulting in force sensors being generally less sensitive. While hyperelastic polymer materials can be utilized to enhance the force sensitivity, the thermodynamic properties of the polymer may weaken the sensing accuracy and reliability. Herein, we demonstrate ultracompact three-dimensional (3D)-printed multicore fiber (MCF) tip probes for simultaneous measurement of nanoforce and temperature with high sensitivity. The sensor is highly sensitive to force-induced deformation due to the special geometric features of the polymer microcantilever, and the high-temperature sensitivity can be implemented through the poly(dimethylsiloxane) (PDMS) microcavity on the same fiber facet. Moreover, the sensitivities of the fiber interferometers are remarkably enhanced by introducing the optical analogue of the Vernier effect. Such a device exhibits a force sensitivity of 56.35 nm/μN, which is more than 103 times that of all-silica fiber force sensors. The PDMS microcavity provides a temperature sensitivity of 1.447 nm/°C, measuring the local temperature of the probe and compensating for temperature crosstalk of the force detection. The proposed compact MCF-tip sensor can simultaneously measure nanoforce and temperature with high sensitivity, facilitating multiparameter sensing in a restricted space environment and showing the potential in miniaturized all-fiber multiparameter sensors.
Synergistic transformation of N-cyclic organics and Cr( vi ) under neutral condition. Fenton chemistry and photogenerated charge separation promote mutually. Se provides acidic surface microenvironment for high photocatalytic adaptability.
We investigate composed image retrieval with text feedback. Users gradually look for the target of interest by moving from coarse to fine-grained feedback. However, existing methods merely focus on the latter, i.e., fine-grained search, by harnessing positive and negative pairs during training. This pair-based paradigm only considers the one-to-one distance between a pair of specific points, which is not aligned with the one-to-many coarse-grained retrieval process and compromises the recall rate. In an attempt to fill this gap, we introduce a unified learning approach to simultaneously modeling the coarse- and fine-grained retrieval by considering the multi-grained uncertainty. The key idea underpinning the proposed method is to integrate fine- and coarse-grained retrieval as matching data points with small and large fluctuations, respectively. Specifically, our method contains two modules: uncertainty modeling and uncertainty regularization. (1) The uncertainty modeling simulates the multi-grained queries by introducing identically distributed fluctuations in the feature space. (2) Based on the uncertainty modeling, we further introduce uncertainty regularization to adapt the matching objective according to the fluctuation range. Compared with existing methods, the proposed strategy explicitly prevents the model from pushing away potential candidates in the early stage, and thus improves the recall rate. On the three public datasets, i.e., FashionIQ, Fashion200k, and Shoes, the proposed method has achieved +4.03%, +3.38%, and +2.40% Recall@50 accuracy over a strong baseline, respectively.
Solid-state hybrid materials with designability in topology and tunable photo-responsiveness hold great promise for multitudinous applications from optoelectronics to information storage/communication. However, the judicious design and synthesis of metal-organic frameworks (MOFs) with intrinsically custom-made nonlinear optical (NLO) properties including multiple photon absorption and harmonic generation effects suitable for miniaturized devices remain highly challenging. Herein, the design and synthesis of a novel pillared framework named after Zn-TCPE-DPNI MOF coordinated by zinc ions (Zn2+), aggregation induced emission (AIE) featured [1,1 '-biphenyl]-4-carboxylic acid (H4TCPE), and N,N '-di(4-pyridyl)-1,4,5,8-naphthalenetetracarboxydiimide (DPNI) are reported. The highly ordered Zn-TCPE-DPNI MOF single crystal exhibits tunable NLO responses by switching incident excitation wavelengths of a femtosecond laser from 900 to 1500 nm. The noticeable transformation from two- or three-photon excited photoluminescence (2PL or 3PL) to the concurrent occurrence of 3PL and third harmonic generation (THG), and eventually to the mere emergence of THG with a high effective susceptibility chi(3) (3 omega) of 2.9 x 10-12 esu is observed. This study paves a novel avenue for the design and synthesis of photoluminescent MOF crystals with tunable NLO responses toward the fabrication of multifunctional NLO devices targeted for optoelectronics and information communication. The design and synthesis of Zn-TCPE-DPNI MOF single crystals exhibiting tunable NLO responses is presented. Noticeable transformation from two- or three-photon excited photoluminescence (2PL or 3PL) to the concurrent occurrence of 3PL and third harmonic generation (THG), and eventually to the mere emergence of THG with a high effective susceptibility chi(3) (3 omega) of 2.9 x 10-12 esu is observed.image
The van der Waals interface structures and behaviors are of great importance in determining the physical properties of two-dimensional atomic crystals and their heterostructures. The delicate interfacial properties are sensitively dependent on the mechanical behaviors of atomically thin films under external strain. Here, we investigated the strain-engineered rippling structures at the CVD-grown bilayer-MoS2 interface with advanced atomic force microscopy (AFM). The in-plane compressive strain is sequentially introduced into the 1L-substrate and 2L-1L interface of bilayer-MoS2 flakes via a fast-cooling process. The thermal strain-engineered rippling structures were directly visualized at the central 2H- and 3R-MoS2 bilayer regions with friction force microscopy (FFM) and bimodal AFM techniques. These rippling structures can be further artificially manipulated into the beating-like rippling features and fully erased via the contact mode AFM scanning. Our results shed lights on the strain-engineered interfacial structures of two-dimensional materials and also inspire the further investigation on the interface engineering of their electronic and optical properties.