Pulsed Optical Vortex Array Generation in a Self-Q-Switched Tm:YALO3 Laser.

Optical vortex arrays are characterized by specific orbital angular momentums, and they have important applications in optical trapping and manipulation, optical communications, secure communications, and high-security information processing. Despite widespread research on optical vortex arrays, the 2 µm wavelength range remains underexplored. Pulsed lasers at 2 µm are vital in laser medicine, sensing, communications, and nonlinear optic applications. The need for 2 µm-pulsed structured optical vortices, combining the advantages of this wavelength range and optical vortex arrays, is evident. Therefore, using just three elements in the cavity, we demonstrate a compact self-Q-switched Tm:YALO3 vortex laser by utilizing the self-modulation effect of a laser crystal and a defect spot mirror. By tuning the position of the defect spot and the output coupler, the resonator delivers optical vortex arrays with phase singularities ranging from 1 to 4. The narrowest pulse widths of the TEM00 LG0,-1, two-, three-, and four-vortex arrays are 543, 1266, 1281, 2379, and 1615 ns, respectively. All the vortex arrays in our study have relatively high-power outputs, slope efficiencies, and single-pulse energies. This work paves the way for a 2 µm-pulsed structured light source that has potential applications in optical trapping and manipulation, free-space optical communications, and laser medicine.

In situ and Real-time Monitoring the Chemical and Thermal Evolution of Lithium-ion Batteries with Single-crystalline Ni-rich Layered Oxide Cathode.

High-capacity Ni-rich layered oxides are promising cathode materials for fabrication of lithium-ion batteries (LIBs) with high energy density. However, thermal runaway of LIBs with these cathodes leads to great safety concerns. In this study, single crystalline LiNi0.9Co0.05Mn0.05O2 (NCM-SC) has been prepared and a flexible optical fiber was buried inside the pouch-type LIBs with NCM-SC cathode to in situ study its real-time temperature evolution during charge/discharge process. NCM-SC exhibits an enhanced Li+ ions transportation efficiency and electrode reaction kinetics, which can effectively reduce the generation of polarization heat and mitigate the internal temperature rise of the pouch-type battery. Meanwhile, solid-electrolyte interface (SEI) film decomposition and gas accumulation are effectively alleviated, due to the enhanced thermal stability of SEI film formed on NCM-SC. Moreover, the single crystal architecture can effectively retard layered to spinal and rock-salt phase transition, mitigate the crack formation and structural collapse. Consequently, NCM-SC exhibits an excellent electrochemical performance and enhanced thermal stability.

Achieving High Activity and Long-Term Stability towards Oxygen Evolution in Acid by Phase Coupling between CeO2-Ir.

The development of efficient and stable catalysts with high mass activity is crucial for acidic oxygen evolution reaction (OER). In this study, CeO2-Ir heterojunctions supported on carbon nanotubes (CeO2-Ir/CNTs) are synthesized using a solvothermal method based on the heterostructure strategy. CeO2-Ir/CNTs demonstrate remarkable effectiveness as catalysts for acidic OER, achieving 10.0 mA cm-2 at a low overpotential of only 262.9 mV and maintaining stability over 60.0 h. Notably, despite using an Ir dosage 15.3 times lower than that of c-IrO2, CeO2-Ir/CNTs exhibit a very high mass activity (2542.3 A gIr-1@1.53 V), which is 58.8 times higher than that of c-IrO2. When applied to acidic water electrolyzes, CeO2-Ir/CNTs display a prosperous potential for application as anodic catalysts. X-ray photoelectron spectrometer (XPS) analysis reveals that the chemical environment of Ir nanoparticles (NP) can be effectively modulated through coupling with CeO2. This modulation is believed to be the key factor contributing to the excellent OER catalytic activity and stability observed in CeO2-Ir/CNTs.

Progress in Electrochemical Immunosensors with Alkaline Phosphatase as the Signal Label.

Electrochemical immunosensors have shown great potential in clinical diagnosis, food safety, environmental protection, and other fields. The feasible and innovative combination of enzyme catalysis and other signal-amplified elements has yielded exciting progress in the development of electrochemical immunosensors. Alkaline phosphatase (ALP) is one of the most popularly used enzyme reporters in bioassays. It has been widely utilized to design electrochemical immunosensors owing to its significant advantages (e.g., high catalytic activity, high turnover number, and excellent substrate specificity). In this work, we summarized the achievements of electrochemical immunosensors with ALP as the signal reporter. We mainly focused on detection principles and signal amplification strategies and briefly discussed the challenges regarding how to further improve the performance of ALP-based immunoassays.

Fabrication of Superhydrophobic Porous Brass by Chemical Dealloying for Efficient Emulsion Separation.

By taking advantage of typical dealloying and subsequent aging methods, a novel homogeneous porous brass with a micro/nano hierarchical structure was prepared without any chemical modification. The treatment of commercial brass with hot concentrated HCl solution caused preferential etching of Zn from Cu62Zn38 alloy foil, leaving a microporous skeleton with an average tortuous channel size of 1.6 µm for liquid transfer. After storage in the atmosphere for 7 days, the wettability of the dealloyed brass changed from superhydrophilic to superhydrophobic with a contact angle > 156° and sliding angle < 7°. The aging treatment enhanced the hydrophobicity of the brass by the formation of Cu2O on the surface. By virtue of the opposite wettability to water and oil, the aged brass separated surfactant-stabilized water-in-oil emulsions with separation efficiency of over 99.4% and permeate flux of about 851 L·m-2·h-1 even after recycling for 60 times. After 10 times of tape peeling or sandpaper abrasion, the aged brass maintained its superhydrophobicity, indicating its excellent mechanical stability. Moreover, the aged brass still retained its superhydrophobicity after exposure to high temperatures or corrosive solutions, displaying high resistance to extreme environments. The reason may be that the bicontinuous porous structure throughout the whole foil endows stable mechanical properties to tolerate extreme environments. This method should have a promising future in expanding the applications of alloys.

Enabling high rate capability and stability all-solid-state batteries via cationic surfactant modification of composite electrolyte.

The garnet-type solid electrolyte Li6.4La3Zr1.4Ta0.6O12 (LLZTO) was modified with a cationic surfactant Cetyltrimethylammonium Bromide (CTAB) to improve the dispersion of LLZTO inorganic particles in Poly (ethylene oxide) (PEO) electrolyte (PEO-LLZTO@CTAB) by a liquid phase casting method. During fabrication, the cationic modifier CTAB is uniformly adsorbed on the surface of LLZTO particles, which can effectively reduce their surface energy and lead to a thin CTAB surface coating layer. This fabricated PEO-LLZTO@CTAB can avoid the aggregation of LLZTO particles in the composite solid-state electrolyte (CSSE) and improve the interfacial contact at the PEO/LLZTO interface, thus reducing the overall resistance of PEO-LLZTO@CTAB/Li half-cell and inhibiting the dendrite growth during cycling. The all-solid-state batteries (ASSBs) with LiFePO4 (LFP) as the cathode, PEO-LLZTO@CTAB as the electrolyte and Li as the anode exhibit a high initial discharge capacity of 146.6 mAh-g-1, excellent rate performance and high-capacity retention of 91.0 % after 300 cycles at 0.2 C multiplier and 60 °C within the voltage range of 2.7-4.0 V.

Controlling the directional excitation of surface plasmon polaritons using tunable non-Hermitian metasurfaces.

In this work, we propose an efficient approach to controlling the directional excitation of surface plasmon polaritons (SPPs) by dynamically modulating the real-part perturbation in a passive parity-time symmetric metasurface. This non-Hermitian system can experience two exceptional points that can induce two unidirectional excitation states of SPPs along opposite directions. Empowered by its superior modulation depth, the energy ratio and energy intensities of two excited SPP states can be effectively manipulated by this non-Hermitian metasurface. To demonstrate these findings, we design and numerically verify non-Hermitian metasurfaces integrated with an Sb2Se3 phase-change material. Our work provides a promising platform for the controllable engineering of SPP excitations, holding significant potential for the development of new plasmonic devices, including on-chip SPP sources, routers and sorters, and integrated optical circuits.

Switchable supermode emission in a doubly-coupled-ring system for multifunctional integrated photonic devices.

Effective integration of optical modes within chip-scale devices is critical to realize functional light emission, as it offers abundant physics and a versatile ability to control the mode evolution. Here, we present an efficient approach to achieve switchable emission by flexibly controlling supermode states in a doubly-coupled-ring system with four guided modes. The lasing conditions, which rely on the system's Hamiltonian, are revealed to yield multiple supermode states, including an exceptional-point state, a (quasi-)dark state, and a bright state. By freely engineering the coupling rate via phase-change material, the proposed system allows the generation of any desired states, enabling switchable and multifunctional emissions in fixed on-chip structures. Beyond the manipulation of various supermode emission states, our work presents a promising path toward the development of multifunctional integrated photonic devices, which may have applications in light storage, optical isolation, sensing, and so on.

Vacancy engineering in Co-doped CuS1-x with fast Electronic/Ionic migration kinetics for efficient Lithium-Ion batteries.

Slow Li ion diffusion kinetics and disordered migration of electrons are two most crucial obstacles to be resolved in electrode material design for higher rate capability of Li-ion batteries. Herein, the Co-doped CuS1-x with abundant high active S vacancies is proposed to accelerate the electronic and ionic diffusion during the energy conversion process, because contraction of Co-S bond can cause the expansion of atomic layer spacing, thus promoting the Li ion diffusion and directional electron migration parallel to the Cu2S2 plane, and also induce the increasing of active sites to improve the Li+ adsorption and electrocatalytic conversion kinetics. Especially, the electrocatalytic studies and plane charge density difference simulations demonstrate that electron transfer near the Co site is more frequent, which is conducive to more rapid energy conversion and storage. Those S vacancies formed by Co-S contraction in CuS1-x structure obviously increase Li ion adsorption energy in Co-doped CuS1-x to 2.21 eV, higher than the 2.1 eV for CuS1-x and 1.88 eV for CuS. Taking these advantages, the Co-doped CuS1-x as anode of Li-ion batterie shows an impressive rate capability of 1309 mAh·g-1 at 1A g-1, and long cycling stability (retaining 1064 mAh·g-1 capacity after 500 cycles). This work provides new opportunities for the design of high-performance electrode material for rechargeable metal-ion batteries.

Tunable dual quasi-bound states in continuum and electromagnetically induced transparency enabled by the broken material symmetry in all-dielectric compound gratings.

Dual quasi-bound states in continuum (quasi-BICs) enabled by the broken geometric symmetry offer an effective way to design high-quality photonic devices, yet challenged by tunable functionalities. Here we employ the material asymmetry originating from the tunable material property of phase-change materials to design quasi-BICs in all-dielectric compound gratings. We find the even and odd quasi-BICs are modulated by the geometric and material asymmetries, respectively, and this effect is ensured by two different types of structural symmetries in the compound structure. Particularly, tunable electromagnetically induced transparency (EIT) can be achieved by modulating the material asymmetry. Furthermore, we systematically design the compound gratings consisting of the phase-change material of Sb2Se3 to demonstrate tunable dual quasi-BICs and EITs. Analytical calculations and numerical simulations are performed to verify these findings. Our work provides a promising way to enhance the flexibility of realizing quasi-BICs, which may boost tunable applications in nanodevices assisted by quasi-BICs.

PEDOT-intercalated NH4V3O8 nanobelts as high-performance cathode materials for potassium ion batteries.

Potassium ion batteries (PIBs) have great potential to replace lithium ion batteries (LIBs) for large-scale energy storage applications because of the low cost and earth abundance of potassium resources. However, it is critically challenging to exploit an appropriate cathode material to accommodate the large size of K+. Herein, a conducting polymer (PEDOT) intercalation method is utilized to tailor the interlayer spacing of NH4V3O8 nanobelts from 7.8 Å to 10.8 Å, and afford rich oxygen vacancies inside the vanadate, thus enhancing its electronic conductivity and accelerating the K+ insertion/extraction kinetics. Benefiting from these features, PEDOT-intercalated NH4V3O8 (PNVO) nanobelts deliver an improved capacity of 87 mA h g-1 at 20 mA g-1, high rate capability of 51 mA h g-1 at 500 mA g-1, and a stable cycle life (capacity retention of 92.5 % after 100 cycles at 50 mA g-1). Even cycled at 200 mA g-1, PNVO nanobelts feature a long cycle life over 300 cycles with a capacity retention of 71.7 %. This work is of great significance for exploitation of PIBs cathode with improved electrochemical performance through pre-intercalation and defect engineering.

Reconfigurable chiral exceptional point and tunable non-reciprocity in a non-Hermitian system with phase-change material.

Non-Hermitian optics has emerged as a feasible and versatile platform to explore many extraordinary wave phenomena and novel applications. However, owing to ineluctable systematic errors, the constructed non-Hermitian phenomena could be easily broken, thus leading to a compromising performance in practice. Here we theoretically proposed a dynamically tunable mechanism through GST-based phase-change material (PCM) to achieve a reconfigurable non-Hermitian system, which is robust to access the chiral exceptional point (EP). Assisted by PCM that provides tunable coupling efficiency, the effective Hamiltonian of the studied doubly-coupled-ring-based non-Hermitian system can be effectively modulated to resist the external perturbations, thus enabling the reconfigurable chiral EP and a tunable non-reciprocal transmission. Moreover, such tunable properties are nonvolatile and require no static power consumption. With these superior performances, our findings pave a promising way for reconfigurable non-Hermitian photonic devices, which may find applications in tunable on-chip sensors, isolators and so on.

Insight into a Nitrogen-Doping Mechanism in a Hard-Carbon-Microsphere Anode Material for the Long-Term Cycling of Potassium-Ion Batteries.

To investigate the alternatives to lithium-ion batteries, potassium-ion batteries have attracted considerable interest due to the cost-efficiency of potassium resources and the relatively lower standard redox potential of K+/K. Among various alternative anode materials, hard carbon has the advantages of extensive resources, low cost, and environmental protection. In the present study, we synthesize a nitrogen-doping hard-carbon-microsphere (N-SHC) material as an anode for potassium-ion batteries. N-SHC delivers a high reversible capacity of 248 mAh g-1 and a promoted rate performance (93 mAh g-1 at 2 A g-1). Additionally, the nitrogen-doping N-SHC material also exhibits superior cycling long-term stability, where the N-SHC electrode maintains a high reversible capacity at 200 mAh g-1 with a capacity retention of 81% after 600 cycles. DFT calculations assess the change in K ions' absorption energy and diffusion barriers at different N-doping effects. Compared with an original hard-carbon material, pyridinic-N and pyrrolic-N defects introduced by N-doping display a positive effect on both K ions' absorption and diffusion.

O-Doping Configurations Reduce the Adsorption Energy Barrier of K-Ions to Improve the Electrochemical Performance of Biomass-Derived Carbon.

In recent years, atomic-doping has been proven to significantly improve the electrochemical performance of biomass-derived carbon materials, which is a promising modification strategy. Among them, there are relatively few reports about O-doping. Here, porous carbon derived from orange peel was prepared by simple carbonization and airflow-annealing processes. Under the coordination of microstructure and surface groups, the derived carbon had excellent electrochemical performance for the K-ion batteries' anode, including a high reversible specific capacity of 320.8 mAh/g, high rate performance of 134.6 mAh/g at a current density of 2000 mA/g, and a retention rate of 79.5% even after 2000 long-term cycles, which shows great application potential. The K-ion storage mechanisms in different voltage ranges were discussed by using various characterization techniques, that is, the surface adsorbed of K-ionswas in the high-potential slope area, and the intercalation behavior corresponded to the low-potential quasi-plateau area. In addition, the density functional theory calculations further confirmed that O-doping can reduce the adsorption energy barrier of K-ions, change the charge density distribution, and promote the K-ion storage. In particular, the surface Faraday reaction between the C=O group and K-ions plays an important role in improving the electrochemical properties.

Hollow Square RodLike Microtubes Composed of Anatase Nanocuboids with Coexposed {100}, {010}, and {001} Facets for Improved Photocatalytic Performance.

In this study, hollow square rodlike microtubes composed of anatase nanocuboids with coexposed {100}, {010}, and {001} facets were successfully synthesized via a mild hydrothermal treatment method in the presence of NH4F by using layered H2Ti3O7 ribbons as the precursor. The precursor H2Ti3O7 ribbons were prepared from H+/Na+ ion-exchanged Na2Ti3O7. The suspension solution of protonated H2Ti3O7 ribbons was adjusted to desired pH values (0.5-13.0) prior to hydrothermal treatment. The elongated direction of the microtubes is along the b axis, according to the profile of the H2Ti3O7 ribbons. The transformation from staggered [Ti3O7]2- sheets to hollow square rodlike microtubes contained the formation and recombination of the dispersed octahedral [Ti(OH)2(OH2)4]2+ monomers, the formation and growth of the initial anatase nuclei, and the reassembly of the anatase nanocuboids along the b-axis direction during the continuous hydrothermal process. The degradation rate of pH 0.5-TiO2 was the highest at 1.66 × 10-2 min-1, which was 1.3, 1.5, 2.0, 2.3, and 18.4 folds higher than that of pH 3.0-TiO2 (1.27 × 10-2 min-1), pH 7.0-TiO2 (1.11 × 10-2 min-1), pH 5.0-TiO2 (0.83 × 10-2 min-1), P25-TiO2 (0.73 × 10-2 min-1), and the blank sample (0.09 × 10-2 min-1), respectively. Compared with P25-TiO2 and the other anatase TiO2 samples, pH 0.5-TiO2 exhibited the best photocatalytic activity, which was mainly attributed to its larger proportion of {010} (or {100}) facets, smaller crystalline size, higher band gap, and larger specific surface area.

Facile synthesis of TiO2/Ag3PO4 composites with co-exposed high-energy facets for efficient photodegradation of rhodamine B solution under visible light irradiation.

In this study, TiO2/Ag3PO4 composites based on anatase TiO2 nanocrystals with co-exposed {101}, {010}/{100}, {001} and [111]-facets and Ag3PO4 microcrystals with irregular and cubic-like polyhedron morphologies were successfully synthesized by combining hydrothermal and ion-exchange methods. The anatase TiO2 nanocrystals with different high-energy facets were controllably prepared via hydrothermal treatment of the exfoliated [Ti4O9]2-/[Ti2O5]2- nanosheet solutions at desired pH values. The Ag3PO4 microcrystal with different morphologies was prepared via the ion-exchange method in the presence of AgNO3 and NH4H2PO4 at room temperature, which was used as a substrate to load the as-prepared anatase TiO2 nanocrystals on its surface and to form TiO2/Ag3PO4 heterostructures. The apparent rate constant of the pH 3.5-TiO2/Ag3PO4 composite was the highest at 12.0 × 10-3 min-1, which was approximately 1.1, 1.2, 1.4, 1.6, 13.3, and 24.0 fold higher than that of pH 0.5-TiO2/Ag3PO4 (10.5 × 10-3 min-1), pH 7.5-TiO2/Ag3PO4 (10.2 × 10-3 min-1), pH 11.5-TiO2 (8.8 × 10-3 min-1), Ag3PO4 (7.7 × 10-3 min-1), blank sample (0.9 × 10-3 min-1), and the commercial TiO2 (0.5 × 10-3 min-1), respectively. The pH 3.5-TiO2/Ag3PO4 composite exhibited the highest visible-light photocatalytic activity which can be attributed to the synergistic effects of its heterostructure, relatively small crystal size, large specific surface area, good crystallinity, and co-exposed high-energy {001} and [111]-facets. The as-prepared TiO2/Ag3PO4 composites still exhibited good photocatalytic activity after three successive experimental runs, indicating that they had remarkable stability. This study provides a new way for the preparation of TiO2/Ag3PO4 composite semiconductor photocatalysts with high energy crystal surfaces and high photocatalytic activity.

Analysis of Ultrahigh Apparent Mobility in Oxide Field-Effect Transistors.

For newly developed semiconductors, obtaining high-performance transistors and identifying carrier mobility have been hot and important issues. Here, large-area fabrications and thorough analysis of InGaZnO transistors with enhanced current by simple encapsulations are reported. The enhancement in the drain current and on-off ratio is remarkable in the long-channel devices (e.g., 40 times in 200 µm long transistors) but becomes much less pronounced in short-channel devices (e.g., 2 times in 5 µm long transistors), which limits its application to the display industry. Combining gated four-probe measurements, scanning Kelvin-probe microscopy, secondary ion mass spectrometry, X-ray photoelectron spectroscopy, and device simulations, it is revealed that the enhanced apparent mobility up to several tens of times is attributed to the stabilized hydrogens in the middle area forming a degenerated channel area while that near the source-drain contacts are merely doped, which causes artifact in mobility extraction. The studies demonstrate the use of hydrogens to remarkably enhance performance of oxide transistors by inducing a new mode of device operation. Also, this study shows clearly that a thorough analysis is necessary to understand the origin of very high apparent mobilities in thin-film transistors or field-effect transistors with advanced semiconductors.

Synthesis of [111]- and {010}-faceted anatase TiO2 nanocrystals from tri-titanate nanosheets and their photocatalytic and DSSC performances.

[111]- and {010}-faceted anatase nanocrystals with controllable crystal size and morphology were synthesized from tri-titanate H2Ti3O7 nanosheets by hydrothermal reaction. The nanostructures and the formation reaction mechanism of the obtained TiO2 nanocrystals were investigated using XRD, FE-SEM, and TEM. Furthermore, the photocatalytic and dye-sensitized solar cell (DSSC) performances of the synthesized anatase nanocrystals were also characterized. Two types of reactions occur in the formation process of the anatase nanocrystals. One is an in situ topochemical conversion reaction of the layered titanate structure to an anatase structure, and another is the dissolution-deposition reaction on the particle surface, which splits the formed nanosheet-like particles into small TiO2 nanocrystals. The surface photocatalytic activity and the DSSC performance of the anatase nanocrystals are dependent on the crystal facet exposed on the particle surface, which increases in the order of non-facet < [111]-facet < {010}-facet. The increasing order corresponds to the increasing order of the bandgap and energy level of the lowest valence band of the anatase nanocrystals. Furthermore, the facet of the anatase also affects the DSSC performance, which is enhanced in the order of non-facet < [111]-facet < {010}-facet.

Photocatalytic and dye-sensitized solar cell performances of {010}-faceted and [111]-faceted anatase TiO2 nanocrystals synthesized from tetratitanate nanoribbons.

The morphology and exposed facet of the anatase-type TiO2 are very important to improve the photocatalytic activity and photovoltaic performance in dye-sensitized solar cells. In this work, we report the synthesis and the photocatalytic and dye-sensitized solar cell performances of anatase-type TiO2 single nanocrystals with exposed {010}- and [111]-facets and with various morphologies by using exfoliated tetratitanate nanoribbons as precursors. The precursor nanoribbons were prepared from the exfoliation of the protonated and, subsequently, tetramethylammonium/H(+) ion-exchanged K2Ti4O9. The colloidal suspension containing the nanoribbons was hydrothermally heated with a microwave-assistance at temperatures from 120 to 190 °C after pH was adjusted to 0.5-14. The dependence of the crystalline phases on temperature and pH indicated that anatase single phase can be obtained at pH 3-13 whereas temperatures higher than 160 °C. The [111]-faceted nanorod-shaped anatase nanocrystals were formed preferentially at pH ≤ 3, whereas the {010}-faceted anatase nanocrystals with morphologies of rhombic, cuboid, and spindle were preferentially at pH ≥5. The morphology observation revealed that the nanoribbons were transformed to anatase nanocrystals mainly by the topotactic structural transformation reaction accompanied by an Ostwald ripening reaction, and pH of the reaction solution took a critical role in the crystal morphology change. At pH ≤1, the mixture of anatase, rutile, and brookite were obtained at higher temperature conditions. The photocatalytic activity and photovoltaic performance were enhanced in an order of surface without a specific facet < [111]-faceted surface < {010}-faceted surface.

Cerenkov third-harmonic generation via cascaded χ(2) processes in a periodic-poled LiTaO3 waveguide.

We report a type of quasi-phase-matched (QPM) Cerenkov third-harmonic generation (CTHG) in a periodic-poled LiTaO3 waveguide. The CTHG results from a guided-to-guided second-harmonic generation cascaded with a guided-to-radiated sum-frequency generation (SFG) in the waveguide. In the guided-to-radiated SFG process, nonlinear interactions with participating and nonparticipating reciprocal vectors would lead to different CTHG radiations. In addition, the power and temperature detuning characters of QPM CTHG were studied. Theoretical predictions were in good agreement with experimental results.