Metal telluride nanosheets by scalable solid lithiation and exfoliation.

Transition metal tellurides (TMTs) have been ideal materials for exploring exotic properties in condensed-matter physics, chemistry and materials science1-3. Although TMT nanosheets have been produced by top-down exfoliation, their scale is below the gram level and requires a long processing time, restricting their effective application from laboratory to market4-8. We report the fast and scalable synthesis of a wide variety of MTe2 (M = Nb, Mo, W, Ta, Ti) nanosheets by the solid lithiation of bulk MTe2 within 10 min and their subsequent hydrolysis within seconds. Using NbTe2 as a representative, we produced more than a hundred grams (108 g) of NbTe2 nanosheets with 3.2 nm mean thickness, 6.2 µm mean lateral size and a high yield (>80%). Several interesting quantum phenomena, such as quantum oscillations and giant magnetoresistance, were observed that are generally restricted to highly crystalline MTe2 nanosheets. The TMT nanosheets also perform well as electrocatalysts for lithium-oxygen batteries and electrodes for microsupercapacitors (MSCs). Moreover, this synthesis method is efficient for preparing alloyed telluride, selenide and sulfide nanosheets. Our work opens new opportunities for the universal and scalable synthesis of TMT nanosheets for exploring new quantum phenomena, potential applications and commercialization.

Long-term outcomes of COVID-19 convalescents: An 18.5-month longitudinal study in Wuhan.

OBJECTIVES: This study aimed to describe the full scope of long-term outcomes and the ongoing pathophysiological alterations among COVID-19 survivors. METHODS: We established a longitudinal cohort of 208 COVID-19 convalescents and followed them at 3.3 (interquartile range [IQR]: 1.3, 4.4, visit 1), 9.2 (IQR: 9.0, 9.6, visit 2), and 18.5 (IQR: 18.2, 19.1, visit 3) months after infection, respectively. Serial changes in multiple physical and psychological outcomes were comprehensively characterized. We, in addition, explored the potential risk factors of SARS-CoV-2 antibody response and sequelae symptoms. RESULTS: We observed continuous improvement of sequelae symptoms, lung function, chest computed tomography (CT), 6-minute walk test, and the Borg dyspnea scale, whereas sequelae symptoms (at least one) and abnormal chest CT patterns still existed in 45.2% and about 30% of participants at 18.5 months, respectively. Anxiety and depression disorders were alleviated for the convalescents, although depression status was sustained for a longer duration. CONCLUSIONS: Most COVID-19 convalescents had an overall improved physical and psychological health status, whereas sequelae symptoms, residual lesions on lung function, exercise impairment, and mental health disorders were still observed in a small proportion of participants at 18.5 months after infection. Implementing appropriate preventive and management strategies for the ever-growing COVID-19 population is warranted.

Room-Temperature In Situ Synthesis of a Highly Efficient CsPbBr3/SiO2 Sol Entirely in Ethanol Solvent by Constructing Amine-Functionalized Silica Micelles.

Cesium lead halide perovskite nanocrystals (CLHP NCs) have drawn considerable attention because of their promising optoelectrical properties. However, owing to the extreme vulnerability of CLHP NCs to water and polar alcohols, until now most synthesis approaches inevitably adopted ecounfriendly solvents. It is still a challenge to employ green polar alcohol (ethanol) as a solvent to synthesize CLHP NCs. In this work, we realized the room-temperature in situ synthesis of CsPbBr3/SiO2 sol entirely in ethanol by innovatively constructing amine-functionalized silica micelles, which originated from the synergistic effect of 3-aminopropyltriethoxysilane and tetraethylorthosilicate (TEOS) during an acid-catalyzed sol-gel process. The sol exhibited high stability and an absolute photoluminescence quantum yield of 61.9% in ethanol without a further modification process. The light-emitting intensity of the sol preserved for 34 days merely declined to 62.1%. This work sheds light on the less common strategy of directly synthesizing CsPbBr3 NCs and long-term stable preservation in a strongly polar solvent.

Room-Temperature in Situ Synthesis of Highly Efficient CsPbBr3/SiO2 Sol in Entirely Ethanol Solvent by Constructing Amine-Functionalized Silica Micelles.

Cesium lead halide perovskite nanocrystals (CLHP NCs) have drawn considerable attention because of their promising optoelectrical properties. However, owing to extreme vulnerability of CLHP NCs to water and polar alcohols, up to date, most of the synthesis approaches have inevitably adopted eco-unfriendly solvents. It is still a big challenge to employ green polar alcohol (ethanol) as a solvent to synthesize CLHP NCs. In this work, we realized a room-temperature in situ synthesis of CsPbBr3/SiO2 sol entirely in ethanol by innovatively constructing amine-functionalized silica micelles, which is originated from the synergistic effect of 3-aminopropyltriethoxysilane and tetraethyl orthosilicate (TEOS) during an acid-catalyzed sol-gel process. The sol exhibited high stability and an absolute photoluminescence quantum yield of 61.9% in ethanol without a further modification process. The light emitting intensity of the sol preserved for 34 days merely declined to 62.1%. This work sheds light on the less common strategy of directly synthesizing CsPbBr3 NCs and long-term stable preservation in a strong polar solvent.

Dynamic Optics with Transparency and Color Changes under Ambient Conditions.

Mechanochromic materials have recently received tremendous attention because of their potential applications in humanoid robots, smart windows, strain sensors, anti-counterfeit tags, etc. However, improvements in device design are highly desired for practical implementation in a broader working environment with a high stability. In this article, a novel and robust mechanochromism was designed and fabricated via a facile method. Silica nanoparticles (NPs) that serve as a trigger of color switch were embedded in elastomer to form a bi-layer hybrid film. Upon stretching under ambient conditions, the hybrid film can change color as well as transparency. Furthermore, it demonstrates excellent reversibility and reproducibility and is promising for widespread application.

A chalcohalide glass/alloy based Ag+ ion - selective electrode with nanomolar detection limit.

In this paper, a silver ion-selective electrode material with lower detection limit is presented. The electrode is based on 22.5As2S3-22.5Ag2S-55AgCl chalcohalide glass membranes. The low detection limit decreases from the micromolar range of the original Ag2S-As2S3 electrode to the nanomolar level (1.89 nM) by introducing AgCl. The addition of AgCl increases the conductivity of the glasses and improves the analytical properties of electrodes because of the joint effects of Ag+ and Cl- on network structure of the glass. The super-Nernstian response behavior was observed for the partially crystallized electrode. The electrode containing AgCl also possesses a high selectivity (except for Hg2+), fast response and good stability.

Structure-Dependent Spectroscopic Properties of Yb3+-Doped Phosphosilicate Glasses Modified by SiO2.

Yb3+-doped phosphate glasses containing different amounts of SiO2 were successfully synthesized by the conventional melt-quenching method. The influence mechanism of SiO2 on the structural and spectroscopic properties was investigated systematically using the micro-Raman technique. It was worth noting that the glass with 26.7 mol % SiO2 possessed the longest fluorescence lifetime (1.51 ms), the highest gain coefficient (1.10 ms·pm²), the maximum Stark splitting manifold of ²F7/2 level (781 cm-1), and the largest scalar crystal-field NJ and Yb3+ asymmetry degree. Micro-Raman spectra revealed that introducing SiO2 promoted the formation of P=O linkages, but broke the P=O linkages when the SiO2 content was greater than 26.7 mol %. Based on the previous 29Si MAS NMR experimental results, these findings further demonstrated that the formation of [SiO6] may significantly affect the formation of P=O linkages, and thus influences the spectroscopic properties of the glass. These results indicate that phosphosilicate glasses may have potential applications as a Yb3+-doped gain medium for solid-state lasers and optical fiber amplifiers.

Size/morphology induced tunable luminescence in upconversion crystals: ultra-strong single-band emission and underlying mechanisms.

In this work, we present a two-step method to controllably synthesize novel and highly efficient upconversion materials, Lu5O4F7:Er(3+),Yb(3+) nano/micro-crystals, and investigate their size/morphology induced tunable upconversion properties. In addition to the common phenomenon aroused by a surface quenching effect, direct experimental evidence for the regulation of phonon modes is obtained in nanoparticles. The findings in this work advance the existing mechanisms for the general explanation of size/morphology induced upconversion features. Because of the adjustment of phonon energy and density as well as the surface quenching effect, the biocompatible Lu5O4F7:Er(3+),Yb(3+) nanoparticles exhibit an ultra-strong single-band red upconversion, rendering them promising for biomedical applications.

Tailoring sodium silicophosphate glasses containing SiO6-octahedra through structural rules and topological principles.

SiO4 tetrahedra in certain sodium silicophosphate glasses can be transformed into SiO6 octahedra that determine the macroscopic properties of silicophosphate glasses to a large extent. In this study, we develop the quantitative evolution rule of each network former. In addition, based on the underlying structure and topology, temperature-dependent topological constrain theory is used to elucidate the composition dependence of glass transition temperature and hardness. The properties of sodium silicophosphate glasses have been accurately predicted. These understandings will help us design new type of silicophosphate glasses containing unique SiO6 octahedra.

Unique sodium phosphosilicate glasses designed through extended topological constraint theory.

Sodium phosphosilicate glasses exhibit unique properties with mixed network formers, and have various potential applications. However, proper understanding on the network structures and property-oriented methodology based on compositional changes are lacking. In this study, we have developed an extended topological constraint theory and applied it successfully to analyze the composition dependence of glass transition temperature (Tg) and hardness of sodium phosphosilicate glasses. It was found that the hardness and Tg of glasses do not always increase with the content of SiO2, and there exist maximum hardness and Tg at a certain content of SiO2. In particular, a unique glass (20Na2O-17SiO2-63P2O5) exhibits a low glass transition temperature (589 K) but still has relatively high hardness (4.42 GPa) mainly due to the high fraction of highly coordinated network former Si((6)). Because of its convenient forming and manufacturing, such kind of phosphosilicate glasses has a lot of valuable applications in optical fibers, optical amplifiers, biomaterials, and fuel cells. Also, such methodology can be applied to other types of phosphosilicate glasses with similar structures.

Aqueous phase preparation of graphene with low defect density and adjustable layers.

Graphene sheets with an adjustable number of layers and a low defect density were prepared by exfoliation of microwave-assisted expanded graphite in the aqueous phase with the assistance of cetyltrimethylammonium bromide. The graphene sheets exhibit excellent film-formation ability, showing potential applications in optical and electrical device fields.

Glass transition temperature and topological constraints of sodium borophosphate glass-forming liquids.

Sodium borophosphate glasses exhibit intriguing mixed network former effect, with the nonlinear compositional dependence of their glass transition temperature as one of the most typical examples. In this paper, we establish the widely applicable topological constraint model of sodium borophosphate mixed network former glasses to explain the relationship between the internal structure and nonlinear changes of glass transition temperature. The application of glass topology network was discussed in detail in terms of the unified methodology for the quantitative distribution of each coordinated boron and phosphorus units and glass transition temperature dependence of atomic constraints. An accurate prediction of composition scaling of the glass transition temperature was obtained based on topological constraint model.

Synthesis, optical and electrochemical properties of ZnO nanowires/graphene oxide heterostructures.

Large-scale vertically aligned ZnO nanowires with high crystal qualities were fabricated on thin graphene oxide films via a low temperature hydrothermal method. Room temperature photoluminescence results show that the ultraviolet emission of nanowires grown on graphene oxide films was greatly enhanced and the defect-related visible emission was suppressed, which can be attributed to the improved crystal quality and possible electron transfer between ZnO and graphene oxide. Electrochemical property measurement results demonstrated that the ZnO nanowires/graphene oxide have large integral area of cyclic voltammetry loop, indicating that such heterostructure is promising for application in supercapacitors.

Broadband near-infrared emission of chromium-doped sulfide glass-ceramics containing Ga2S3 nanocrystals.

Upon 808 nm excitation, an intense broadband near-infrared emission from Cr4+ has been observed in 80GeS2-20Ga2S3 chalcogenide glass-ceramics (GCs) containing Ga2S3 nanocrystals. The emission band peaking at 1250 nm covers the O, E, S bands (1000-1500 nm). The formation of Ga2S3 nanocrystals (∼20 nm) increases the emission intensity of Cr4+ by more than three times. The quantum efficiency of the present GCs is as great as 36% at room temperature.

Three-dimensional photoprecipitation of oriented LiNbO3-like crystals in silica-based glass with femtosecond laser irradiation.

We demonstrate crystals (LiNbO(3)-like) that were space-selectively nucleated and grown in the bulk of silica-based glass by femtosecond laser irradiation at a high repetition rate (typ. 300 kHz). Oriented crystals with their polar axis mostly aligned with or perpendicular to the laser scanning direction have been fabricated by manipulation of the temperature gradient in adjusting the laser parameters. The mechanism for the orientation of femtosecond laser-induced crystallization is briefly discussed.

Broadband near-infrared emission in Er3+-Tm3+ codoped chalcohalide glasses.

The near-IR emission spectra of Er3+-Tm3+ codoped 70GeS2-20In2S3-10CsI chalcohalide glasses were studied with an 808 nm laser as an excitation source. A broad emission extending from 1.35 to 1.7 microm with a FWHM of approximately 160 nm was recorded in a 0.1 mol.% Er2S3, 0.5 mol.% Tm2S3 codoped chalcohalide glass. The fluorescence decay curves of glasses were measured by monitoring the emissions of Tm3+ at 1460 nm and Er3+ at 1540 nm, and the lifetimes were obtained from the first-order exponential fit. The luminescence mechanism and the possible energy-transfer processes are discussed with respect to the energy-level diagram of Er3+ and Tm3+ ions.

A photo-stable chalcogenide glass.

Photo-darkening and photo-bleaching are well known phenomena in As-Se and Ge-Se chalcogenide glasses, respectively. Consequently, a systematic dependence of photo-induced optical changes in Ge(x)As(45-x)Se(55) glass series on x is expected between these two extremes. This prediction of photosensitivity on Ge/As ratio has been exploited to demonstrate the first intrinsically photo-stable chalcogenide glass at x approximately 10, which would be suitable for fabricating photo-insensitive optical components for various applications.

Three-photon-excited upconversion luminescence of niobium ions doped silicate glass by a femtosecond laser irradiation.

We report on the bluish green upconversion luminescence of niobium ions doped silicate glass by a femtosecond laser irradiation. The dependence of the fluorescence intensity on the pump power density of laser indicates that the conversion of infrared irradiation to visible emission is dominated by three-photon excitation process. We suggest that the charge transfer from O(2-) to Nb(5+) can efficiently contribute to the bluish green emission. The results indicate that transition metal ions without d electrons play an important role in fields of optics when embedded into silicate glass matrix.

Selective metallization on insulator surfaces with femtosecond laser pulses.

We report selective metallization on surfaces of insulators (glass slides and lithium niobate crystal) based on femtosecond laser modification combined with electroless plating. The process is mainly composed of four steps: (1) formation of silver nitrate thin films on the surfaces of glass or crystal substrates; (2) generation of silver particles in the irradiated area by femtosecond laser direct writing; (3) removal of unirradiated silver nitrate films; and (4) selective electroless plating in the modified area. We discuss the mechanism of selective metallization on the insulators. Moreover, we investigate the electrical and adhesive properties of the copper microstructures patterned on the insulator surfaces, showing great potential of integrating electrical functions into lab-on-a-chip devices.