Multicomponent Glasses Research Articles

Third-order optical nonlinear features of Er3+ and Pr3+ activated multicomponent borate glasses in nanosecond pulse regime: A comparative study

In the current work, the borate-based glass specimens bearing composition (mol %) 5Na 2 O–10ZnO–10Bi 2 O 3 ‒(75‒ x )B 2 O 3 – x RE (where RE = Er 2 O 3 and Pr 6 O 11 , and x ranges from 0 to 5 mol %) were synthesized by conventional melt-quench method. The effect of rare earth ions concentration on photonic nonlinearities has been explored by the Z-scan method under the pumping of 532 nm in a nanosecond pulse regime. The Z-signatures revealed the occurrence of nonlinear absorption and refraction in the studied glass specimens. The nonlinear optical features were improved with respect to the rare earth concentration. The nonlinear optical features were superior for Er 3+ doped glasses compared to Pr 3+ doped glasses. This greatness of nonlinear optical features in Er 3+ doped glasses was attributed to the existence of a large number of electrons (11 electrons) in the 4 f outer shell compared to those existing in the 4 f outer shell of Pr 3+ (2 electrons). The enhancement of nonlinear gap features was also attributed to the creation of non-bridging oxygens in the host network when rare earths are loaded into the composition. The nonlinear photonic outcomes endorse that heavily Er 3+ loaded glasses are superior over Pr 3+ doped glasses for nonlinear optical device fabrications to work in the visible region.

Пассивные стекла в системах наблюдения

The analysis of the possibilities of determining the spectrum of electromagnetic radiation from celestial objects using the optical-electronic system of the telescope using CCD receivers is carried out. It is shown that with the introduction of new CCD-type receivers into photometry, the efficiency of observing celestial objects has significantly increased, but despite the positive result, it is necessary to eliminate problems when registering objects with weak radiation during measurements. The purpose of the article is based on the results of experimental studies of thermomechanical and optical properties of multicomponent glasses to provide a justification for the introduction of new materials with a wider transmission range of radiation in various spectra as elements of optical systems of telescopes. In the course of research of new optical materials using the spectroscopy method, optimal compositions of multicomponent glasses were found, allowing to perceive electromagnetic radiation from celestial bodies in various ranges of the infrared spectrum. In conclusion, the results of the study are presented, showing that the introduction of indium and lead fluorides into the composition of multicomponent glass significantly increases the transmission range, which will increase the efficiency of the optical system when using these materials for its elements.

Optical properties of AIE organic chromophores embedded erbium-doped glass composites fabricated by spark plasma sintering

Encapsulation strategies can isolate the organic chromophores and prevent chemical or photochemical degradation. Inorganic transparent glass matrix has excellent utility as encapsulation matrices. Although the sol-gel method can make this encapsulation, the unclear sol-gel synthetic mechanism limits the synthesis of multi-component glass whose properties can be modified. A novel technique to encapsulate organic chromophores within multi-component glasses is required. In this letter, an organic chromophore was successfully encapsulated within a multi-component glass matrix by spark plasma sintering (SPS). The glass composite has great chemical and photochemical stability. Besides, a non-radiative energy transfer process between rare earth ions and organic chromophores was observed in the glass composites. These results indicate that the glass composite has great potential for optical application, and SPS can be a novel technique for encapsulating organic chromophores.

Revealing local order via high energy EELS

Short range order (SRO) is critical in determining the performance of many important engineering materials. However, accurate characterization of SRO with high spatial resolution – which is needed for the study of individual nanoparticles and at material defects and interfaces – is often experimentally inaccessible. Here, we locally quantify SRO via scanning transmission electron microscopy with extended energy loss fine structure analysis. Specifically, we use novel instrumentation to perform electron energy loss spectroscopy out to 12 keV, accessing energies which are conventionally only possible using a synchrotron. Our data is of sufficient energy resolution and signal-to-noise ratio to perform quantitative extended fine structure analysis, which allows determination of local coordination environments. To showcase this technique, we investigate a multicomponent metallic glass nanolaminate and locally quantify the SRO with <10 nm spatial resolution; this measurement would have been impossible with conventional synchrotron or electron microscopy methods. We discuss the nature of SRO within the metallic glass phase, as well as the wider applicability of our approach for determining processing–SRO–property relationships in complex materials.

Optical Properties of Er3+-Yb3+ Ions Co-activated Multicomponent Phosphate Glasses for Near-Infrared Applications

Optical Properties of Er3+-Yb3+ Ions Co-activated Multicomponent Phosphate Glasses for Near-Infrared Applications

Electronic structure and surface morphology of multicomponent iron-based metallic glasses

Electronic structure and surface morphology of multicomponent iron-based metallic glasses

Enhancement of significant colour properties through Ta2O5 incorporation into ZnO–TeO2 binary glasses: An effective method for purposeful utilizations in industry and technology

The fact that multicomponent glass systems offer tuneable optical properties according to different additive rates increases their potential for use in daily industrial and optoelectronic applications that require high optical and colour performance. Therefore, it is vital to determine the optical and colour performances of glass systems in detail. The purpose of this research is to examine the monotonic effects of Ta2O5 on a set of glass samples and the resulting changes to colour concepts to better understand how to acquire these changes at their optimum level and make the most of the optimization possibilities available with Ta2O5. Accordingly, many optical properties such as Average Visible Transmittance (AVT), colour, Colour Render Index (CRI), Correlated Colour Temperature (CCT) that change with Ta2O5 doping ratio in binary Zinc-Tellurite oxide glasses-based systems are examined and their potential to be used for effective optoelectronic applications are presented. With the addition of Ta2O5 into (25ZnO·75TeO2)y(Ta2O5)x (x = 0–7 mol% and y = 100-x mol%) glassy system, all optical and colour properties were improved significantly. The Ta2O5 contribution increases the AVT and changes the colour coordinates of the glass system along the Planckian locus curve from the yellow region to the D65 colour coordinates. In addition, a comprehensive analysis of 15 coloured samples is provided, focusing on the cases in which Ta2O5 enhances the CRIext value. An enrichment was observed for TCS07 and TCS14, and a value of 100 was obtained specifically for TCS09 with a 3% Ta2O5 contribution. It can be concluded that the Ta2O5 is a promising multi-functional tool for colour enhancement of ZnO–TeO2 binary glasses making them more suitable for daily applications as well as applications in advanced technological purposes.

Study of concentration and temperature-dependent photoluminescence properties in DyF3-doped fluorophosphate glasses for thermal stable photonic device

The novel P2O5–ZnO–B2O3–Na2O–NaF multi-component fluorophosphate glasses doped with DyF3 were prepared via the conventional melt-quenching process. The effects of DyF3 concentration on the glass structure and photoluminescence properties were systematically discussed. The J-O analysis and radiative properties of Dy3+ ions in fluorophosphate glass were investigated. Upon the excitation of 349 nm, the fluorescence intensity of 4F9/2 → 6HJ/2 (J = 15, 13, 11, 9) transitions increase first and then decrease with the DyF3 concentration, and the optimum concentration was determined to be 1.5 mol%. The 1.5 mol% DyF3-doped glass exhibit a high photoluminescence quantum yield (54.65%) and great thermal stability. Finally, the temperature-dependent emission spectra contour map reveals that the fluorescence emission of the fluorophosphate glass with 1.5 mol% DyF3 demonstrates a downtrend with the temperature, and the fluorescence intensity of the yellow emission transition (4F9/2 → 6H13/2) at 473 K can still maintain 70% of that at the initial condition (298 K). These results suggest that these DyF3-doped fluorophosphate glasses may be applied for thermal stable photonic devices.

Influence of Al2O3/SiO2 ratio in multicomponent LNAS glasses and glass-ceramics on the crystallization behavior, microstructure and mechanical performance

Transparent glass-ceramics containing eucryptite and nepheline crystalline phases were prepared from alkali (Li, Na) aluminosilicate glasses with various mole substitutions of Al2O3 for SiO2. The relationships between glass network structure and crystallization behavior of Li2O–Na2O–Al2O3–SiO2 (LNAS) glasses were investigated. It was found that the crystallization of the eucryptite and nepheline in LNAS glasses significantly depended on the concentration of Al2O3. LNAS glasses with the addition of Al2O3 from 16 to 18 mol% exhibited increasing Q4 (mAl) structural units confirmed by NMR and Raman spectroscopy, which promoted the formation of eucryptite and nepheline crystalline phases. With the Al2O3 content increasing to 19–20 mol%, the formation of highly disordered (Li, Na)3PO4 phase which can serve as nucleation sites was inhibited and the crystallization mechanism of glass became surface crystallization. Glass-ceramics containing 18 mol% Al2O3 showed high transparency ∼84% at 550 nm. Moreover, the microhardness, elastic modulus and fracture toughness are 8.56 GPa, 95.7 GPa and 0.78 MPa m1/2 respectively. The transparent glass-ceramics with good mechanical properties show high potential in the applications of protective cover of displays.

High-efficiency 3.5 [formula omitted] luminescence of heavily Er[formula omitted] doped multicomponent glasses

The ∼3.5μm mid-infrared laser based on a high concentration of Er3+-doped multicomponent glasses possesses unique advantages, but the existing traditional glass hosts, which are inherently flawed, lead to challenging research. In this paper, oxyhalide glasses with tellurite (TeO2-Na2O-ZnO as the main body) and chloride (ZnCl2 as the modifier) are obtained with a high doping concentration of Er3+. It is worth noting that the microstructure can be adjusted to obtain excellent luminescence properties, while ensuring the thermal properties of the matrix. Both the actual performance test and theoretical calculation show that the scheme of realizing ∼3.5μm luminescence by high Er3+ doping in the present oxyhalide glass matrix is reasonable and effective, which provides a new choice for Er3+-doped ∼3.5μm laser gain medium in the future.

Cyclic ablation resistance at 2300 °C of (Hf0.4Zr0.4Ta0.2)B2-SiC-Si coating for C/SiC composites prepared by SiC-assisted reactive infiltration of silicon

Developing coatings is of prime importance for improving the ablation resistance of Cf/SiC composites at ultra-high temperatures due to the inherent preparation defects in the SiC matrix and the low melting point of the produced SiO2. In this paper, a (Hf0.4Zr0.4Ta0.2)B2-SiC-Si (HZTS) coating with a quaternary solid solution of ultra-high temperature boride was designed and coated on the surface of Cf/SiC substrate by SiC-assisted reactive infiltration of silicon. The obtained HZTS coating has a high interfacial bonding strength of 18.25 MPa with the substrate due to its dense structure and uniform constituent distribution, as well as their physical and chemical adhesion. The coating also presents an excellent cycle ablation resistance with a respective mass and linear ablation rates of 2.1 × 10−2 mg/s and 0.4 μm/s after 15 cycles of 60 s ablation at 2300 °C, which are attributed to the formation of highly thermo-stable Hf-Zr-Ta-O solid solution and multicomponent silicate glass.

Multi-component oxide lens glass with ultra-high mechanical properties inspired by the high-entropy concept

Lenses with high transmittance, high refractive index and excellent scratch resistance are in urgent need for cameras in high-end smartphones, and existing resin lenses exhibits intrinsic upper limits in those properties. Glass, with its naturally high refractive index and mechanical properties, is considered an ideal candidate for high-end lenses, however, due to the lack of targeted design, the intrinsic hardness, modulus and fracture toughness of conventional glass are low and its scratch resistance is inadequate. Here, we combined multi-compositional design and structural modulation of high mechanical lens glass with high-entropy concept, and successfully prepared multi-component 31.6RO-4.1Y2O3-23.7TiO2-7.4ZrO2-33.2Al2O3 (R = Ba, Sr, Ca) glasses with ultra-high hardness (11.06 GPa), modulus (147.6 GPa) and indentation fracture toughness (1.334 MPa m0.5). The excellently comprehensive properties of the glass are attributed to the synergistic effect of multiple high dissociation energy and high field strength oxides, which leads to the movement of low-coordinated Al[4] to the higher-coordinated Al[5]/Al[6].

Correlation of structure and ionic-conductivity in phosphate glass using MAS-NMR and impedance spectroscopy: Influence of sodium salt

In the process of diminishing the safety concerns of sodium-ion batteries, the development of glass-based solid electrolyte materials has received adequate interest. Nevertheless, achieving a high ionic-conductivity at room temperature for glass materials remains a challenging task because of the poor correlation between the conductivity and the glass structure. Here, we attempt to understand the effective influence of NaCl on the structure and ionic-conductivity of the phosphate-based glass network. For this study, $x\mathrm{NaCl}\text{\ensuremath{-}}(100\text{\ensuremath{-}}x$) ($31.725\phantom{\rule{4pt}{0ex}}{\mathrm{Na}}_{2}\mathrm{O}\text{\ensuremath{-}}12.69\phantom{\rule{0.16em}{0ex}}{\mathrm{Al}}_{2}{\mathrm{O}}_{3}\text{\ensuremath{-}}31.725\phantom{\rule{0.16em}{0ex}}{\mathrm{P}}_{2}{\mathrm{O}}_{5}\text{\ensuremath{-}}8.46\phantom{\rule{0.16em}{0ex}}\mathrm{NaF}\text{\ensuremath{-}}5.40\phantom{\rule{0.16em}{0ex}}{\mathrm{Na}}_{2}{\mathrm{SO}}_{4}\text{\ensuremath{-}}10\phantom{\rule{0.16em}{0ex}}{\mathrm{MoO}}_{3}$) glass systems (mol %) were selected, where $x=0$, 5, 10, 15, and 20 mol %. To investigate structural changes with the addition of different NaCl concentrations, $^{27}\mathrm{Al}, ^{23}\mathrm{Na}, ^{31}\mathrm{P}$ magic angle spinning nuclear magnetic resonance (MAS-NMR), $^{31}\mathrm{P}$ two-dimensional (2D) phase-adjusted spinning sideband (PASS), and $^{31}\mathrm{P}$ 2D J-resolved NMR techniques and Raman spectroscopic techniques were utilized. Impedance spectroscopy and ac conductivity spectra were used to assess ionic-conductivity and sodium-ion dynamics, respectively. Impedance spectral analysis reveals that the ionic-conductivity of the base glass is increased by 2.4 times (from 1.85 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}7}$ to 4.44 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}7}$ S/cm at 373 K) with the addition of 20 mol % of NaCl. Raman spectra confirm the presence of P\ensuremath{-}O\ensuremath{-}Mo and the absence of Mo\ensuremath{-}O\ensuremath{-}Mo bonds in these glass systems, and $^{31}\mathrm{P}$ 2D J-resolved spectra indicate the absence of P\ensuremath{-}O\ensuremath{-}P bonds. Upon increasing the NaCl concentration, significant changes in the shapes of $^{31}\mathrm{P}$ and $^{27}\mathrm{Al}$ MAS-NMR spectra were observed, indicating the effective influence of NaCl on the distribution of alumina and phosphorus structural units. Irrespective of the temperature, sodium-ion dynamic studies show that the mean-square displacement $\ensuremath{\langle}{R}^{2}({t}_{p})\ensuremath{\rangle}$ decreases with increasing NaCl concentration up to 10 mol % and then increases with a further increase in NaCl concentration. This investigation aids in understanding the sodium-ion dynamics and the structural information of a multicomponent glass system to enhance the room-temperature conductivity.

Examining phase separation and crystallization in glasses with X-ray nano-computed tomography

X-ray nano-computed tomography (nano-CT) is a powerful technique to characterize and visualize 3 dimensional (3D) phenomena in complex glasses at the nanoscale. This technique can offer a unique opportunity to explore the intricate morphology of multicomponent glass and glass-ceramic samples, due to its low X-ray energy and high spatial resolution (down to 50 nm). In the current demonstration paper, nano-CT provided insight into crystallization and phase separation, as well as a variety of other phenomena, including corrosion, fracture, and porosity. At scales ranging from 100 to 20 μm, the microstructures of phase separation in borosilicate, complex silicate, and chalcogenide glass compositions were examined. In addition, crystallites present in simulant nuclear waste glasses, volcanic glasses, and other related samples were explored. Nano-CT analysis can add to the understanding of (1) the formation processes, (2) distributions, interactions, and compositions of phases, and (3) the mechanisms, structures, and growth of crystallization and phase separation. Nano-CT offers wide potential in the field of glass science, especially when (1) common characterization methods are insufficient, (2) simple sample preparation is required, (3) 3D rendering is needed, or (4) compelling images of small, complex features are desired.

Insights into the mechanism and kinetics of dissolution of aluminoborosilicate glasses in acidic media: Impact of high ionic field strength cations

Achieving thinner and higher performance display/substrate glasses and transparent glass-ceramics with tunable properties requires a precise control of acid-etching process, thus necessitating a comprehensive understanding of glass composition–structure–dissolution behavior relationships in acidic medium. Unfortunately, the literature on this subject has been focused only on a narrow set of glass chemistries. Therefore, consensus on the mechanisms that govern the acidic dissolution of multicomponent silicate glasses over a broad compositional space is still lacking. The present work employs a suite of state-of-the-art spectroscopic techniques, including 1D and 2D NMR, TEM-EELS, ICP-OES, and XPS, to provide an insight into the mechanism and kinetics of corrosion of alkali/alkaline-earth aluminoborosilicate glasses (comprising high field strength cations – HFSCs, i.e., La3+, Ti4+, Zr4+ and Nb5+) in acidic media (HCl; pH = 2). Incorporating the HFSCs into the glasses induces significant structural changes in their network, thus, impacting the forward rate dissolution kinetics. Based on the results, we hypothesize that the glasses dissolve at pH = 2 through an ‘interfacial dissolution – re-precipitation mechanism (IDPM)’ and ‘in-situ recondensation’ coupled pattern, wherein the IDPM results in a Si-rich alteration layer, followed by local recondensation occurring due to limited kinetics near the interfacial solution between the uncorroded glass surface and the outer alteration layer.

Spectroscopic investigation on the photoluminescent traits of Dy3+ activated multicomponent borosilicate glasses for W-LED applications

The spectroscopic exploration of Dy3+ activated multicomponent borosilicate (DBS) glasses have been performed via optical absorption, fluorescence measurements, CIE colorimetry analysis and CCT values to investigate their role in the advancement of lighting sector. Oscillator strength values evaluated from the absorbance spectrum were utilized to determine phenomenological Judd-Ofelt (JO) parameters through least square fitting procedure. The fluorescence spectra of DBS glasses under the irradiation of 348 nm epitomize three emission bands which fall in yellow, blue and red region. Various radiative characteristics of the synthesised glass were evaluated by using JO intensity parameters. The color characteristics of DBS glasses were also investigated and the estimated features recommend synthesised glasses for diverse lighting applications.

Prediction and screening of glass properties based on high-throughput molecular dynamics simulations and machine learning

The design of novel glass materials has been plagued by inefficient Edisonian "trial-and-error" discovery approaches. The machine learning (ML) algorithm was combined with molecular dynamics method to predict the properties of glass overcome the defect of single method. In this paper, six ML algorithms were systematically studied using the data set generated by molecular dynamics. It is demonstrated that this method has excellent and reliable prediction performance in the whole synthetic space. The ML model and the hyperparameter suitable for glass property prediction were selected by comparing the performance of the model after tuning the hyperparameter. The ML model was utilized for rapid and low-cost screening of components (105) of multicomponent glass to develop a database of component attributes as an example of its possible application. Five samples were prepared with random components for experimental validation, and the relative errors of densities and elastic moduli were less than 10%. This study can readily be extended to anticipate various compositional-property combinations, thus replacing empirical approaches of glass property prediction with related properties and applications.

The multicomponent oxide glass as a statistical ensemble of neighboring glassy compounds in the composition space

AbstractThe rapid and low‐cost development of multicomponent oxide glasses is a long‐standing issue in condensed matters and materials science. However, traditional experimental approaches based on trial‐and‐error and empirical rules are time consuming and high‐cost. Recently, with the proposal of the materials genome engineering, the “glass genome” has also attracted much attention, which can accelerate the development of multicomponent oxide glasses. Here, we present an alternative and more suitable description of a multicomponent oxide glass as a statistical ensemble of its neighboring glassy compounds (NGCs) in the composition space. Subsequently, the NGCs method was proposed to predict the structural features and physical properties of the multicomponent oxide glass by the statistical averages of structural features and physical properties of the NGCs. What is more, the NGCs method was systematically verified at the atomic‐level view through molecular dynamics simulations. The predicted results through the NGCs method were in good agreement with the simulated results in multicomponent oxide glasses (Na2O‐SiO2and Na2O‐CaO‐SiO2systems). This work supports the physical picture of multicomponent oxide glasses and further promotes the development of “glass genome,” which will accelerate the research of glass materials.

A new approach to design multicomponent metallic glasses using the mendeleev number

ABSTRACT Designing novel Multicomponent Metallic Glasses (MMGs) based on empirical parameters such as enthalpy of mixing () and configurational entropy () is a time-consuming exercise that requires various assumptions, limiting the capability to predict new MMG compositions. The current study involves constructing a modified Mendeleev Number () element scale based on many important elemental properties that impact the glass forming phenomena. Machine learning (ML) was used to assess the competence of the proposed to predict MMGs. The ML findings demonstrate that proposed can be utilised as a salient attribute to predict MMGs with 87.8% cross-validation accuracy. Further, the mean square variation in the of the alloy constituents () provides a delineated zone of glass forming multicomponent alloys. In summary, the research work presents a novel phenomenological coordinate system that can effectively predict new MMGs while avoiding the limitations of empirical parameters based design strategies.

Effect of pressure quenching on the structures and properties of borosilicate glasses: Insights from molecular dynamics simulations

Combining thermal and pressure effect represents a novel approach to modify glass properties. However, the microscopic structural origin of these property modifications is complex and far from fully understood, especially in multicomponent glasses with mixed glass formers. In this paper, we have utilized classical molecular dynamics simulations with a set of composition dependent potentials to investigate pressure-quenching effect on sodium borosilicate glasses. Processes including hot compression, cold compression and subsequent annealing on the structures and properties are investigated and compared. It was found that applying pressure up to 10 GPa at the glass transition temperature led to permanent densifications and a dramatic increase of elastic moduli by 90%, while thermal annealing reversed the increase and applying pressure at ambient temperture did not increase the modulus. The main structural change of the hot compressed sample is the increase of four-fold coordinated boron while silicon remains four-fold coordinated. The sodium environment shows an increase of coordination number and a decrease of Na O and Na Na bond distances. Medium range structure is also changed with an increase of 8-membered rings. These results provide atomistic insights of the pressure quench effect on borosilicate glasses. • Compared cold compression, compression near T g and annealing effect on glass structure and properties • Up to 90% increase of elastic moduli due to hot compression while cold compression led to little change of elastic properties • Hot compression increases [4] B and Na coordination while a decrease of Na O bond distance • Medium range structure change observed in ring size distribution • Combing thermal and pressure effect a novel way to modify glass properties