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At least 1,063 records · Page 59

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DOE OSTI2023

Revealing the relationship between liquid fragility and medium-range order in silicate glasses

Despite decades of studies, the nature of the glass transition remains elusive. In particular, the sharpness of the dynamical arrest of a melt at the glass transition is captured by its fragility. Here, we reveal that fragility is governed by the medium-range order structure. Based on neutron-diffraction data for a series of aluminosilicate glasses, we propose a measurable structural parameter that features a strong inverse correlation with fragility, namely, the average medium-range distance (MRD). We use in-situ high-temperature neutron-scattering data to discuss the physical origin of this correlation. We argue that glasses exhibiting low MRD values present an excess of small network rings. Such rings are unstable and deform more readily with changes in temperature, which tends to increase fragility. These results reveal that the sharpness of the dynamical arrest experienced by a silicate glass at the glass transition is surprisingly encoded into the stability of rings in its network.

36 MATERIALS SCIENCE↗

DOE OSTI2011

A molecular view of vapor deposited glasses

Recently, novel organic glassy materials that exhibit remarkable stability have been prepared by vapor deposition. The thermophysical properties of these new ''stable'' glasses are equivalent to those that common glasses would exhibit after aging over periods lasting thousands of years. The origin of such enhanced stability has been elusive; in the absence of detailed models, past studies have discussed the formation of new polyamorphs or that of nanocrystals to explain the observed behavior. In this work, an atomistic molecular model of trehalose, a disaccharide of glucose, is used to examine the properties of vapor-deposited stable glasses. Consistent with experiment, the model predicts the formation of stable glasses having a higher density, a lower enthalpy, and higher onset temperatures than those of the corresponding ''ordinary'' glass formed by quenching the bulk liquid. Simulations reveal that newly formed layers of the growing vapor-deposited film exhibit greater mobility than the remainder of the material, thereby enabling a reorganization of the film as it is grown. They also reveal that ''stable'' glasses exhibit a distinct layered structure in the direction normal to the substrate that is responsible for their unusual properties.

36 MATERIALS SCIENCE↗

DOE OSTI2011

Structural origin of the nonlinear optical properties of lead niobium germanate film glasses

The structural origin of the nonlinear optical susceptibility (/{chi}{sup (3)}/) of lead-niobium-germanate film glasses with large Nb{sub 2}O{sub 5} contents has been investigated. /{chi}{sup (3)}/ shows a strong enhancement with the Nb content in the films with /{chi}{sup (3)}/ values close to 2 x 10{sup -11} esu at 800 nm for a Nb content as high as 0.71. Boling-Glass-Owyoung and Lines' semiempirical models predict accurately the values of /{chi}{sup (3)}/ for transparent bulk glasses but not for film glasses. This discrepancy is related to the remarkable structural differences between them. Raman spectroscopy suggests the formation of a three-dimensional (3D) structure of [NbO{sub 6}] octahedra in the case of film glasses having large Nb contents, while X-ray photoelectron spectroscopy shows that a significant fraction of these units contain Nb{sup 4+} ions. The combination of a 3D structure of [NbO{sub 6}] with the presence of Nb{sup 4+} polarons and their migration through electron intervalence transfer is proposed as the origin of the observed enhancement of /{chi}{sup (3)}/ in the film glasses.

36 MATERIALS SCIENCE↗

DOE OSTI2011

Thermal studies of Se{sub 85-x}Te{sub 15}In{sub x} (x = 3,6,9,12) glasses

Bulk glasses of compositions Se{sub 85-x}Te{sub 15}In{sub x} (x = 3,6,9,12) are prepared by melt quenching technique and Differential scanning calorimetry (DSC) is employed to study the thermal stability, crystallization mechanism as well as specific heat of these glasses. It is found that the addition of indium increases the glass transition temperature. From the heating rate dependence of the glass transition temperature the activation energy of glass transition is determined using Kissinger's equation for non-isothermal crystallization of materials. An attempt has been made to explain the variation in the value of T{sub c}, T{sub p} and {Delta}C{sub p} for the composition Se{sub 73}Te{sub 15}In{sub 12} using rigidity percolation threshold (RPT). From the values of (T{sub c}-T{sub g}) the stable glass system is determined.

36 MATERIALS SCIENCE↗

DOE OSTI2012

Thermodynamic, Raman and electrical switching studies on Si{sub 15}Te{sub 85-x}Ag{sub x} (4 {<=} x {<=} 20) glasses

We have investigated thermal properties of bulk Si{sub 15}Te{sub 85-x}Ag{sub x} (4 {<=} x {<=} 20) glasses in detail, through alternating differential scanning calorimetry experiments. The composition dependence of thermal parameters reveal the signatures of rigidity percolation and chemical threshold at compositions x = 12 and x = 19, respectively. The stability and glass forming ability of these glasses have also been determined using the data obtained from different thermodynamic quantities and it is found that the Si{sub 15}Te{sub 85-x}Ag{sub x} glasses in the region 12 {<=} x {<=} 17 are more stable when compared to other glasses of the same series. Further, the blueshift observed in Raman spectroscopy investigations, in the composition range 12 {<=} x {<=} 13, support the occurrence of stiffness threshold in this composition range. All Si{sub 15}Te{sub 85-x}Ag{sub x} (4 {<=} x {<=} 20) glasses are found to exhibit memory type switching (for sample thickness 0.25 mm) in the input current range 3-9 mA. The effect of rigidity percolation and chemical thresholds on switching voltages are observed at x = 12 and 19, respectively.

36 MATERIALS SCIENCE↗

DOE OSTI2012

Thermal analysis, spectral characterization and refractive index studies of lithium doped PbO-ZnO-B{sub 2}O{sub 3} glass

Lithium containing lead zinc borate glasseshave been prepared by melt quenching technique. X-ray diffraction reveals the amorphous nature of the glass. Differential scanning calorimeter (DSC) study was carried out in the temperature range RT to 600 deg. C temperature and found glass transition temperature of these glasses decreases with increase in inter substitution of Pb and Zn lithium content. PZB glasses are stable, IR spectra of these glasses show characteristics band originating from borate groups namely [BO{sub 3}] [BO{sub 4}]and B-O-B stretching vibrations respectively, and found that structure is not affected with effect of lithium content. Refractive index of these glasses are in the range of 1.47 with increasing lithium content refractive index decreases indicating decrease in scattering of light.

36 MATERIALS SCIENCE↗

DOE OSTI2014

XRD, lead equivalent and UV-VIS properties study of Ce and Pr lead silicate glasses

In this work, Cerium (Ce) and Praseodymium (Pr) containing lead silicate glasses were produced with 2 different molar ratios low (0.2 wt%) and high (0.4wt%). These types of glasses can satisfy the characteristics required for radiation shielding glasses and minimize the lead composition in glass. The radiation shielding properties of the synthesized glasses is explained in the form of lead equivalent study. The XRD diffraction and UV-VIS analysis were performed to observe the structural changes of the synthesis glasses at 1.5 Gy gamma radiation exposures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Transition threshold in Ge{sub x}Sb{sub 10}Se{sub 90−x} glasses

Ge{sub x}Sb{sub 10}Se{sub 90−x} glasses with Ge content from 7.5 to 32.5 at. % have been prepared by melt-quench technique, and the physical parameters including glass transition temperature (T{sub g}), density (ρ), compactness (C), shear elastic moduli (C{sub s}), compression elastic moduli (C{sub c}), refractive index (n), and optical bandgap (E{sub g}) have been investigated. While all these physical parameters show threshold behavior in the glass with a chemically stoichiometric composition. Raman spectra analysis also indicates that, with increasing Ge content, Se-chains or rings gradually disappear until all Se-atoms are consumed in the glass with a chemically stoichiometric composition. With further increasing Ge content, homopolar Ge-Ge and Sb-Sb bonds are formed and the chemical order in the glasses is violated. The threshold behavior of the physical properties in the Ge{sub x}Sb{sub 10}Se{sub 90−x} glasses can be traced to demixing of networks above the chemically stoichiometric composition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Analysis of emission spectra of Ho{sup 3+}:LFBCd glasses

In the present paper, we report on the absorption and emission properties of (0.1-1.5 mol %) Ho{sup 3+} doped LFBCd (Li{sub 2}O{sub −}LiF{sub −}B{sub 2}O{sub 3−}CdO) glasses prepared via melt quenching method. On exciting these glasses at (λ{sub exci}) = 452 nm, two emissions at 556 nm ({sup 5}S{sub 2}→{sup 5}I{sub 8}; Green), 655 nm ({sup 5}F{sub 5}→{sup 5}I{sub 8}; Red) have been obtained. Upon exciting these glasses with a 980 nm diode laser, NIR emissions at 1195 nm ({sup 5}I{sub 6}→{sup 5}I{sub 8}), 1951 nm ({sup 5}I{sub 7}→{sup 5}I{sub 8}) have been measured for 1 mol % Ho{sup 3+}:LFBCd glass. For higher concentration beyond 1.0 mol %, emission quenching of Ho{sup 3+} glass has been noticed and which has successfully been explained in terms of an energy level diagram. From absorption cross-section data, stimulated emission cross-section has been evaluated by applying McCumber's theory and further cross-sectional gain has also been computed for the emissions at 1195 nm (∼1.20 μm) and 1951 nm (∼2.0 μm) of 1 mol % Ho{sup 3+}:LFBCd glass.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Effect of CaF{sub 2} addition on optical properties of barium phosphate glasses

Ternary barium phosphate glasses, (50−X)BaO−XCaF{sub 2}−50P{sub 2}O{sub 5} have been prepared by adding 0-10 mol% of CaF{sub 2} to binary barium phosphate glasses. The amorphous nature of the prepared glasses was confirmed by X-ray diffraction technique. The UV-Visible absorption spectra have been recorded, optical band gap energy Eopt and Urbach energy Etail were determined. Shift in Eopt and Etail with increase in concentration of CaF{sub 2} is noted. FTIR analysis was carried out to investigate the short and intermediate-range orders in glasses. Shift of (P-O-P) band to higher wave number with the substitution of BaO with CaF{sub 2} shows the shortening of the phosphate chains. Hardness and density of glass samples were measured and correlated with the composition of glasses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Fast and slow crystal growth kinetics in glass-forming melts

Published values of crystal growth rates are compared for supercooled glass-forming liquids undergoing congruent freezing at a planar crystal-liquid interface. For the purposes of comparison pure metals are considered to be glass-forming systems, using data from molecular-dynamics simulations. For each system, the growth rate has a maximum value U{sub max} at a temperature T{sub max} that lies between the glass-transition temperature T{sub g} and the melting temperature T{sub m}. A classification is suggested, based on the lability (specifically, the propensity for fast crystallization), of the liquid. High-lability systems show “fast” growth characterized by a high U{sub max}, a low T{sub max} / T{sub m}, and a very broad peak in U vs. T / T{sub m}. In contrast, systems showing “slow” growth have a low U{sub max}, a high T{sub max} / T{sub m}, and a sharp peak in U vs. T / T{sub m}. Despite the difference of more than 11 orders of magnitude in U{sub max} seen in pure metals and in silica, the range of glass-forming systems surveyed fit into a common pattern in which the lability increases with lower reduced glass-transition temperature (T{sub g} / T{sub m}) and higher fragility of the liquid. A single parameter, a linear combination of T{sub g} / T{sub m} and fragility, can show a good correlation with U{sub max}. For all the systems, growth at U{sub max} is coupled to the atomic/molecular mobility in the liquid. It is found that, across the diversity of glass-forming systems, T{sub max} / T{sub g} = 1.48 ± 0.15.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Indentation size effect and the plastic compressibility of glass

Oxide glasses exhibit significant densification under an applied isostatic pressure at the glass transition temperature. The glass compressibility is correlated with the chemical composition and atomic packing density, e.g., borate glasses with planar triangular BO{sub 3} units are more disposed for densification than silicate glasses with tetrahedral units. We here show that there is a direct relation between the plastic compressibility following hot isostatic compression and the extent of the indentation size effect (ISE), which is the decrease of hardness with indentation load exhibited by most materials. This could suggest that the ISE is correlated with indentation-induced shear bands, which should form in greater density when the glass network is more adaptable to volume changes through structural and topological rearrangements under an applied pressure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Field-assisted patterned dissolution of silver nanoparticles in phosphate glass

Phosphate glass samples doped with silver ions through a Na⁺-Ag⁺ ion-exchange process were treated in a hydrogen atmosphere at temperatures near 430°C for durations ranging from 4 to 5 h. Such treatment causes metallic silver precipitation at the surface as well as nanoclustering of silver atoms under the surface under conditions very similar to those used for silicate glasses. The presence of silver clusters resulted in a characteristic coloring of the glass and was verified by the observation of a plasmon resonance peak near 410–420 nm in the absorption spectra. Applying a DC voltage between 1.4 and 2 kV at temperatures between 120 and 130°C led to dissolution of the clusters in the area under the positive electrode, thereby bleaching the glass color. The use of a patterned doped-silicon electrode further led to the formation of a 300 nm thick surface relief on the glass surface and of a volume complex permittivity grating extending at least 4 μm under the surface. Such volume complex refractive index gratings may find applications in passive or active (laser) photonic devices in rare-earth doped phosphate glasses, where conventional bulk grating formation techniques have limited applicability.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2014

Study of optical properties of Erbium doped Tellurite glass-polymer composite

Chalcogenide glasses have wide applications in optical device technology. But it has some disadvantages like thermal instability. Among them Tellurite glasses exhibits high thermal Stability. Doping of rare earth elements into the Tellurite glasses improve its optical properties. To improve its mechanical properties composites of this Tellurite glasses with polymer are prepared. Bulk samples of Er{sub 2}O{sub 3} doped TeO{sub 2}‐WO{sub 3}‐La{sub 2}O{sub 3} Tellurite glasses are prepared from high purity oxide mixtures, melting in an alumina crucible in air atmosphere. Composites of this Tellurite glasses with polymer are prepared by powder mixing method and the thin films of these composites are prepared using polymer press. Variations in band gap of these composites are studied from the UV/Vis/NIR absorption.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Radiation hardening in sol-gel derived Er{sup 3+}-doped silica glasses

The aim of the present paper is to report the effect of radiation on the Er{sup 3+}-doped sol-gel silica glasses. A possible application of these sol-gel glasses could be their use in harsh radiation environments. The sol-gel glasses are fabricated by densification of erbium salt-soaked nanoporous silica xerogels through polymeric sol-gel technique. The radiation-induced attenuation of Er{sup 3+}-doped sol-gel silica is found to increase with erbium content. Electron paramagnetic resonance studies reveal the presence of E′{sub δ} point defects. This happens in the sol-gel aluminum-silica glass after an exposure to γ-rays (kGy) and in sol-gel silica glass after an exposure to electrons (MGy). The concentration levels of these point defects are much lower in γ-ray irradiated sol-gel silica glasses. When the samples are co-doped with Al, the exposure to γ-ray radiation causes a possible reduction of the erbium valence from Er{sup 3+} to Er{sup 2+} ions. This process occurs in association with the formation of aluminum oxygen hole centers and different intrinsic point defects.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Spectroscopic study of neodymium doped lead-bismuth-borate glasses

This paper reports on different physical and optical properties of rare earth doped heavy metal oxide glasses. The glass composition of 10Bi{sub 2}O{sub 3}-30PbO-60B{sub 2}O{sub 3}-xNd{sub 2}O{sub 3} where x = 0, 0.1, 0.2, 0.5 and 1 (in mol %) has been synthesized using melt-quenching technique. Refractive index measurements for these glasses were done and physical parameters were studied. Structural properties of these glasses were analysed through infrared spectra that was recorded between 1600cm{sup −1} and 300cm{sup −1} in transmission mode. The optical absorption spectra were recorded in the wavelength range from 300 to 700 nm. The transitions originated from ground state energy {sup 4}I{sub 9/2}. The energy level analysis has been carried out by considering absorption spectral bands. The results thus obtained are comparable with reports on similar glasses, indicating that the prepared glasses may have potential laser applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Spectroscopic and nonlinear optical studies of pure and Nd-doped lanthanum strontium borate glasses

Borate glasses of the system xNd{sub 2}O{sub 3}-(1-x) La{sub 2}O{sub 3}-SrCO{sub 3}-10H{sub 3}BO{sub 3} (with x = 0 and 0.05) were prepared by using a convectional melt quenching technique. The amorphous nature of the quenched glasses has been confirmed by powder X-ray diffraction analysis. In order to study the spectroscopic and nonlinear optical properties of fabricated glasses, ultraviolet-visible transmission spectroscopy and open aperture z-scan measurements have been employed. In Nd doped glasses, the transition {sup 4}I{sub 9/2} → {sup 4}G{sub 5/2} + {sup 2}G{sub 7/2} has found more prominent than the other transitions. Optical band gap energies of glasses have been determined and found less for Nd doped glass.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

Thermal and fragility studies on microwave synthesized K{sub 2}O-B{sub 2}O{sub 3}-V{sub 2}O{sub 5} glasses

Glasses with composition xK{sub 2}O–60B{sub 2}O{sub 3}–(40-x) V{sub 2}O{sub 5} (15 ≤ x ≤ 39 mol %) was prepared by an energy efficient microwave method. The heat capacity change (ΔC{sub p}) at glass transition (T{sub g}), width of glass transition (ΔT{sub g}), heat capacities in the glassy (C{sub pg}) and liquid (C{sub pl}) state for the investigated glasses were extracted from Modulated Differential Scanning Calorimetry (MDSC) thermograms. The width of glass transition is less than 30°C, indicating that these glasses belongs to fragile category. Fragility functions [NBO]/(V{sub m}{sup 3}T{sub g}) and (ΔC{sub p}/C{sub pl})increases with increasing modifier oxide concentration. Increase in fragility is attributed to the increasing coordination of boron. Further, addition of K{sub 2}O creates NBOs and the flow mechanism involves bond switching between BOs and NBOs. Physical properties exhibit compositional dependence and these properties increase with increasing K{sub 2}O concentration. The observed variations are qualitatively analyzed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗