Fragility and the rate of change of the energy landscape topography

Beg, Cameran; Kieffer, John

doi:10.1016/j.nocx.2022.100101

Cited by 2 publications

(2 citation statements)

References 44 publications

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“…The free energy landscape model for SCLs has been widely accepted for the analysis of their glass transition and structural relaxation phenomena, in which SCLs consist of many basins (valleys) with different depths, that is, the local region with shallow basins and the local region with deep basins. [48][49][50] Very recently, the present authors 32 proposed that the local region with shallow basins would correspond to the local fragile region in the DNCF model, whereas the local region with deep basins would correspond to the local strong region, consequently an activation energy for crystal nucleation in the local fragile region would be low compared with the local strong region.…”

Section: Heterogeneous Structure and Nanoscale Composition Fluctuationsmentioning

confidence: 76%

“…proposed that the nucleation of fresnoite Ba 2 TiSi 2 O 8 crystals takes place predominantly in some “floppy regions,” and not in “rigid regions.” Abyzov et al 26 . proposed that nucleation processes may proceed with detectable rates only in “liquid‐like regions” and are suppressed in “solid‐like regions.” The terms of “floppy regions” and “liquid‐like regions” would correspond to “nanoscale fragile regions,” and “rigid regions” and “solid‐like regions” would have the same structural meaning as “strong regions.” The free energy landscape model for SCLs has been widely accepted for the analysis of their glass transition and structural relaxation phenomena, in which SCLs consist of many basins (valleys) with different depths, that is, the local region with shallow basins and the local region with deep basins 48–50 . Very recently, the present authors 32 proposed that the local region with shallow basins would correspond to the local fragile region in the DNCF model, whereas the local region with deep basins would correspond to the local strong region, consequently an activation energy for crystal nucleation in the local fragile region would be low compared with the local strong region.…”

Section: Scientific Background Behind Nucleation and Nanocrystallizationmentioning

confidence: 86%

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A new perspective for nucleation and nanocrystallization from interfacial energy and nanoscale composition fluctuations in glasses

Komatsu,

Honma

2023

Int J of Appl Glass Sci

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Nucleation behaviors in glasses/supercooled liquids (SCLs) such as lithium disilicate Li2O–2SiO2, cordierite Mg2Al4Si5O18, fresnoite Ba2TiSi2O8, and K2O–Nb2O5–GeO2/TeO2 glasses were analyzed and discussed from the interfacial energy γ at SCL–nucleus interfaces and nanoscale composition fluctuations. Based on the fragility concept for SCLs and the intrinsic origin of γ, the magnitude order of γ(fragile SCL) < γ(strong SCL) was proposed to be a crucial guide for an understanding of high homogeneous nucleation rates and prominent nanocrystallization. The role of nucleating agent TiO2/ZrO2 in accelerating the nucleation rate in cordierite‐based and β‐spodumene‐type Li2O–Al2O3–SiO2‐based glasses was discussed from the new perspective of γ(homoepitaxial‐like nucleation) < γ(heteroepitaxial‐like nucleation). Ferroelectric nanocrystals such as SrxBa1–xNb2O6 in borate glasses and fluoride nanocrystals such as CaF2 are also well understood from the proposed guidelines. The present article provides a new perspective for nucleation in glasses/SCLs, contributing to the comprehensive composition design of new innovative glass‐ceramics.

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Section: Heterogeneous Structure and Nanoscale Composition Fluctuationsmentioning

confidence: 76%

Section: Scientific Background Behind Nucleation and Nanocrystallizationmentioning

confidence: 86%

A new perspective for nucleation and nanocrystallization from interfacial energy and nanoscale composition fluctuations in glasses

Komatsu,

Honma

2023

Int J of Appl Glass Sci

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Boosting cation mobility in sol-gel derived organic–inorganic hybrid solid electrolytes through physical conditioning

Keshishian,

Wang,

Kieffer

2024

The Journal of Chemical Physics

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Organic–inorganic hybrid materials are explored for application as solid electrolytes for lithium-ion batteries. The material consists of a porous silica network, of which the pores are infiltrated by poly(ethylene oxide) and lithium perchlorate. The synthesis involves two steps: First, the inorganic backbone is created by the acid-catalyzed sol-gel synthesis of tetraethyl orthosilicate to ensure continuity of the backbone in three dimensions. In the second step, the polymer and salt are imbued into the porous backbone via solvent exchange. During drying, the cylindrical disk-shaped specimens shrink mainly in the radial direction, which results in spatially non-uniform structural developments. While this inhomogeneity is not discernible in the material’s chemical compositional or thermal properties, it is manifest in its ionic conductivity and adiabatic elastic modulus. The ionic conductivity in the center of the specimens is projected to be between one and two orders of magnitude higher than the measured average across the sample diameter. The process that yields a structure with enhanced ionic mobility during post-synthesis physical conditioning is inferred from careful analysis and numerical interpretation of measurable quantities, and the implications for the design of nanostructured hybrid electrolytes with high ionic conductivity are discussed.

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Fragility and the rate of change of the energy landscape topography

Cited by 2 publications

References 44 publications

A new perspective for nucleation and nanocrystallization from interfacial energy and nanoscale composition fluctuations in glasses

A new perspective for nucleation and nanocrystallization from interfacial energy and nanoscale composition fluctuations in glasses

Boosting cation mobility in sol-gel derived organic–inorganic hybrid solid electrolytes through physical conditioning

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