Material functionalities from molecular rigidity: Maxwell’s modern legacy

Micoulaut, Matthieu; Yue, Yuanzheng

doi:10.1557/mrs.2016.298

Cited by 30 publications

(20 citation statements)

References 29 publications

(31 reference statements)

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“…Other properties Several other properties have been shown to be correlated with the topology of the atomic network [142]. For instance, stiffness was found to scale with the number of constraints per atom in select systems [25,143].…”

Section: 6mentioning

confidence: 99%

Topological Constraint Theory and Rigidity of Glasses

Bauchy¹

2019

21st Century Nanoscience – A Handbook

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Topological constraint theory has become an increasingly popular tool to predict the compositional dependence of glass properties or pinpoint promising compositions with tailored functionalities. This approach reduces complex disordered networks into simpler mechanical trusses. Thereby, topological constraint theory captures the important atomic topology that controls macroscopic properties while filtering out less relevant second-order structural details. As such, topological constraint theory can be used to decode the genome of glass, that is, to identify and decipher how the basic structural building blocks of glasses control their engineering properties-in the same way as the human genome offers information that serves as a blueprint for an individual's growth and development. Thanks to its elegance and simplicity, topological constraint theory has enabled the development of various physics-based models that can analytically predict various properties of glass. In this Chapter, I introduce some general background in glass science, concepts of atomic rigidity, and topological constraint theory. The topological constraints enumeration scheme is presented for various archetypical glasses and is used to understand the origin of their glass-forming ability. Finally, various topological models enabling the prediction of glass properties are reviewed, with a focus on hardness, fracture toughness, viscosity, fragility, glass transition temperature, and dissolution kinetics. Time Scientific progress Fig. 1: The discovery of new materials largely defines the progress of our civilization. Glass genome and discovery of new compositionsRevealing the full potential of glass requires the discovery of new glass formulations showing unique properties. However, this task is especially complicated for non-crystalline glassy materials for several reasons. First, virtually all the elements of the periodic table can be turned into a glass, if cooled fast enough from the liquid state [9]. Second, unlike crystals, glasses do not have to satisfy any fixed stoichiometry thanks to their out-of-equilibrium nature. As such, the composition of glasses can be continuously changed. For all these reasons, the number of possible glass compositions has been estimated to be around 1052! Yet, only about 200,000 glass compositions have been produced in the last 6000 years of human glass history [9]. These numbers demonstrate that the range of possible glasses remains largely unexplored-so that there exists an incredible opportunity for the future discovery of new glass formulations with unusual functionalities.However, although it offers a large room for improvement, the astronomical number of possible glass compositions is also a challenge. Indeed, such a large parametric space renders traditional Edisonian discovery approach based on trial-and-error largely inefficient. To accelerate the discovery of new glass formulations, it is necessary to decode the Glass Genome, that is, to decipher how the properties of glasses are controlled by their und...

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Section: 6mentioning

confidence: 99%

Topological Constraint Theory and Rigidity of Glasses

Bauchy¹

2019

21st Century Nanoscience – A Handbook

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“…The structures of the glasses, and the pristine and irradiated minerals were analyzed within the framework of topological constraint theory (TCT); also known as rigidity theory [53][54][55]. TCT captures the relevant features of the atomic topology which influence the kinetics of solid dissolution [35], while filtering out less relevant structural details.…”

Section: Molecular Dynamics (Md) Simulations For Assessing the Networmentioning

confidence: 99%

Rate controls on silicate dissolution in cementitious environments

Oey¹,

Hsiao²,

Callagon³

et al. 2017

RILEM Tech Lett

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The dissolution rate of silicate minerals and glasses in alkaline environments is of importance in cementitious systems due to its influences on: (a) earlyage reactivity that affects the rate of strength gain and microstructure formation, and/or, (b) chemical durability of aggregates; compromises in which can result deleterious processes such as alkali-silica reaction (ASR). In spite of decades of study, quantitative linkages between the atomic structure of silicates and their dissolution rate in aqueous media (i.e., chemical reactivity) has remained elusive. Recently, via pioneering applications of molecular dynamics simulations and nanoscale-resolved measurements of dissolution rates using vertical scanning interferometry, a quantitative basis has been established to link silicate dissolution rates to the topology (rigidity) of their atomic networks. Specifically, an Arrhenius-like expression is noted to capture the dependence between silicate dissolution rates and the average number of constraints placed on a central atom in a network (n c , i.e., an indicator of the network's rigidity). This finding is demonstrated by: (i) ordering fly ashes spanning Ca-rich/poor variants in terms of their reactivity, and, (ii) assessing alterations in the reactivity of albite, and quartz following irradiation due to their potential to induce ASR in concrete exposed to radiation, e.g., in nuclear power plants.

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“…Topological constraint theory has opened a new avenue to accelerate the discovery of new materials with tailored properties in which the usual and unusual tools of experimental condensed matter physics and ab initio MD simulations are now playing a crucial role. In a recent issue of MRS Bulletin, varied glass functionalities were examined using the approach. Some of the functionalities included enhanced thermal stability, Vickers hardness, chemical doping of photonic glasses to promote radiative transition and emission bandwidth, optimization of amorphous semiconductors and low‐/high‐k dielectrics for modern micro‐/nanoelectronics devices, phase‐change materials, granular materials, and nanoengineering of concrete .…”

Section: Correlating Melt Dynamics With Glass Topological Phases In Cmentioning

confidence: 99%

“…Topological constraint theory (TCT) evolved in 1979 with the basic premise that the glass forming tendency of a melt is optimized at a special connectivity usually described in terms of the mean coordination number,

〈 r 〉

, equal to 2.40. Here

〈 r 〉

= Σ n i · r i / N , where n i is the number of atoms possessing a coordination number r i and N = Σ n i designates the total number of atoms comprising a network.…”

Section: Introductionmentioning

confidence: 99%

“…Schematically, the three generic topological phases of network glasses are illustrated in Figure b.The existence of IPs is a striking development in the field, since networks formed in this phase possess unique thermal, optical, mechanical, and electrical properties, including nearly reversible glass transition, weak aging, minimum creep, maximum fracture toughness, among others. These unusual functionalities in the IPs have attracted widespread interest in applications of glasses and thin‐films. Here we will show that in chalcogenides the three topological phases formed in chalcogenide glasses are encoded in their melt dynamics.…”

Section: Introductionmentioning

confidence: 99%

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Topological Phases of Chalcogenide Glasses Encoded in the Melt Dynamics

Boolchand

Bauchy

Micoulaut

et al. 2018

Physica Status Solidi (b)

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Select Raman scattering and modulated differential scanning calorimetry (DSC) experiments on specially homogenized binary GexSe100–x and GexS100–x chalcogenide glasses, supported by ab initio MD simulations are undertaken. In both chalcogenides, the glasses exhibit a super‐strong behavior (with a melt fragility index, m(x) < 20) in the 20(1)% < x < 26(1)% composition range, defining the fragility window, and with m(x) > 20 as one goes away from the fragility window. Remarkably, molecular dynamics (MD) simulations confirm the existence of the fragility window. Furthermore, in both chalcogenide glasses, the enthalpy of relaxation at Tg, ΔHnr(x), becomes minuscule (≈0) in the 20(1)% < x < 26(1)% range, defining the reversibility window, and with ΔHnr(x) increasing by an order magnitude abruptly with x outside that window. Thus, super‐strong melts formed in the fragility window give rise to isostatically rigid glasses in the reversibility window and fragile melts formed at x < 20(1)% and at x > 26(1)% give rise to flexible‐ and stressed‐rigid glasses, respectively. Melt dynamics for the examined glass systems unequivocally encode the nature of the glass topological phases.

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Material functionalities from molecular rigidity: Maxwell’s modern legacy

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Cited by 30 publications

References 29 publications

Topological Constraint Theory and Rigidity of Glasses

Topological Constraint Theory and Rigidity of Glasses

Rate controls on silicate dissolution in cementitious environments

Topological Phases of Chalcogenide Glasses Encoded in the Melt Dynamics

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