Icosahedral Order, Frustration, and the Glass Transition: Evidence from Time-Dependent Nucleation and Supercooled Liquid Structure Studies

Shen, Yuefei; Kim, T. H.; Gangopadhyay, A. K.; Kelton, K. F.

doi:10.1103/physrevlett.102.057801

Cited by 159 publications

(73 citation statements)

References 35 publications

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“…The qualitative change in the ordering kinetics evident in Fig. 3 below about 28°C is strikingly similar to the phenomena referred to as fast crystal growth in certain glass-forming liquids, where diffusion limitations activate the rapid development of local order through a diffusionless process (41)(42)(43)(44). We speculate that the rapid growth in elasticity before the development of the Frank-Kasper phase may reflect the formation of clusters with tetrahedral, or perhaps more symmetrically arranged (e.g., icosahedral) coordination (45), facilitating fast nucleation of BCC order, which ultimately slowly reorganizes into the σ-phase.…”

Section: Discussionmentioning

confidence: 61%

Sphericity and symmetry breaking in the formation of Frank–Kasper phases from one component materials

Lee

Leighton

Bates

2014

Proc. Natl. Acad. Sci. U.S.A.

230

362

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Frank-Kasper phases are tetrahedrally packed structures occurring in numerous materials, from elements to intermetallics to selfassembled soft materials. They exhibit complex manifolds of Wigner-Seitz cells with many-faceted polyhedra, forming an important bridge between the simple close-packed periodic and quasiperiodic crystals. The recent discovery of the Frank-Kasper σ-phase in diblock and tetrablock polymers stimulated the experiments reported here on a poly(isoprene-b-lactide) diblock copolymer melt. Analysis of small-angle X-ray scattering and mechanical spectroscopy exposes an undiscovered competition between the tendency to form self-assembled particles with spherical symmetry, and the necessity to fill space at uniform density within the framework imposed by the lattice. We thus deduce surprising analogies between the symmetry breaking at the body-centered cubic phase to σ-phase transition in diblock copolymers, mediated by exchange of mass, and the symmetry breaking in certain metals and alloys (such as the elements Mn and U), mediated by exchange of charge. Similar connections are made between the role of sphericity in real space for polymer systems, and the role of sphericity in reciprocal space for metallic systems such as intermetallic compounds and alloys. These findings establish new links between disparate materials classes, provide opportunities to improve the understanding of complex crystallization by building on synergies between hard and soft matter, and, perhaps most significantly, challenge the view that the symmetry breaking required to form reduced symmetry structures (possibly even quasiperiodic crystals) requires particles with multiple predetermined shapes and/or sizes.symmetry breaking | sphericity | Frank-Kasper phases | block polymers T he discovery of materials with aperiodic order, often referred to as "quasicrystals," 30 years ago (1, 2) heralded new and promising vistas for designing materials endowed with unique properties. In the 1950s Frank and Kasper (3, 4) recognized complex tetrahedral atomic-and molecular-packing geometries that bridge the familiar close-packed crystals [e.g., face-centered cubic (FCC), hexagonally close-packed (HCP), and body-centered cubic (BCC) structures] characterized by periodic order, and quasiperiodic crystals (QCs) that extend crystallography beyond the 230 space groups relevant to periodic crystals (5, 6). The scientific literature is replete with examples of Frank-Kasper phases in hard materials, particularly in the area of intermetallics (7-9), but also in a few complex elemental crystals, including manganese (10, 11) and uranium (12). Recently, this class of crystalline order has cropped up in a host of soft materials, including dendrimers (13), surfactant solutions (14), and block polymers (15, 16), often in close proximity to QC phases (17)(18)(19). To the best of our knowledge the principles underlying the formation of Frank-Kasper phases across both categories of materials have not been established, presenting enticing challenges to sc...

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Section: Discussionmentioning

confidence: 61%

Sphericity and symmetry breaking in the formation of Frank–Kasper phases from one component materials

Lee

Leighton

Bates

2014

Proc. Natl. Acad. Sci. U.S.A.

230

362

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“…Such entities are homogeneously formed in glass-forming melts, and act as growth nuclei of crystals above the glass transition [4]. The formation of icosahedral nanoclusters has often been studied by molecular dynamics simulations into or out of liquids [5][6][7][8].…”

Section: Introductionmentioning

confidence: 99%

Crystallization of Supercooled Liquid Elements Induced by Superclusters Containing Magic Atom Numbers

Tournier

2014

Metals

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A few experiments have detected icosahedral superclusters in undercooled liquids. These superclusters survive above the crystal melting temperature T m because all their surface atoms have the same fusion heat as their core atoms, and are melted by liquid homogeneous and heterogeneous nucleation in their core, depending on superheating time and temperature. They act as heterogeneous growth nuclei of crystallized phase at a temperature T c of the undercooled melt. They contribute to the critical barrier reduction, which becomes smaller than that of crystals containing the same atom number n. After strong superheating, the undercooling rate is still limited because the nucleation of 13-atom superclusters always reduces this barrier, and increases T c above a homogeneous nucleation temperature equal to T m /3 in liquid elements. After weak superheating, the most stable superclusters containing n = 13, 55, 147, 309 and 561 atoms survive or melt and determine T c during undercooling, depending on n and sample volume. The experimental nucleation temperatures T c of 32 liquid elements and the supercluster melting temperatures are predicted with sample volumes varying by 18 orders of magnitude. The classical Gibbs free energy change is used, adding an enthalpy saving related to the Laplace pressure change associated with supercluster formation, which is quantified for n = 13 and 55.

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“…In fact, Cu content did not forming direct ratio to GFA in Zr-Cu system. For example, it was well know that the tow best glass formers were Zr 50 Cu 50 [10,13] and Zr 35.5 Cu 64.5 [9] , at which 2mm rods could be cast completely metallic glasses, in Zr-Cu systems, according to previously reported experimental and simulations result. However, the f F-ICO values for Zr 50 Cu 50 and Zr 35.5 Cu 64.…”

Section: Resultsmentioning

confidence: 76%

“…Full Icosahedra(F-ICO) as a short-range order had been found in a lot of amorphous alloys. F-ICO clusters were observed not only in Zr-Cu binary amorphous alloy, but also in high temperature melt by ab initio molecular dynamics(MD) [8,9,10] . In previous works, F-ICO increased the viscosity of the liquids and contributed to an enhance GFA [11,12] , whereas other types of polyhedral could not show the property.…”

Section: Introductionmentioning

confidence: 99%

Relation of Structure, Composition and Glass Forming Ability in Zr-Cu Binary Amorphous Alloys

2016

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Abstract.Molecular dynamics simulation was used to simulate Zr-Cu binary system, in which the relationship between structure, composition and glass forming ability was study. Atomic local structures were analyzed from view of chemical and topological short range order. Reduction fraction of full icosahedra(B c ) was developed to establish the relation of structure-composition and glass forming ability(GFA) in Zr-Cu binary system. Obviously peaks were observed at some certain compositions which own the good GFA. As a structure factor, B c could be a indicator of GFA of Zr-Cu alloys. Our works contributed to further understanding the effect of atomic structures on glass forming.

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Icosahedral Order, Frustration, and the Glass Transition: Evidence from Time-Dependent Nucleation and Supercooled Liquid Structure Studies

Cited by 159 publications

References 35 publications

Sphericity and symmetry breaking in the formation of Frank–Kasper phases from one component materials

Sphericity and symmetry breaking in the formation of Frank–Kasper phases from one component materials

Crystallization of Supercooled Liquid Elements Induced by Superclusters Containing Magic Atom Numbers

Relation of Structure, Composition and Glass Forming Ability in Zr-Cu Binary Amorphous Alloys

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