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Theoretical studies of UO2(OH)(H2O)n+, UO2(OH)2(H2O)n, NpO2(OH)(H2O)n, and PuO2(OH)(H2O)n+ (n<=21) complexes in aqueous solution
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Computing the viscosity of supercooled liquids. II. Silica and strong-fragile crossover behavior

J. Chem. Phys. 131, 164505 (2009); doi:10.1063/1.3243854

Published 27 October 2009

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Akihiro Kushima,1 Xi Lin,2 Ju Li,3 Xiaofeng Qian,1 Jacob Eapen,4 John C. Mauro,5 Phong Diep,5 and Sidney Yip1
1Department of Nuclear Science and Engineering and Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
2Department of Mechanical Engineering and Division of Materials Science and Engineering, Boston University, Boston, Massachusetts 02215, USA
3Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA
4Department of Nuclear Engineering, North Carolina State University, Raleigh, North Carolina 27695, USA
5Science and Technology Division, Corning Incorporated, Corning, New York 14831, USA
A recently developed atomistic method capable of calculating the fragile (non-Arrhenius) temperature behavior of highly viscous liquids is further tested by studying a model of SiO2, a glass former well known for its Arrhenius temperature behavior (strong). The method predicts an Arrhenius temperature variation, in agreement with experiments, the origin of which is revealed by both quantitative and qualitative results on transition state pathways, activation barrier analysis, energy landscape connectivity, and atomistic activation mechanisms. Also predicted is a transition from fragile to strong behavior at a lower viscosity, below the range of measurements, which had been previously suggested on the basis of molecular dynamics simulations. By systematically comparing our findings with corresponding results on the binary Lennard-Jones system (fragile) we gain new insights into the topographical features of the potential energy landscape, characteristics that distinguish strong from fragile glassy systems. We interpret fragility as a universal manifestation of slowing of dynamics when the system becomes trapped in deep energy basins. As a consequence, all glass-forming systems, when cooled from their normal liquid state, should exhibit two transitions in temperature scaling of the viscosity, a strong-to-fragile crossover followed by a second transition reverting back to strong behavior. ©2009 American Institute of Physics
History: Received 2 February 2009; accepted 16 September 2009; published 27 October 2009
Permalink: http://link.aip.org/link/?JCPSA6/131/164505/1
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KEYWORDS and PACS

Keywords
PACS
  • 66.20.-d
    Viscosity of liquids; diffusive momentum transport
  • 61.20.-p
    Structure of liquids
  • 61.20.Ja
    Computer simulation of liquid structure
  • 64.70.P-
    Glass transitions of specific systems
  • 64.70.pm
    Glass transition in liquids
  • YEAR: 2009

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PUBLICATION DATA

ISSN:
0021-9606 (print)   1089-7690 (online)
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