Densified network glasses and liquids with thermodynamically reversible and structurally adaptive behaviour

Nature Communications
M Bauchy, M Micoulaut

Abstract

If crystallization can be avoided during cooling, a liquid will display a substantial increase of its viscosity, and will form a glass that behaves as a solid with a relaxation time that grows exponentially with decreasing temperature. Given this 'off-equilibrium' nature, a hysteresis loop appears when a cooling/heating cycle is performed across the glass transition. Here we report on molecular dynamics simulations of densified glass-forming liquids that follow this kind of cycle. Over a finite pressure interval, minuscule thermal changes are found, revealing glasses of 'thermally reversible' character with optimal volumetric or enthalpic recovery. By analysing the topology of the atomic network structure, we find that corresponding liquids adapt under the pressure-induced increasing stress by experiencing larger bond-angle excursions. The analysis of the dynamic behaviour reveals that the structural relaxation time is substantially reduced in these adaptive liquids, and also drives the reversible character of the glass transition. Ultimately, the results substantiate the notion of stress-free (Maxwell isostatic) rigidity in disordered molecular systems, while also revealing new implications for the topological engineering of c...Continue Reading

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Citations

Aug 9, 2016·The Journal of Chemical Physics·Isabella PignatelliGaurav Sant
Aug 30, 2016·ACS Applied Materials & Interfaces·Georgi V Stoychev, Leonid Ionov
Dec 20, 2016·The Journal of Physical Chemistry. B·Hicham JabraouiSaid Ouaskit
May 24, 2016·Reports on Progress in Physics·Matthieu Micoulaut
Nov 10, 2015·Physical Review Letters·Yingtian YuMathieu Bauchy
Apr 22, 2017·Physical Review Letters·M Micoulaut, M Bauchy
Jun 15, 2020·The Journal of Chemical Physics·W SongM Micoulaut
Dec 14, 2018·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Huynh Anh HuyGiang Hoang Nguyen
Feb 24, 2018·The Journal of Chemical Physics·Yingtian YuMathieu Bauchy
Sep 6, 2017·ACS Applied Materials & Interfaces·N M Anoop KrishnanMathieu Bauchy

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