Unifying different interpretations of the nonlinear response in glass-forming liquids

Abstract

This work aims at reconsidering several interpretations coexisting in the recent literature concerning non-linear susceptibilities in supercooled liquids. We present experimental results on glycerol and propylene carbonate showing that the three independent cubic susceptibilities have very similar frequency and temperature dependences, both for their amplitudes and phases. This strongly suggests a unique physical mechanism responsible for the growth of these non-linear susceptibilities. We show that the framework proposed by two of us [BB, Phys. Rev. B 72, 064204 (2005)], where the growth of non-linear susceptibilities is intimately related to the growth of "glassy domains", accounts for all the salient experimental features. We then review several complementary and/or alternative models, and show that the notion of cooperatively rearranging glassy domains is a key (implicit or explicit) ingredient to all of them. This paves the way for future experiments which should deepen our understanding of glasses.

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Cited by in corpus (8)

• The glass transition in molecules, colloids and grains: universality and specificity
• Third and Fifth Harmonic Responses in Viscous Liquids
• Modeling non-linear dielectric susceptibilities of supercooled molecular liquids
• Nonlinear response theory for Markov processes III: Stochastic models for dipole reorientations
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• Emergence of a Hump in the Cubic Dielectric Response of Glycerol
• Nonlinear dielectric response in glasses: restoring forces and avoided spin-glass criticality
• Amorphous Order & Non-linear Susceptibilities in Glassy Materials