Modeling non-linear dielectric susceptibilities of supercooled molecular liquids

Abstract

Advances in high-precision dielectric spectroscopy has enabled access to non-linear susceptibilities of polar molecular liquids. The observed non-monotonic behavior has been claimed to provide strong support for theories of dynamic arrest based on thermodynamic amorphous order. Here we approach this question from the perspective of dynamic facilitation, an alternative view focusing on emergent kinetic constraints underlying the dynamic arrest of a liquid approaching its glass transition. We derive explicit expressions for the frequency-dependent higher-order dielectric susceptibilities exhibiting a non-monotonic shape, the height of which increases as temperature is lowered. We demonstrate excellent agreement with the experimental data for glycerol, challenging the idea that non-linear response functions reveal correlated relaxation in supercooled liquids.

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Cited by in corpus (5)

• The Many Faces of Fluctuation-Dissipation Relations Out of Equilibrium
• Emergence of a Hump in the Cubic Dielectric Response of Glycerol
• Nonlinear dielectric response in glasses: restoring forces and avoided spin-glass criticality
• Nonlinear response theory for Markov processes IV: The asymmetric double well potential model revisited
• Chain-length-dependent correlated molecular motion in polymers