6533b7d1fe1ef96bd125c2e7
RESEARCH PRODUCT
Modeling non-linear dielectric susceptibilities of supercooled molecular liquids
Thomas Specksubject
Materials scienceFOS: Physical sciencesGeneral Physics and AstronomyDisordered Systems and Neural Networks (cond-mat.dis-nn)DielectricCondensed Matter - Soft Condensed MatterCondensed Matter - Disordered Systems and Neural NetworksAmorphous solidDielectric spectroscopyCondensed Matter::Soft Condensed MatterNonlinear systemChemical physicsSoft Condensed Matter (cond-mat.soft)PolarRelaxation (physics)Physical and Theoretical ChemistrySupercoolingGlass transitiondescription
Advances in high-precision dielectric spectroscopy have 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 the 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.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2021-01-01 |