Modeling non-linear dielectric susceptibilities of supercooled molecular liquids

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 provide strong support for theories dynamic arrest based on the thermodynamic amorphous order. Here, we approach this question from perspective facilitation, an alternative view focusing emergent kinetic constraints underlying a liquid approaching its glass transition. We derive explicit expressions frequency-dependent higher-order exhibiting shape, height which increases as temperature is lowered. demonstrate excellent agreement with experimental data glycerol, challenging idea that response functions reveal correlated relaxation supercooled