Emergence of a Hump in the Cubic Dielectric Response of Glycerol
arXiv:2410.00867 · doi:10.1103/PhysRevLett.134.218202
Abstract
We report a direct determination of the cubic dielectric spectra of a realistic polar molecule, glycerol, from molecular dynamic (MD) simulations. From the liquid state to the mildly supercooled regime, we observed the emergence and growth of a hump in the cubic modulus, traditionally associated with collective effects in the dynamics. Its evolution follows that of dynamical correlations probed by the four-point susceptibility and that of the activation energy of the relaxation time. In particular, its appearance at high temperature coincides with the onset of super-activation. We show that, for this system, the shape of cubic spectra is only weakly affected by dipolar cross-correlations. The good agreement with experimental observations, despite the difference in temperature range, demonstrates the relevance of this approach to help get an insight into the intricate effects probed by non-linear dielectric spectroscopy.
arXiv comment8 pages including appendix, 9 figures including appendix
References in corpus (27)
- Theoretical perspective on the glass transition and amorphous materials
- String-like Clusters and Cooperative Motion in a Model Glass-Forming Liquid
- Direct observation of molecular cooperativity near the glass transition
- Uncorrelated Modes of the Nonlinear Power Spectrum
- Spatial correlations in the dynamics of glassforming liquids: Experimental determination of their temperature dependence
- Spontaneous and induced dynamic fluctuations in glass-formers I: General results and dependence on ensemble and dynamics
- Dynamic heterogeneity in amorphous materials
- Fifth-order susceptibility unveils growth of thermodynamic amorphous order in glass-formers
- Spontaneous and induced dynamic correlations in glass-formers II: Model calculations and comparison to numerical simulations
- Non-linear susceptibility in glassy systems: a probe for cooperative dynamical length scales
- Cooperativity and the freezing of molecular motion at the glass transition
- Evidence of growing spatial correlations at the glass transition from nonlinear response experiments
- Thirty milliseconds in the life of a supercooled liquid
- Does a growing static length scale control the glass transition?
- Intermolecular Cross-Correlations in the Dielectric Response of Glycerol
- Nonlinear response theory for Markov processes: Simple models for glassy relaxation
- Can the glass transition be explained without a growing static length scale?
- Dynamic Correlation Length Scales under Isochronal Conditions
- Investigation of nonlinear effects in glassy matter using dielectric methods
- Higher-order correlation functions and nonlinear response functions in a Gaussian trap model
- On the breakdown of the simple Arrhenius law in the normal liquid state
- Unifying different interpretations of the nonlinear response in glass-forming liquids
- Revisiting the Concept of Activation in Supercooled Liquids
- Glassy Dynamics from First-Principles Simulations
- Modeling non-linear dielectric susceptibilities of supercooled molecular liquids
- Nonlinear response theory for Markov processes III: Stochastic models for dipole reorientations
- Nonlinear dielectric response in glasses: restoring forces and avoided spin-glass criticality