Nonlinear dielectric response in glass formers: Restoring forces and avoided spin-glass criticality.

Experimental measurements of nonlinear dielectric response in glass formers like supercooled glycerol or propylene carbonate have been interpreted as providing evidence for a growing thermodynamic length scale when lowering temperature. A heuristic picture based on coherently flipping "superdipoles" with disordered internal structure has been argued to capture the essence of the experimentally reported behavior, pointing to the key role of effectively disordered interactions in structural glasses. We test these ideas by devising an explicit one-dimensional model of interacting spins incorporating both the spin-glass spirit of the superdipole argument and the necessary long-time decorrelation of structural disorder, encoded here in a slow dynamics of the coupling constants.

Crossing the Frontier of Validity of the Material Time Approach in the Aging of a Molecular Glass.

We studied the physical aging of glycerol in response to upward temperature steps of amplitude ranging from 0.3 to 18 K. This was done using a specially designed experimental setup allowing quick heating of a liquid film while measuring the evolution of its dielectric properties.

Simultaneously measuring the dichroism and the dielectric response of an azobenzene-doped organic glass former.

We have designed an experimental setup allowing to simultaneously measure both the dielectric response of a supercooled liquid and the dynamics of azobenzene chromophores dispersed in it. Both the azobenzene chromophores and the organic glass former have been synthesized with similar reaction paths: they are chemically similar, apart from the azobenzene group responsible for the strong optical absorption in the [350; 450 nm] range for the chromophores, while the embedding supercooled liquid is optically transparent. This material is deposited on transparent electrodes with an inter-electrode gap as small as 4 µm-obtained thanks to optical lithographic techniques.

Orientational dynamics in supercooled glycerol computed from MD simulations: self and cross contributions.

The orientational dynamics of supercooled glycerol is probed using molecular dynamics simulations for temperatures ranging from 323 K to 253 K, through correlation functions of first and second ranks of Legendre polynomials, pertaining respectively to dielectric spectroscopy (DS) and depolarized dynamic light scattering (DDLS). The self, cross, and total correlation functions are compared with relevant experimental data. The computations reveal the low sensitivity of DDLS to cross-correlations, in agreement with what is found in experimental work, and strengthen the idea of directly comparing DS and DDLS data to evaluate the effect of cross-correlations in polar liquids.

Non-linear physical aging of supercooled glycerol induced by large upward ideal temperature steps monitored through cooling experiments.

The physical aging of supercooled glycerol induced by upward temperature steps of amplitude reaching 45 K was studied by a new method consisting in heating a micrometer-thick liquid film at a rate of up to 60 000 K/s, holding it at a constant high temperature for a controlled duration before letting it quickly cool down to the initial temperature. By monitoring the final slow relaxation of the dielectric loss, we were able to obtain quantitative information on the liquid response to the initial upward step. The so-called TNM (Tool-Narayanaswamy-Moynihan) formalism provided a good description of our observations despite the large distance from equilibrium, provided that different values of the nonlinearity parameter were used for the cooling phase and for the (much further from equilibrium) heating phase.