Third harmonics nonlinear susceptibility in supercooled liquids: a comparison to the box model.

The box model, originally introduced to account for the nonresonant hole burning (NHB) dielectric experiments in supercooled liquids, is compared to the measurements of the third harmonics P(3) of the polarisation, reported recently in glycerol, close to the glass transition temperature T(g) [C. Crauste-Thibierge, C. Brun, F. Ladieu, D. L'Hôte, G. Biroli, and J.-P. Bouchaud, Phys. Rev. Lett. 104, 165703 (2010)]. In this model, each box is a distinct dynamical relaxing entity (hereafter called dynamical heterogeneity (DH)) which follows a Debye dynamics with its own relaxation time τ(dh). When it is submitted to a strong electric field, the model posits that a temperature increase δT(dh), depending on τ(dh), arises due to the dissipation of the electrical power. Each DH has thus its own temperature increase, on top of the temperature increase of the phonon bath δT(ph). Contrary to the "fast" hole burning experiments where δT(ph) is usually neglected, the P(3) measurements are, from a thermal point of view, fully in a stationary regime, which means that δT(ph) can no longer be neglected a priori. This is why the version of the box model that we study here takes δT(ph) into account, which implies that the δT(dh) of the DHs are all coupled together. The value of P(3), including both the "intrinsic" contribution of each DH as well as the "spurious" one coming from δT(ph), is computed within this box model and compared to the P(3) measurements for glycerol, in the same range of frequencies and temperatures T. Qualitatively, we find that this version of the box model shares with experiments some nontrivial features, e.g., the existence of a peak at finite frequency in the modulus of P(3) as well as its order of magnitude. Quantitatively, however, some experimental features are not accounted for by this model. We show that these differences between the model and the experiments do not come from δT(ph) but from the "intrinsic" contribution of the DHs. Finally, we show that the interferences between the 3ω response of the various DHs are the most important issue leading to the discrepancies between the box model prediction and the experiments. We argue that this could explain why the box model is quite successful to account for some kinds of nonlinear experiments (such as NHB) performed close to T(g), even if it does not completely account for all of them (such as the P(3) measurements). This conclusion is supported by an analytical argument which helps understanding how a "space-free" model as the box model is able to account for some of the experimental nonlinear features.