SPEC (CNRS URA 2464), DSM/IRAMIS CEA Saclay, Bat.772, F-91191 Gif-sur-Yvette, France.
J Chem Phys. 2010 Dec 21;133(23):234901. doi: 10.1063/1.3507252.
We present a detailed study of the heating effects in dielectric measurements carried out on a liquid. Such effects come from the dissipation of the electric power in the liquid and give contribution to the nonlinear third harmonics susceptibility χ(3), which depends on the frequency and temperature. This study is used to evaluate a possible "spurious" contribution to the recently measured nonlinear susceptibility of an archetypical glassforming liquid (glycerol). Those measurements have been shown to give a direct evaluation of the number of dynamically correlated molecules temperature dependence close to the glass transition temperature T(g) ≈ 190 K [Crauste-Thibierge et al., Phys. Rev. Lett. 104, 165703 (2010)]. We show that the heating contribution is totally negligible (i) below 204 K at any frequency; (ii) for any temperature at the frequency where the third harmonics response χ(3) is maximum. Besides, this heating contribution does not scale as a function of f/f(α), with f(α)(T) the relaxation frequency of the liquid. In the high frequency range, when f/f(α) ≥ 1, we find that the heating contribution is damped because the dipoles cannot follow instantaneously the temperature modulation due to the heating phenomenon. An estimate of the magnitude of this damping is given.
我们对液体介电测量中的加热效应进行了详细研究。这些效应来自液体中电功率的耗散,并对非线性三阶极化率 χ(3) 产生贡献,χ(3) 取决于频率和温度。这项研究用于评估最近测量典型玻璃形成液体(甘油)的非线性极化率时可能存在的“虚假”贡献。这些测量被证明可以直接评估在玻璃化转变温度 T(g) ≈ 190 K 附近与温度相关的动态相关分子的数量[Crauste-Thibierge 等人,Phys. Rev. Lett. 104, 165703 (2010)]。我们表明,加热贡献在以下情况下可以忽略不计:(i)在任何频率下低于 204 K;(ii)在三阶谐波响应 χ(3) 最大的任何温度下。此外,这种加热贡献不随 f/f(α) 变化,其中 f(α)(T) 是液体的弛豫频率。在高频范围,当 f/f(α) ≥ 1 时,我们发现加热贡献被阻尼,因为由于加热现象,偶极子不能即时跟随温度调制。给出了这种阻尼的幅度估计。