Cheng Shiwang, Sokolov Alexei P
Department of Chemical Engineering and Materials Science, Michigan State University, East Lansing, Michigan 48824, USA.
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
J Chem Phys. 2020 Mar 7;152(9):094904. doi: 10.1063/1.5143360.
We study experimentally the temperature evolution of the thickness of the interfacial layer, L(T), between bulk matrices and the surface of nanoparticles in nanocomposites through broadband dielectric spectroscopy. Analyses revealed a power-law dependence between the logarithm of structural relaxation time in the interfacial layer, τ(T), and the L(T): lnτ(T)/τ∝L (T)/T, with τ ∼ 10 s, and β index ∼0.67 at high temperatures and ∼1.7 at temperatures close to the glass transition temperature. In addition, our analysis revealed that the L(T) is comparable to the length scale of dynamic heterogeneity estimated from previous nonlinear dielectric measurements and the four-point NMR [ξ(T)], with L(T) ∼ ξ(T). These observations may suggest a direct correlation between the L(T) and the size of the cooperatively rearranging regions and have strong implications for understanding the dynamic heterogeneity and cooperativity in supercool liquids and their role in interfacial dynamics.
我们通过宽带介电谱实验研究了纳米复合材料中本体基质与纳米颗粒表面之间界面层厚度L(T)的温度演变。分析揭示了界面层中结构弛豫时间τ(T)的对数与L(T)之间的幂律依赖关系:lnτ(T)/τ∝L (T)/T,其中τ ∼ 10 s,在高温下β指数约为0.67,在接近玻璃化转变温度时约为1.7。此外,我们的分析表明,L(T)与先前非线性介电测量和四点核磁共振[ξ(T)]估计的动态非均匀性长度尺度相当,即L(T) ∼ ξ(T)。这些观察结果可能表明L(T)与协同重排区域的大小之间存在直接关联,并且对于理解过冷液体中的动态非均匀性和协同性及其在界面动力学中的作用具有重要意义。