Wojnarowska Zaneta, Dulski Mateusz, Shen Jie, Ruta Beatrice, Rosenthal Martin, Paluch Marian
Institute of Physics, the University of Silesia in Katowice, 75 Pułku Piechoty 1A, 41-500 Chorzów, Poland.
Institute of Material Sciences, the University of Silesia in Katowice, 75 Pułku Piechoty 1A, 41-500 Chorzów, Poland.
J Phys Chem B. 2025 Jun 5;129(22):5601-5606. doi: 10.1021/acs.jpcb.5c00410. Epub 2025 May 22.
Condensed matter physics has long struggled to obtain a comprehensive picture of the liquid-glass transition. Consequently, over the years, universal manifestations of glassy and supercooled dynamics have been established, including a correlation between the static dielectric constant (Δε) and relaxation stretching (β), as well as β and Kirkwood correlation factor (), or deviation degree from Arrhenius behavior of structural relaxation times quantified by dynamic fragility (). Herein, we report a simple, highly polar liquid that breaks all of these rules established for glass-forming liquids. We show that the fluorine-assisted self-assembly, confirmed by temperature-dependent Raman and XRD measurements, brings peculiarities in relaxation dynamics, that is, extremely low dielectric strength, Debye-like shape of dielectric permittivity spectra, much below unity, and enormous acceleration of structural relaxation times and viscosity at = + 20 K. All these peculiarities reveal a strong effect of molecular self-assembly on the dynamics of glass-forming systems.
长期以来，凝聚态物理一直在努力获取有关液 - 玻璃转变的全面图景。因此，多年来已经确立了玻璃态和过冷动力学的普遍表现，包括静态介电常数（Δε）与弛豫拉伸（β）之间的相关性，以及β与柯克伍德相关因子（）之间的相关性，或者由动态脆性（）量化的结构弛豫时间偏离阿仑尼乌斯行为的程度。在此，我们报告了一种简单的、高度极性的液体，它打破了所有为玻璃形成液体所确立的这些规则。我们表明，通过温度相关的拉曼和XRD测量证实的氟辅助自组装，在弛豫动力学中带来了特殊性，即极低的介电强度、介电常数谱的德拜型形状、远低于1以及在 = + 20 K时结构弛豫时间和粘度的极大加速。所有这些特殊性都揭示了分子自组装对玻璃形成系统动力学的强烈影响。
