Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, USA.
J Chem Phys. 2012 Mar 28;136(12):124512. doi: 10.1063/1.3697841.
Dynamics of water, especially in the temperature range of the "no man's land", remain a mystery. We present detailed study of dynamics in aqueous LiCl solution that is often considered as a model for bulk water. We employ broadband dielectric and light scattering spectroscopy in a broad frequency and temperature range. Our analysis reveals no sign of the fragile-to-strong crossover (FSC) neither in structural relaxation nor in translational motions. Our experimental results combined with a large selection of literature data lead to the clear conclusion-there is no FSC in dynamics of aqueous solutions at T ∼ 200-230 K. Instead, our analysis reveals appearance of the so-called excess wing at the high frequency tail of the structural relaxation peak. We discuss the localized nature of the relaxation process that contributes to the excess wing.
水的动力学,特别是在“无人区”的温度范围内,仍然是一个谜。我们对经常被认为是块状水模型的水溶液中的动力学进行了详细的研究。我们在很宽的频率和温度范围内使用宽带介电和光散射光谱。我们的分析显示,无论是在结构弛豫还是在平移运动中,都没有脆弱到强转变(FSC)的迹象。我们的实验结果结合大量文献数据得出了明确的结论——在 T∼200-230 K 的水溶液动力学中没有 FSC。相反,我们的分析显示出在结构弛豫峰的高频尾部出现所谓的过剩翼。我们讨论了导致过剩翼的弛豫过程的局部性质。