Department of Materials Science and Engineering, University of California at Davis, Davis, California 95616, USA.
Science and Technology Division, Corning Incorporated, Corning, New York 14831, USA.
J Chem Phys. 2018 Mar 21;148(11):111101. doi: 10.1063/1.5022787.
The rheological behavior of supercooled Se, AsSe, and AsSe liquids is studied in the linear regime as a function of frequency, extending over nearly 11 orders of magnitude, using oscillatory parallel plate rheometry. While the viscoelastic response of the AsSe liquid is characterized by a single relaxation time scale, the Se and the AsSe liquids display two distinct relaxation processes, both of which are coupled to viscosity, although their time scales differ by nearly 3-5 orders of magnitude. The ultra-slow relaxation process appears to be related to the dynamics of -Se-Se-Se- chain segments in the structure of these liquids, with characteristic time scale and shear modulus that are dependent on the average chain length. The fast mode, on the other hand, is associated with the glassy modulus and is tentatively assigned to a Johari-Goldstein β-process. These results, when taken together, are consistent with the presence of a hierarchical free energy landscape that characterizes the dynamics of the fragile Se and AsSe liquids.
使用振荡平行板流变仪研究了过冷 Se、AsSe 和 AsSe 液体在线性 regime 下作为频率函数的流变行为,其频率范围扩展近 11 个数量级。虽然 AsSe 液体的粘弹性响应具有单个弛豫时间尺度,但 Se 和 AsSe 液体显示出两个不同的弛豫过程,它们都与粘度相关,尽管它们的时间尺度相差近 3-5 个数量级。超慢弛豫过程似乎与这些液体结构中 -Se-Se-Se- 链段的动力学有关,其特征时间尺度和剪切模量取决于平均链长。另一方面,快模态与玻璃化模量有关,暂定为 Johari-Goldstein β 过程。这些结果结合在一起,与存在描述脆弱 Se 和 AsSe 液体动力学的分层自由能景观一致。