Department of Materials Science and Engineering, McMaster University, Hamilton, Ontario L8S 4L7, Canada.
Department of Physics, Umeå University, 901 87 Umeå, Sweden.
J Chem Phys. 2018 Apr 14;148(14):144502. doi: 10.1063/1.5019832.
We report on the temperature, pressure, and time (T, p, and t)-dependent features of thermal conductivity, κ, of partially ordered, non-equilibrium state of C-OG, the orientational glass of Buckminsterfullerene (at T below the orientational freezing temperature T) made more unstable (i) by partially depressurizing its high-p formed state to elastically expand it and (ii) by further pressurizing that state to elastically contract it. The sub-T effects observed on heating of C-OG differ from those of glasses because phonon propagation depends on the ratio of two well-defined orientational states of C molecules and the density of the solid. A broad peak-like feature appears at T near T in the κ-T plots of C-OG formed at 0.7 GPa, depressurized to 0.2 GPa and heated at 0.2 GPa, which we attribute to partial overlap of the sub-T and T features. A sub-T local minimum appears in the κ-T plots at T well below T of C-OG formed at 0.1 GPa, pressurized to 0.5 GPa and heated at 0.5 GPa and it corresponds to the state of maximum disorder. Although Buckminsterfullerene is regarded as an orientationally disordered crystal, variation of its properties with T and p is qualitatively different from other such crystals. We discuss the findings in terms of the nature of its disorder, sensitivity of its rotational dynamics to temperature, and the absence of the Johari-Goldstein relaxation. All seem to affect the phenomenology of its glass-like transition.
我们报告了部分有序、非平衡状态的 C-OG(富勒烯的取向玻璃,在低于取向冻结温度 T 的温度 T 下)的热导率κ随温度、压力和时间(T、p 和 t)的依赖性特征,该状态通过部分降低其高压形成状态的压力使其弹性膨胀(i)和进一步加压使其弹性收缩(ii)使其更加不稳定。在 C-OG 的加热过程中观察到的亚 T 效应与玻璃不同,因为声子传播取决于 C 分子的两个定义明确的取向状态的比例和固体的密度。在在 0.7 GPa 下形成、减压至 0.2 GPa 并在 0.2 GPa 下加热的 C-OG 的 κ-T 图中出现了一个宽的峰状特征,我们将其归因于亚 T 和 T 特征的部分重叠。在在 0.1 GPa 下形成、加压至 0.5 GPa 并在 0.5 GPa 下加热的 C-OG 的 κ-T 图中,在远低于 T 的温度 T 处出现了一个亚 T 局部最小值,它对应于最大无序状态。尽管富勒烯被认为是一种取向无序的晶体,但它的性质随 T 和 p 的变化与其他此类晶体的定性不同。我们根据其无序的性质、其旋转动力学对温度的敏感性以及不存在 Johari-Goldstein 弛豫来讨论这些发现。所有这些似乎都影响了其玻璃转变的现象学。