Glassy Dynamics in a Molecular Liquid
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arXiv
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| Format: | Preprint |
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2024
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| author | Kumar, Shubham Sarkar, Sarmistha Bagchi, Biman |
| author_facet | Kumar, Shubham Sarkar, Sarmistha Bagchi, Biman |
| contents | A universal dynamical crossover temperature, Tcr, in glassy liquids, associated with the α-\b{eta} bifurcation temperature, TB, has been observed in dielectric spectroscopy and other experiments. Tcr lies significantly above the glass transition temperature. Here, we introduce a new class of glass-forming liquids, binary mixtures of prolate and oblate ellipsoids. This model system exhibits sharp thermodynamic and dynamic anomalies, such as the specific heat jump during heating and a sharp variation in the thermal expansion coefficient around a temperature identified as the glass transition temperature, Tg. The same temperature is obtained from the fit of the calculated relaxation times to the Vogel-Fulcher-Tammann (VFT) form. As the temperature is lowered, the single peak rotational relaxation spectrum splits into two at a temperature TB significantly above the estimated Tg. Similar bifurcation is also observed in the distribution of short-to-intermediate time translational diffusion. Interrogation of the two peaks reveals a lower extent of dynamic heterogeneity in the population of the faster mode. We observe an unexpected appearance of a sharp peak in the product of rotational relaxation time τ2 and diffusion constant D at a temperature Tcr, close to TB, but above the glass transition temperature. Additionally, we coarse-grain the system into cubic boxes, each containing, on average, ~62 particles, to study the average dynamical properties. Clear evidence of large-scale sudden changes in the diffusion coefficient and rotational correlation time signals first-order transitions between low and high-mobility domains. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2403_19141 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Glassy Dynamics in a Molecular Liquid Kumar, Shubham Sarkar, Sarmistha Bagchi, Biman Soft Condensed Matter A universal dynamical crossover temperature, Tcr, in glassy liquids, associated with the α-\b{eta} bifurcation temperature, TB, has been observed in dielectric spectroscopy and other experiments. Tcr lies significantly above the glass transition temperature. Here, we introduce a new class of glass-forming liquids, binary mixtures of prolate and oblate ellipsoids. This model system exhibits sharp thermodynamic and dynamic anomalies, such as the specific heat jump during heating and a sharp variation in the thermal expansion coefficient around a temperature identified as the glass transition temperature, Tg. The same temperature is obtained from the fit of the calculated relaxation times to the Vogel-Fulcher-Tammann (VFT) form. As the temperature is lowered, the single peak rotational relaxation spectrum splits into two at a temperature TB significantly above the estimated Tg. Similar bifurcation is also observed in the distribution of short-to-intermediate time translational diffusion. Interrogation of the two peaks reveals a lower extent of dynamic heterogeneity in the population of the faster mode. We observe an unexpected appearance of a sharp peak in the product of rotational relaxation time τ2 and diffusion constant D at a temperature Tcr, close to TB, but above the glass transition temperature. Additionally, we coarse-grain the system into cubic boxes, each containing, on average, ~62 particles, to study the average dynamical properties. Clear evidence of large-scale sudden changes in the diffusion coefficient and rotational correlation time signals first-order transitions between low and high-mobility domains. |
| title | Glassy Dynamics in a Molecular Liquid |
| topic | Soft Condensed Matter |
| url | https://arxiv.org/abs/2403.19141 |