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DOI | 10.1073/pnas.2020878118 |
Evidence of a liquid-liquid transition in a glass-forming ionic liquid | |
Harris M.A.; Kinsey T.; Wagle D.V.; Baker G.A.; Sangoro J. | |
发表日期 | 2021 |
ISSN | 00278424 |
卷号 | 118期号:11 |
英文摘要 | A liquid-liquid transition (LLT) is a transformation from one liquid to another through a first-order transition. The LLT is fundamental to the understanding of the liquid state and has been reported in a few materials such as silicon, phosphorus, triphenyl phosphite, and water. Furthermore, it has been suggested that the unique properties of materials such as water, which is critical for life on the planet, are linked to the existence of the LLT. However, the experimental evidence for the existence of an LLT in many molecular liquids remains controversial, due to the prevalence and high propensity of the materials to crystallize. Here, we show evidence of an LLT in a glass-forming trihexyltetradecylphosphonium borohydride ionic liquid that shows no tendency to crystallize under normal laboratory conditions. We observe a step-like increase in the static dielectric permittivity at the transition. Furthermore, the sizes of nonpolar local domains and ion-coordination numbers deduced from wide-angle X-ray scattering also change abruptly at the LLT. We independently corroborate these changes in local organization using Raman spectroscopy. The experimental access to the evolution of local order and structural dynamics across a liquid-liquid transition opens up unprecedented possibilities to understand the nature of the liquid state. © 2021 National Academy of Sciences. All rights reserved. |
英文关键词 | Glass transition; Ionic liquids; Liquid-liquid transition; Mesoscale organization |
语种 | 英语 |
来源期刊 | Proceedings of the National Academy of Sciences of the United States of America |
文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/180261 |
作者单位 | Department of Chemical and Biomolecular Engineering, University of Tennessee, Knoxville, TN 37996, United States; Department of Chemistry and Physics, Florida Gulf Coast University, Fort Myers, FL 33965, United States; Department of Chemistry, University of Missouri, Columbia, MO 65211, United States |
推荐引用方式 GB/T 7714 | Harris M.A.,Kinsey T.,Wagle D.V.,et al. Evidence of a liquid-liquid transition in a glass-forming ionic liquid[J],2021,118(11). |
APA | Harris M.A.,Kinsey T.,Wagle D.V.,Baker G.A.,&Sangoro J..(2021).Evidence of a liquid-liquid transition in a glass-forming ionic liquid.Proceedings of the National Academy of Sciences of the United States of America,118(11). |
MLA | Harris M.A.,et al."Evidence of a liquid-liquid transition in a glass-forming ionic liquid".Proceedings of the National Academy of Sciences of the United States of America 118.11(2021). |
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