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3. Evidence of a liquid–liquid transition in a glass-forming ionic liquid

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   Harris, Matthew A.; Kinsey, Thomas; Wagle, Durgesh V.; Baker, Gary A.; Sangoro, Joshua (March 2021, Proceedings of the National Academy of Sciences)

   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. 

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4. Liquid–liquid phase separation in artificial cells

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5. Liquid–liquid transition kinetics in D-mannitol

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   Cao, Chengrong; Tang, Wei; Perepezko, John H. (August 2022, The Journal of Chemical Physics)

   The kinetics of the first order liquid–liquid transition (LLT) in a single-component liquid D-mannitol have been examined in detail by the high rate of flash differential scanning calorimetry measurements. By controlling the annealing temperature, the phase X formation from the supercooled liquid is distinguished by either a nucleation-growth or a spinodal-decomposition type of LLT. In the measured time–temperature-transformation curve the portion covering the nucleation-growth type of LLT can be well fitted with a classical nucleation theory analysis. 

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