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   https://doi.org/10.1016/j.jnoncrysol.2020.120601  

   Zhu, Weidi; Gulbiten, Ozgur; Aitken, Bruce; Sen, Sabyasachi (February 2021, Journal of Non-Crystalline Solids)

   null (Ed.)
2. Evidence of a liquid–liquid transition in a glass-forming ionic liquid

   https://doi.org/10.1073/pnas.2020878118  

   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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3. Single-Molecular Dissection of Liquid–Liquid Phase Transitions

   https://doi.org/10.1021/jacs.3c03812  

   Pokhrel, Pravin; Jonchhe, Sagun; Pan, Wei; Mao, Hanbin (August 2023, Journal of the American Chemical Society)
4. Low viscosity liquid bridges: Stretching of liquid bridges immersed in a higher viscosity liquid

   https://doi.org/10.1016/j.jciso.2023.100079  

   Lopez, Ramon; Vaswani, Jovina; Butler, Dylan T.; McCarthy, Joseph; Velankar, Sachin S. (April 2023, JCIS Open)
5. Electrochemical Liquid‐Liquid‐Solid Growth of Ag‐In Crystals with Liquid Indium Alloy Electrodes

   https://doi.org/10.1002/celc.202400229  

   Wu, Henry; Hazelnis, Joshua_P; Maldonado, Stephen (June 2024, ChemElectroChem)

   Abstract Synthesis of intermetallic crystals by electrodeposition of Ag from alkaline aqueous electrolytes containing AgCN onto liquid metal electrodes via an electrochemical liquid‐liquid‐solid (ec‐LLS) process has been performed. X‐ray diffraction, scanning electron microscopy, and transmission electron microscopy were performed to identify crystalline products. Ec‐LLS experiments performed with pure liquid Hg and Ga electrodes resulted in the formation of polycrystalline Ag₂Ga and Ag₂Hg₃. Experiments performed with In‐containing liquid metals preferentially yielded Ag₉In₄and AgIn₂products with liquid Hg_0.35In_0.65and Ga_0.86In_0.14, respectively. The product distribution with liquid Hg_0.35In_0.65depended on the level of Ag supersaturation during the electrodeposition. A mechanism that accounts for the aforementioned observations is presented and discussed. This work described the formation of Ag−In intermetallic phases by the isothermal electroreduction of Ag into different liquid metal solvents via ec‐LLS. Electrodeposition of Ag into a pure Ga or pure Hg liquid metal pool yielded precisely the compounds predicted from isothermal cross‐sections of the respective binary phase diagrams. These compounds were not found when using liquid Hg or Ga containing appreciable In. The smaller enthalpy of formation for AgIn₂was consistent with its synthesis in Ga_0.86In_0.14. However, the observed product of Ag₉In₄in Hg‐containing liquid metals could not be rationalized solely from thermodynamic factors. Instead, this observation was consistent with a kinetic pathway based on the lability of Hg‐metal bonds and nearly identical crystal structures of Ag₉In₄and Ag₂Hg₃. Site exchange of Hg for In is consistent with our prior observations^[23]of In exchange into Hg−Pd structures during Pd electrodeposition. This mechanism is not based on any direct role of electrochemistry other than aspects that dictate the operative supersaturation of the metal solute. 

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