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Solvent penetration experiments and small-angle X-ray scattering reveal that phospholipids dissolved in a deep eutectic solvent (DES) spontaneously self-assemble into vesicles above the lipid chain melting temperature. This means DESs are one of the few nonaqueous solvents that mediate amphiphile self-assembly, joining a select set of H-bonding molecular solvents and ionic liquids.

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A deep eutectic solvent is an effective cryoprotective agent for several human cell lines.

Phospholipids are shown by solvent penetration experiments to form lamellar phases and spontaneously spawn vesicles in a wide range of deep eutectic solvents (DESs) composed of alkylammonium halide salts and glycerol or ethylene glycol, which are shown to be nanostructured by X-ray scattering. In contrast with molecular solvents, the chain melting temperature of each phospholipid, which determines the stability of the swellable bilayer phase, depends on the structure of the cation, anion, and molecular H-bond donor that constitute the DES. Chain melting is most sensitive to the length of the alkyl chain of the cation, which is partitioned between apolar domains in the bulk, nanostructured DES and those within the lipid bilayer. This is moderated by the structures of the anion and the molecular hydrogen bond donor, which determine the extent of polar/apolar segregation in the bulk liquid.

Liquid metals (LMs) have emerged as novel materials for biomedical applications. Here, the interactions taking place between cells and LMs are reported, presenting a unique opportunity to explore and understand the LM‐biological interface. Several high‐resolution imaging techniques are used to characterize the interaction between droplets of gallium LM and bacterial, fungal, and mammalian cells. Adhesive interactions between cells and LM droplets are observed, causing deformation of the LM droplet surface, resulting in surface wrinkling and in some cases, breakage of the native oxide layer present on the LM droplet surface. In many instances, the cell wall deforms to intimately contact the LM droplets. Single‐cell force spectroscopy is performed to quantify the adhesion forces between cells and LM and characterize the nature of the adhesion. It is proposed that the flexible nature of the cell enables multiple adhesion sites with the LM droplets, imparting tensile forces on the LM droplet surface, which results in surface wrinkling on the LM droplets due to their liquid nature. Molecular dynamics simulations also suggest that flexible biomolecules on the cell surface can disrupt the Ga2O3 layer formed at the LM droplet surface. This study reveals a unique biointerfacial interaction and provides insights into the mechanisms involved.

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