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Tuning the Spontaneous Formation of Helical Lipid Nanotubes by Bilayer Compositional Control

par Villanueva, Martin Eduardo;Ruysschaert, Jean Marie ;Waeytens, Jehan ;Bouchet, Ana Maria;Losada Perez, Patricia
Référence Langmuir, 41, 50, page (34119-34129)
Publication Publié, 2025-12-01

Article révisé par les pairs

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Résumé :

Helical lipid nanotubes are self-assembled structures with potential applications in targeted drug encapsulation and as scaffolds for nanoscale materials. Their rational design relies on the interplay among molecular shape, intermolecular forces, and geometrical constraints, and achieving a specific helical geometry requires understanding how these parameters balance to favor the desired structure. In this study, the compositional control of binary mixtures comprising an asymmetric glycolipid called Ohmline (OHM) and common phosphatidylcholines (DOPC or DPPC) is proposed as a facile route to modulate lipid helical nanotube self-assembly. The aim of this work is to elucidate how bilayer composition governs nanotube formation by linking the thermodynamic mixing behavior, molecular interactions, and nanomechanical properties of OHM/PC systems. A combination of thermodynamic, spectroscopic and nanomechanical measurements of OHM/PC mixtures enabled us to uncover the interplay between the favorable interactions in the mixing process and the bilayer nanomechanics involved in tubulation. While both phospholipids mix favorably with the glycolipid, DOPC-containing mixtures are energetically more favorable. DOPC modulates the tilt order of the glycolipid within the bilayer, reducing the thermodynamic driving force for tube closure and leading to the stabilization of ribbon-like structures with a longer helical pitch. Conversely, DPPC increases membrane rigidity, decreases the OHM tilt, and raises the energy barrier associated with the tubulation process. These observations are consistent with theoretical frameworks that emphasize lipid tilt and curvature elasticity as central mechanisms governing tubulation. Our findings not only reveal the structural determinants underlying lipid nanotube formation but also pave the way for the rational design of lipid-based nanotubular platforms with tailored functional properties.