Supporting Data for Self-Assembly of Unusually Stable Thermotropic Network Phases by Cellobiose-Based Guerbet Glycolipids

These files contain data along with associated output from instrumentation supporting all results reported in the referenced paper. Bicontinuous thermotropic liquid crystal (LC) materials, such as double gyroid (DG) phases, are highly promising for various applications due to their intricate 3D network structures. However, the lack of robust molecular design rules for shape-filling amphiphiles hinders their utility. To address this, we synthesized cellobiose-based glycolipids with Guerbet-type branched alkyl tails and examined their thermotropic LC self-assembly. Through techniques including differential scanning calorimetry (DSC), polarized optical microscopy (POM), and small-angle X-ray scattering (SAXS), we found that Guerbet cellobiosides have a strong propensity to form DG morphology across broad thermotropic phase ranges. The stability of these assemblies depends on the alkyl tail structure and anomeric configuration of the glycolipid in a previously unrecognized manner. Molecular simulations provide further insights, revealing molecular motifs crucial for network phase self-assembly, paving the way for future designs and applications of network LC materials.