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The structure-properties relationship of rhamnolipids, RLs, well knownmicrobial bioamphiphiles (biosurfactants), is exlored in detail by couplingcryogenic transmission electron microscopy (cryo-TEM) and both ex situ and insitu small angle X-ray scattering (SAXS). The self-assembly of three RLs withreasoned variation of their molecular structure (RhaC10, RhaC10C10 andRhaRhaC10C10) and a rhamnose-free C10C10 fatty acid is studied in water as afunction of pH. It is found that RhaC10 and RhaRhaC10C10 form micelles in abroad pH range and RhaC10C10 undergoes a micelle-to-vesicle transition frombasic to acid pH occurring at pH 6.5. Modelling coupled to fitting SAXS dataallows a good estimation of the hydrophobic core radius (or length), thehydrophilic shell thickness, the aggregation number and the surface area perRL. The essentially micellar morphology found for RhaC10 and

Self-Assembly of Rhamnolipids Bioamphiphiles: Understanding Structure-Properties Relationship using Small-Angle X-Ray Scattering