In particular, this article demonstrates the correlation between molecular changes (Raman Spectroscopy) and microstructural evolution of rheological properties (DLS, DLS-optical microrheology) for the first time for surfactant-based wormlike micellar system. Whereby, Raman Spectroscopy provides information about the molecular structure and DLS-microrheology characterizes viscoelastic properties, the combination of data delivered allows for a deeper understanding of the molecular changes underlying the viscoelastic ones. The study illustrates the utility of the combined DLS, DLS-optical microrheology and Raman Spectroscopy in providing new molecular structural insights into the self-assembly process in complex fluids.

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