The molecular architecture of sugar-based surfactants
strongly
affects their self-assembled structure, i.e., the type of micelles
they form, which in turn controls both the dynamics and rheological
properties of the system. Here, we report the segmental and mesoscopic
structure and dynamics of a series of C16 maltosides with differences
in the anomeric configuration and degree of tail unsaturation. Neutron
spin-echo measurements showed that the segmental dynamics can be modeled
as a one-dimensional array of segments where the dynamics increase
with inefficient monomer packing. The network dynamics as characterized
by dynamic light scattering show different relaxation modes that can
be associated with the micelle structure. Hindered dynamics are observed
for arrested networks of worm-like micelles, connected to their shear-thinning
rheology, while nonentangled diffusing rods relate to Newtonian rheological
behavior. While the design of novel surfactants with controlled properties
poses a challenge for synthetic chemistry, we demonstrate how simple
variations in the monomer structure can significantly influence the
behavior of surfactants.