Mechanical Properties and Concentrations of Poly(ethylene glycol) in Hydrogels and Brushes Direct the Surface Transport of Staphylococcus aureus

Surface-associated transport of flowing bacteria, including cell rolling, is a mechanism for otherwise immobile bacteria to migrate on surfaces and could be associated with biofilm formation or the spread of infection. This work demonstrates how the moduli and/or local polymer concentration play critical roles in sustaining contact, dynamic adhesion, and transport of bacterial cells along a hydrogel or hydrated brush surface. In particular, stiffer more concentrated hydrogels and brushes maintained the greatest dynamic contact, still allowing cells to travel along the surface in flow. This study addressed how the mechanical properties, molecular architectures, and thicknesses of minimally adhesive poly(ethylene glycol) (PEG) based coatings influence the flow-driven surface motion of Staphylococcus aureus MS2 cells. Three protein-repellant PEG-dimethylacrylate hydrogel films (similar to 100 mu m thick) and two protein-repellant PEG brushes (8-16 nm thick) were sufficiently fouling-resistant to prevent the accumulation of flowing bacteria. However, the rolling or hopping-like motions of gently flowing S. aureus cells along the surfaces were specific to the particular hydrogel or brush, distinguishing these coatings in terms of their mechanical properties (with moduli from 2 to 1300 kPa) or local PEG concentrations (in the range 10-50% PEG). On the stiffer hydrogel coatings having higher PEG concentrations, S. aureus exhibited long runs of surface rolling, 20-50 mu m in length, an increased tendency of cells to repeatedly return to some surfaces after rolling and escaping, and relatively long integrated contact times. By contrast, on the softer more dilute hydrogels, bacteria tended to encounter the surface for brief periods before escaping without return. The dynamic adhesion and motion signatures of the cells on the two brushes were bracketed by those on the soft and stiff hydrogels, demonstrating that PEG coating thickness was not important in these studies where the vertically oriented surfaces minimized the impact of gravitational forces. Control studies with similarly sized poly(ethylene oxide)-coated rigid spherical microparticles, that also did not arrest on the PEG coatings, established that the bacterial skipping and rolling signatures were specific to the S. aureus cells and not simply diffusive. Dynamic adhesion of the S. aureus cells on the PEG hydrogel surfaces correlated well with quiescent 24 h adhesion studies in the literature, despite the orientation of the flow studies that eliminated the influence of gravity on bacteria-coating normal forces.