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We investigated the surface structure of hydrogels ofpoly(N,N-dimethylacrylamide) (PDMA) hydrogels synthesized and cross-linkedsimultaneously by redox free radical polymerization. We demonstrate theexistence of a less cross-linked layer at the surface of the gel at least attwo different length scales characterized by shear rheology and by neutronreflectivity, suggesting the existence of a gradient in cross-linking. Thecomposition of the layer is shown to depend on the degree of hydrophobicity ofthe mold surface and is weaker for more hydrophobic molds. While themacroscopic tests proved the existence of a relatively thick under-cross-linkedlayer, we also demonstrated by neutron reflectivity that the gel surface at thesubmicrometric scale (500 nm) was also affected by the surface treatment of themold. These results should have important implications for the measurement ofmacroscopic surface properties of these hydrogels such as friction or adhesion.

Structure of Surfaces and Interfaces of Poly( N,N -dimethylacrylamide) Hydrogels