Surface gradients of chemistry or morphology represent powerful tools for the high-throughput investigation of interfacial phenomena in the areas of physics, chemistry, materials science and biology. A wide variety of methods for the fabrication of such gradients has been developed in recent years, relying on principles ranging from diffusion to time-dependent irradiation in order to achieve a gradual change of a particular parameter across a surface. In this review we have endeavoured to cover the principal fabrication approaches for surface-chemical and surface-morphological gradients that have been described in the literature, and to provide examples of their applications in a variety of different fields.
Bone degradation by osteoclasts depends on the formation of a sealing zone, composed of an interlinked network of podosomes, which delimits the degradation lacuna into which osteoclasts secrete acid and proteolytic enzymes. For resorption to occur, the sealing zone must be coherent and stable for extended periods of time. Using titanium roughness gradients ranging from 1 to 4.5 mm R a as substrates for osteoclast adhesion, we show that microtopographic obstacles of a length scale well beyond the range of the 'footprint' of an individual podosome can slow down sealing-zone expansion. A clear inverse correlation was found between ring stability, structural integrity and sealing-zone translocation rate. Direct live-cell microscopy indicated that the expansion of the sealing zone is locally arrested by steep, three-dimensional 'ridge-like barriers', running parallel to its perimeter. It was, however, also evident that the sealing zone can bypass such obstacles, if pulled by neighbouring regions, extending through flanking, obstacle-free areas. We propose that sealing-zone dynamics, while being locally regulated by surface roughness, are globally integrated via the associated actin cytoskeleton. The effect of substrate roughness on osteoclast behaviour is significant in relation to osteoclast function under physiological and pathological conditions, and may constitute an important consideration in the design of advanced bone replacements.
A simple dipping process has been used to prepare PEGylated surface gradients from the polycationic polymer poly(l-lysine), grafted with poly(ethylene glycol) (PLL-g-PEG), on metal oxide substrates, such as TiO2 and Nb2O5. PLL-g-PEG coverage gradients were prepared during an initial, controlled immersion and characterized with variable angle spectroscopic ellipsometry and x-ray photoelectron spectroscopy. Gradients with a linear change in thickness and coverage were generated by the use of an immersion program based on an exponential function. These single-component gradients were used to study the adsorption of proteins of different sizes and shapes, namely, albumin, immunoglobulin G, and fibrinogen. The authors have shown that the density and size of defects in the PLL-g-PEG adlayer determine the amount of protein that is adsorbed at a certain adlayer thickness. In a second step, single-component gradients of functionalized PLL-g-PEG were backfilled with nonfunctionalized PLL-g-PEG to generate two-component gradients containing functional groups, such as biotin, in a protein-resistant background. Such gradients were combined with a patterning technique to generate individually addressable spots on a gradient surface. The surfaces generated in this way show promise as a useful and versatile biochemical screening tool and could readily be incorporated into a method for studying the behavior of cells on functionalized surfaces.
Gradient surfaces enable rapid screening and high-throughput investigations in various fields, such as biology and tribology. A new method is described for the preparation of material-independent morphological gradients, in which the density and height of roughness features are varied along two orthogonal axes. A polystyrene-particle-density gradient was produced by a dip-coating process on titanium-oxide-coated silicon wafers. A controlled exposure to ultraviolet light enabled the generation of a particle-height gradient in the orthogonal direction. These gradients were replicated to generate material-independent morphology gradients. MC3T3 cell proliferation studies were performed on titanium-coated replicas and showed a higher cell density on the high-feature-density region of the gradient. The cell area coverage was found to increase with decreasing particle height.
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