Carbon Nitride : Characterization and Protein Interactions

Abstract: This thesis concerns synthesis and characterization of carbon-based materials and theinvestigation of the possible use, of a selection of these materials, in biomedicalapplications. Protein adsorption and blood plasma tests were used for this purposeutilizing a surface sensitive technique called spectroscopic ellipsometry.The materials were synthesized by physical vapor deposition and characterizedregarding microstructure, mechanical properties and optical properties. The ternaries BC-N and Si-C-N as well as carbon and carbon nitrides (CNx) of different microstructureshave been examined. In the B-C-N work, the intention was to investigate the possibilityto combine the two materials CNx and BN, interesting on their own regarding highhardness and extreme elasticity, to produce a material with even better properties.Theoretical calculations were performed to elucidate the different element substitutionsand defect arrangements in the basal planes promoting curvature in the fullerene-likemicrostructure. The Si-C-N ternary was investigated with the consideration of finding away to control the surface energy for certain applications. Amorphous carbon and threemicrostructures of CNx were analyzed by spectroscopic ellipsometry in the UV-VIS-NIRand IR spectral ranges in order to get further insight into the bonding structure of thematerial.In the second part of this work focus was held on studies of macromolecularinteractions on silicon, carbon and CNx film surfaces using ellipsometry. One purposewas to find relevance (or not) for these materials in biological environments. Materials for bone replacement used today, e.g. stainless steel, cobalt-chromium alloys andtitanium alloys suffer from corrosion in body fluids, generation of wear particles inarticulating systems, infections and blood coagulation and cellular damage leading toimpaired functionality and ultimately to implant failure. Artificial heart valves made ofpyrolytic carbon are used today, with friction and wear problems. Thus, there is still aneed to improve biomaterials. The aim of the fourth paper was to investigate theinteraction between carbon-based materials and proteins. Therefore, amorphous carbon(a-C), amorphous (a), graphitic (g) and fullerene-like (FL) CNx thin films were exposedto human serum albumin and blood plasma and the amount of protein was measured insitu using spectroscopic ellipsometry. Surface located and accessible proteins after blood plasma incubations were eventually identified through incubations in antibody solutions.Antibody exposures gave indications of surface response to blood coagulation,complement activation and clotting. The a-C and FL-CNx films might according to theresults have a future in soft tissue applications due to the low immuno-activity, whereasthe g-CNx film possibly might be a candidate for bone replacement applications."Layered" structures of fibrinogen, a fibrous but soft protein involved in manyprocesses in our body, were grown in situ and dynamically monitored by ellipsometry inorder to understand the adsorption process and molecule arrangement onto a siliconsurface.In the last paper of this thesis, the effects of ion concentration and proteinconcentration on the refractive index of water-based solutions used in in situ ellipsometrymeasurements were demonstrated and spectral refractive index data for water solutionswith different ionic strengths and protein concentrations have been provided.