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Carbon Nitride: Characterization and Protein Interactions
Linköping University, Department of Physics, Chemistry and Biology, Applied Optics . Linköping University, The Institute of Technology.
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

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.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press , 2009. , 67 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1263
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:liu:diva-19710ISBN: 978-91-7393-593-7 (print)OAI: oai:DiVA.org:liu-19710DiVA: diva2:227672
Public defence
2009-08-28, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2009-07-16 Created: 2009-07-16 Last updated: 2016-08-31Bibliographically approved
List of papers
1. Microstructure, mechanical properties, and wetting behaviorof Si-C-N thin films grown by reactive magnetron sputtering
Open this publication in new window or tab >>Microstructure, mechanical properties, and wetting behaviorof Si-C-N thin films grown by reactive magnetron sputtering
2001 (English)In: Surface and Coatings Technology, ISSN 0257-8972, Vol. 141, no 2-3, 145-155 p.Article in journal (Refereed) Published
Abstract [en]

Silicon–carbon–nitride (Si–C–N) thin films were deposited by reactive magnetron co-sputtering of C and Si targets in a mixed Ar/N2 discharge. Films were grown to a thickness of more than 0.5 μm on graphite and Si(001) substrates held at a negative floating potential of −35 V, and substrate temperature between 100 and 700°C. The total pressure was constant at 0.4 Pa (3 mtorr), and the nitrogen fraction in the gas mixture was varied between 0 and 100%. As-deposited films were analyzed with respect to composition, state of chemical bonding, microstructure, mechanical properties, and wetting behavior by Rutherford backscattering spectroscopy (RBS), energy dispersive spectroscopy (EDS), X-ray photoelectron spectrometry (XPS), transmission electron microscopy (TEM), scanning electron microscopy (SEM), nanoindentation and contact angle measurements, respectively. Depending on the deposition condition, ternary SixCyNz films within the composition range 1≤x≤34 at.%, 34≤y≤81 at.%, and 16.5≤z≤42 at.% were prepared with a textured, amorphous-to-graphite-like microstructure. For Si–C–N films with low Si content, C---C, C---N and Si---C bonds were present. At higher Si content, N preferentially bonds to Si, while less C---N bonds were observed. Films containing more than 12 at.% of Si contained widely dispersed crystallites, 2–20 nm in diameter. Incorporation of a few at.% Si resulted in a dramatic reduction of the film surface energy compared to pure CN films. The measured contact angles using distilled water and glycerol liquids were for some films comparable with those on a polytetrafluoroethylene (PTFE), Teflon® surface. The hardness of Si–C–N films could be varied over the range 9–28 GPa.

Place, publisher, year, edition, pages
Elsevier, 2001
Keyword
Silicon-carbon-nitride thin films; Magnetron sputtering; Properties
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-19703 (URN)10.1016/S0257-8972(01)01236-1 (DOI)
Available from: 2009-07-16 Created: 2009-07-16 Last updated: 2016-08-31Bibliographically approved
2. Fullerene-like B C N thin films a computational andexperimental study
Open this publication in new window or tab >>Fullerene-like B C N thin films a computational andexperimental study
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2004 (English)In: Materials Science and Engineering B, Vol. 113, no 3, 242-247 p.Article in journal (Refereed) Published
Abstract [en]

Ab initio calculations show that the energy cost for incorporating lattice defects such as pentagons and heptagons is significantly reduced for BCN compared to BN, thus promoting bending of basal planes in these compounds. Boron–carbon–nitride (Bsingle bondCsingle bondN) thin films with a fullerene-like (FL) microstructure were then deposited by dual cathode magnetron sputtering from C and B4C targets. Up to 1 μm thick films were grown at a total gas pressure of 3 mTorr (0.4 Pa) in varying Ar/N2 ratios, and substrate temperatures between 225 and 350 °C. Compositional and microstructural studies were performed using RBS, SEM and HREM, respectively. Depending on the deposition condition, ternary BxCyNz films with fullerene-like microstructure could be prepared in agreement with the calculations within the composition range 0 ≤ x ≤ 53, 15 ≤ y ≤ 62, and 24 ≤ z ≤ 50 at.%. Fullerene-like structures also tend to form at lower temperatures in the case of BCN compared to CN. Nanoindentation measurements show that all BxCyNz films exhibited a highly elastic response independent of elemental composition. In addition, the calculations suggest a driving force for C and BN phase separation.

Place, publisher, year, edition, pages
Elsevier, 2004
Keyword
Ab initio calculations; Fullerene-like materials; BCN compounds; Thin films Reactive magnetron sputtering
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-19704 (URN)10.1016/j.mseb.2004.08.013 (DOI)
Available from: 2009-07-16 Created: 2009-07-16 Last updated: 2016-08-31Bibliographically approved
3. Spectroscopic ellipsometry characterization of amorphous carbon and amorphous,graphitic and fullerene-like carbon nitride thin films
Open this publication in new window or tab >>Spectroscopic ellipsometry characterization of amorphous carbon and amorphous,graphitic and fullerene-like carbon nitride thin films
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2009 (English)In: Thin Solid Films, ISSN 0040-6090, Vol. 517, no 24, 6652-6658 p.Article in journal (Refereed) Published
Abstract [en]

Carbon nitride (CNx) and amorphous carbon (a-C) thin films are deposited by reactive magnetron sputtering onto silicon (001) wafers under controlled conditions to achieve amorphous, graphitic and fullerene-like microstructures. As-deposited films are analyzed by Spectroscopic Ellipsometry in the UV–VIS–NIR and IR spectral ranges in order to get further insight into the bonding structure of the material. Additional characterization is performed by High Resolution Transmission Electron Microscopy, X-ray Photoelectron Spectroscopy, and Atomic Force Microscopy. Between eight and eleven resonances are observed and modeled in the ellipsometrically determined optical spectra of the films. The largest or the second largest resonance for all films is a feature associated with C–N or C–C modes. This feature is generally associated with sp3 C–N or sp3 C–C bonds, which for the nitrogen-containing films instead should be identified as a three-fold or two-fold sp2 hybridization of N, either substituted in a graphite site or in a pyridine-like configuration, respectively. The π→πlow asterisk electronic transition associated with sp2 C bonds in carbon films and with sp2 N bonds (as N bonded in pyridine-like manner) in CNx films is also present, but not as strong. Another feature present in all CNx films is a resonance associated with nitrile often observed in carbon nitrides. Additional resonances are identified and discussed and moreover, several new, unidentified resonances are observed in the ellipsometric spectra.

Place, publisher, year, edition, pages
Elsevier, 2009
Keyword
Carbon nitride; Amorphous carbon; Spectroscopic ellipsometry; Spectral decomposition; Fullerene-like; Structural properties; X-ray photoelectron spectroscopy; Transmission electron microscopy
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-19705 (URN)10.1016/j.tsf.2009.04.065 (DOI)
Note
Original Publication: Torun Berlind, Andrej Furland, Zs. Czigany, Jörg Neidhardt, Lars Hultman and Hans Arwin, Spectroscopic ellipsometry characterization of amorphous carbon and amorphous,graphitic and fullerene-like carbon nitride thin films, 2009, Thin Solid Films, (517), 24, 6652-6658. http://dx.doi.org/10.1016/j.tsf.2009.04.065 Copyright: Elsevier Science B.V., Amsterdam. http://www.elsevier.com/ Available from: 2009-07-16 Created: 2009-07-16 Last updated: 2016-08-31Bibliographically approved
4. Protein adsorption on thin films of carbon and carbon nitride monitored with in situ ellipsometry
Open this publication in new window or tab >>Protein adsorption on thin films of carbon and carbon nitride monitored with in situ ellipsometry
2011 (English)In: ACTA BIOMATERIALIA, ISSN 1742-7061, Vol. 7, no 3, 1369-1378 p.Article in journal (Refereed) Published
Abstract [en]

Amorphous carbon and amorphous, graphitic and fullerene-like carbon nitride thin filmswere deposited by reactive magnetron sputtering and optically characterized withspectroscopic ellipsometry. The films were exposed to human serum albumin and theadsorption was monitored in situ using dynamic ellipsometry. From the ellipsometric data theadsorbed amount of proteins was quantified in terms of surface mass density using de Feijter'smodel. The results indicated larger adsorption of proteins onto the amorphous films comparedto the films with a more ordered microstructure. Complementary studies with labeled HSAusing radioimmunoassay showed up to 6 times higher protein adsorption compared to theellipsometry measurement which partly might be explained by differences in surfaceroughness (from 0.3 to 13 nm) among the films. The elutability of adsorbed labeled HSAusing unlabeled HSA and sodium dodecyl sulphate was low compared to a silicon reference.In addition, the four types of films were incubated in blood plasma followed by antifibrinogen,anti-HMWK or anti-C3c revealing the materials response to complement andcontact activation. Three of the films indicated immunoactivity, whereas the amorphouscarbon showed less immunoactivity compared to a titanium reference. All films showedindications of a stronger ability to initiate the intrinsic pathway of coagulation, compared tothe reference. Finally, the surfaces bone bonding ability was investigated by examination oftheir ability to form calcium phosphate (CaP) crystals in a simulated body fluid, with a-CNxdepositing most CaP after 21 days of incubation.

Place, publisher, year, edition, pages
Elsevier Science B.V. Amsterdam, 2011
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-19706 (URN)10.1016/j.actbio.2010.10.024 (DOI)000287643900049 ()
Note
Original Publication: Torun Berlind, Pentti Tengvall, Lars Hultman and Hans Arwin, Protein adsorption on thin films of carbon and carbon nitride monitored with in situ ellipsometry, 2011, ACTA BIOMATERIALIA, (7), 3, 1369-1378. http://dx.doi.org/10.1016/j.actbio.2010.10.024 Copyright: Elsevier Science B.V. Amsterdam http://www.elsevier.com/ Available from: 2009-07-16 Created: 2009-07-16 Last updated: 2016-08-31Bibliographically approved
5. Formation and cross-linking of fibrinogen layers monitored with in situ spectroscopic ellipsometry
Open this publication in new window or tab >>Formation and cross-linking of fibrinogen layers monitored with in situ spectroscopic ellipsometry
2010 (English)In: Colloids and Surfaces B: Biointerfaces, ISSN 0927-7765, E-ISSN 1873-4367, Vol. 75, no 2, 410-417 p.Article in journal (Other academic) Published
Abstract [en]

Thick matrices of fibrinogen with incorporation of a matrix metalloproteinaseinhibitor were covalently bonded on functionalized silicon surfaces using an ethyl-3-dimethyl-aminopropyl-carbodiimide and N-hydroxy-succinimide affinity ligand couplingchemistry. The growth of the structure was followed in situ using dynamic ellipsometryand characterized at steady-state with spectroscopic ellipsometry. The growth wascompared with earlier work on ex situ growth of fibrinogen layers studied by singlewavelength ellipsometry. It is found that in situ growth and ex situ growth yield differentstructural properties of the formed protein matrix. Fibrinogen matrices with thicknessesup to 58 nm and surface mass densities of 1.6 μg/cm2 have been produced.

Keyword
Fibrinogen, ellipsometry, coupling chemistry, protein adsorption
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-19707 (URN)10.1016/j.colsurfb.2009.09.013 (DOI)000276921900004 ()
Note
Original Publication: Torun Berlind, Michal Poksinski, Pentti Tengvall and Hans Arwin, Formation and cross-linking of fibrinogen layers monitored with in situ spectroscopic ellipsometry, Colloids and Surfaces B: Biointerfaces, 2010, (75), 2, 410-417. http://dx.doi.org/10.1016/j.colsurfb.2009.09.013 Copyright: Elsevier Science B.V., Amsterdam. http://www.elsevier.com/ Available from: 2009-07-16 Created: 2009-07-16 Last updated: 2013-10-14Bibliographically approved
6. Effects of ion concentration on refractive indices offluids measured by the minimum deviation technique
Open this publication in new window or tab >>Effects of ion concentration on refractive indices offluids measured by the minimum deviation technique
Show others...
2008 (English)In: Physica Status Solidi. C, Current topics in solid state physics, ISSN 1610-1634, Vol. 5, no 5, 1249-1252 p.Article in journal (Refereed) Published
Abstract [en]

The prism minimum deviation technique has been used to measure the fluid dependence of refractive indices. Fluids with varying ion concentration (0 to 1.0 M) and varying protein concentration (0.01-10 mg/ml) have been examined and the measurements show that these parameters influence the refractive index values. Also it is shown by simulations that it is important to take the change of refractive index of the fluid into account when evaluating insitu protein adsorption measurements.

Place, publisher, year, edition, pages
Weinheim: WILEY-VCH Verlag GmbH & Co. KGaA, 2008
Keyword
07.60.Fs, 78.20.Ci, 87.14.E-
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-19708 (URN)10.1002/pssc.200777897 (DOI)
Available from: 2009-07-16 Created: 2009-07-16 Last updated: 2013-10-14Bibliographically approved

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