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ABSTRACT: The high energy X-ray reflectivity technique has been applied to study the interfacial structure of protein adsorbates and protein adsorption kinetics in situ. For this purpose, the adsorption of lysozyme at the hydrophilic silica-water interface has been chosen as a model system. The structure of adsorbed lysozyme layers was probed for various aqueous solution conditions. The effect of solution pH and lysozyme concentration on the interfacial structure was measured. Monolayer formation was observed for all cases except for the highest concentration. The adsorbed protein layers consist of adsorbed lysozyme molecules with side-on or end-on orientation. By means of time-dependent X-ray reflectivity scans, the time-evolution of adsorbed proteins was monitored as well. The results of this study demonstrate the capabilities of in situ X-ray reflectivity experiments on protein adsorbates. The great advantages of this method are the broad wave vector range available and the high time resolution.
Langmuir 10/2008; 24(18):10216-21. · 4.19 Impact Factor
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Osama Shekhah,
Hui Wang,
Stefan Kowarik,
Frank Schreiber,
Michael Paulus, Metin Tolan,
Christian Sternemann,
Florian Evers,
Denise Zacher,
Roland A Fischer,
Christof Wöll
Journal of the American Chemical Society 01/2008; 129(49):15118-9. · 9.91 Impact Factor
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ABSTRACT: Experimentally derived static structure factors obtained for the aggregation-prone protein insulin were analyzed with a statistical mechanical model based on the Derjaguin-Landau-Verwey-Overbeek potential. The data reveal that the protein self-assembles into equilibrium clusters already at low concentrations. Furthermore, striking differences regarding interaction forces between aggregation-prone proteins such as insulin in the preaggregated regime and natively stable globular proteins are found.
Physical Review Letters 08/2007; 99(2):028101. · 7.37 Impact Factor
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ABSTRACT: The multi-purpose experimental endstation of beamline BL9 at the Dortmund Electron Accelerator (DELTA) is dedicated to diffraction experiments in grazing-incidence geometry, reflectivity and powder diffraction measurements. Moreover, fluorescence analysis and inelastic X-ray scattering experiments can be performed. Recently, a new set-up for small-angle and wide-angle X-ray scattering utilizing detection by means of an image-plate scanner was installed and is described in detail here. First small-angle X-ray scattering experiments on aqueous solutions of lysozyme with different cosolvents and of staphylococcal nuclease are discussed. The application of the set-up for texture analysis is emphasized and a study of the crystallographic texture of natural bio-nanocomposites, using lobster and crab cuticles as model materials, is presented.
Journal of Synchrotron Radiation 06/2007; 14(Pt 3):244-51. · 2.73 Impact Factor
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ABSTRACT: The effects of various kosmotropic and chaotropic cosolvents and salts on the intermolecular interaction potential of positively charged lysozyme is evaluated at varying protein concentrations by using synchrotron small-angle X-ray scattering in combination with liquid-state theoretical approaches. The experimentally derived static structure factors S(Q) obtained without and with added cosolvents and salts are analysed with a statistical mechanical model based on the Derjaguin-Landau-Verwey-Overbeek (DLVO) potential, which accounts for repulsive and attractive interactions between the protein molecules. Different cosolvents and salts influence the interactions between protein molecules differently as a result of changes in the hydration level or solvation, in charge screening, specific adsorption of the additives at the protein surface, or increased hydrophobic interactions. Intermolecular interaction effects are significant above protein concentrations of 1 wt %, and with increasing protein concentration, the repulsive nature of the intermolecular pair potential V(r) increases markedly. Kosmotropic cosolvents like glycerol and sucrose exhibit strong concentration-dependent effects on the interaction potential, leading to an increase of repulsive forces between the protein molecules at low to medium high osmolyte concentrations. Addition of trifluoroethanol exhibits a multiphasic effect on V(r) when changing its concentration. Salts like sodium chloride and potassium sulfate exhibit strong concentration-dependent changes of the interaction potential due to charge screening of the positively charged protein molecules. Guanidinium chloride (GdmCl) at low concentrations exhibits a similar charge-screening effect, resulting in increased attractive interactions between the protein molecules. At higher GdmCl concentrations, V(r) becomes more repulsive in nature due to the presence of high concentrations of Gdm(+) ions binding to the protein molecules. Our findings also imply that in calculations of thermodynamic properties of proteins in solution and cosolvent mixtures, activity coefficients may not generally be neglected in the concentration range above 1 wt % protein.
ChemPhysChem 05/2007; 8(5):679-89. · 3.41 Impact Factor
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ABSTRACT: Measurements of Langmuir pressure/area isotherms, rheology, grazing incidence X-ray diffraction (GIXD), and grazing incidence diffuse X-ray scattering out of the specular plane (GIXOS) have been used to investigate the influence of a hydrosol containing charged mineral nanoparticles on the thermodynamic and structural properties of a DPPC monolayer. The mineral adsorption layer that is formed via electrostatic interaction underneath the lipid layer alters the thermodynamic properties of the phospholipid monolayer in terms of maximal achievable compression, compressibility, and phase behavior. Modifications appear in the latter case as a coolinglike effect. Rheology measurements of the bulk viscoelastic properties revealed a stabilizing effect of the transient bulk network on the surfactant layer. The lipid chain lattice is found to be reorganized and adapted to the internal atomic structure of the mineral particles. A model for the superposition of Bragg rods from the lipid chains and the minerals is applied to separate these scattering contributions. In the vicinity of the mineral particles, the (2) reflection for DPPC on a liquid substrate was found, indicating strongly suppressed fluctuations at the surface. An estimation of the Debye-Waller factor associated with the lipid layer organization is used to quantify the damping of fluctuations within the lipid matrix due to the rigidifying and stabilizing effect of the mineral particles.
Langmuir 09/2005; 21(16):7349-57. · 4.19 Impact Factor
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ABSTRACT: A new internet-based synchrotron experiment for students is presented. A polarimeter and computer software have been developed for measuring via the internet the X-ray magnetic circular dichroism of PtFe around its Pt L(II) and L(III) absorption edges. From the experiment, students can examine the X-ray magnetic circular dichroism of a thin PtFe foil utilizing circular-polarized synchrotron radiation emitted by the superconducting asymmetric wiggler at the synchrotron radiation source DELTA of the University of Dortmund.
Journal of Synchrotron Radiation 04/2005; 12(Pt 2):246-50. · 2.73 Impact Factor
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ABSTRACT: A dedicated setup comprising an efficient cryogenic device for the in situ preparation of large surface areas of prototypical organic glass formers in a wide temperature range (170–340 K) is presented. This setup provides the necessary temperature and vibrational stability for surface x-ray and neutron scattering experiments, including the extremely sensitive technique of x-ray photon correlation spectroscopy (XPCS). XPCS is an emerging method which is made possible by the high coherent photon flux produced by third-generation synchrotrons. We demonstrate that microscopic motion at the surface can be studied in a direct way in the liquid and supercooled state using XPCS. In addition, we have used a charge-coupled-device detector to record two-dimensional images of static speckle patterns forming on surfaces in the glassy state. © 2003 American Institute of Physics.
Review of Scientific Instruments 08/2003; 74(9):4033-4040. · 1.37 Impact Factor
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ABSTRACT: Capillary wave dynamics on glycerol surfaces has been investigated by means of x-ray photon correlation spectroscopy performed at grazing angles. The measurements show that thermally activated capillary wave motion is slowed down exponentially when the sample is cooled below 273 K. This finding directly reflects the freezing of the surface waves. The wave-number dependence of the measured time constants is in quantitative agreement with theoretical predictions for overdamped capillary waves.
Phys. Rev. B. 01/2001; 63(7).
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ABSTRACT: A kinematical scattering theory for the interpretation of X-ray photon correlation spectroscopy (XPCS) measurements from fluctuating surfaces is discussed in detail. First a general formulation without approximations is given. Then as an example XPCS measurements of capillary wave dynamics on glycerol surfaces will be presented and compared to the calculations applying the usual approximations. It turns out that these approximations work well if the perpendicular wave-vector transfer is small. The measurements confirm on micrometer length scales the prediction from classical hydrodynamics that all waves are overdamped due to the high viscosity of glycerol. In addition, the measurements show that thermally activated capillary wave motion is slowed down exponentially when the sample is cooled below 273 K. Further, the extension of XPCS measurements down to nanometer scales is discussed.
Applied Surface Science.
