0000000000714758
AUTHOR
K. Lowack
Nonlinear hairy layer theory of electrophoretic fingerprinting applied to consecutive layer by layer polyelectrolyte adsorption onto charged polystyrene latex particles
The consecutive layer-by-layer adsorption of poly(allylamine hydrochloride) (PAH) and poly(styrenesulfonate) (PSS) on colloidal charged latex particles is investigated by measuring the electrophoretic mobility as a function of pH and ionic strength over a broad range (electrophoretic fingerprinting). Meaningful interpretation of the data required the development of a nonlinear approach to hairy particle electrophoresis including dissociation, adsorption, and association. Steric and electrostatic exclusion of mobile ions from the hairy layer has been considered. Also, the surface conductivity correction is extended to the case of charged hairy layer particles. We deposited up to three polyel…
Layer-by-layer deposited multilayer assemblies of polyelectrolytes and proteins: from ultrathin films to protein arrays
We have recently introduced a new method of creating ultrathin films of polyelectrolytes based on the electrostatic attraction between opposite charges. Multilayer assemblies are adsorbed in a layer-by-layer fashion from aqueous solutions of the polymers. The total film thickness can easily be adjusted by varying the ionic strength of the solution. Here, we report on the temperature stability and the water content of the multilayer assemblies. Furthermore, we have extended our concept to the incorporation of protein layers into films of synthetic polyelectrolytes. The well established system biotin/streptavidin was used to construct such multilayers, also by biospecific recognition. Adsorpt…
Characterizing the Glassy Phase of a Statistical Copolymer Monolayer
Monolayers of a statistical copolymer with a poly(methacrylate) chain and hydrophilic and hydrophobic side groups are investigated at the air/water interface. The isotherms suggest a fluid and a frozen phase. With in-situ X-ray reflectivity the monolayer thickness is determined to be 2.5 nm or less. The shear viscosity in the fluid phase is extremely high yet can be described in the framework of the free area model. However, the parameter which characterizes the overlap of holes available for a diffusing monomer unit is a factor of 2 higher than expected, suggesting local diffusion barriers formed by nanosized clusters. In the glassy phase single-molecule fluorescence shows anomalous diffus…
Layer-by-Layer Adsorption: The Solid/Liquid-Interface as a Template for the Controlled Growth of Well-Defined Nanostructures of Polyelectrolytes, Proteins, DNA and Polynucleotides
This report describes the construction of ultrathin films whose structure can be tailored on the molecular scale. The resulting supramolecular film architectures may include functional biological macromolecules such as proteins or polynucleotides. The average distances of two functional layers can be adjusted on the nanometer scale (from less than lnm to several tens of nanometers), with a precision of approximately 0.1 nm. This control is achieved by varying the number and the thickness of the polyelectrolyte interlayers and requires the capability of steering each adsorption step with high accuracy. A crucial factor is the fabrication and manipulation of the film surface at each adsorptio…
Molecular Mechanisms Controlling the Self-Assembly Process of Polyelectrolyte Multilayers
The distance dependent interaction between polyelectrolyte-covered mica surfaces in aqueous solution was investigated with the surface forces apparatus. We find the following: (i) The surface charge changes sign, when an oppositely charged polyelectrolyte from a concentrated polyelectrolyte solution is adsorbed. (ii) Tails and loops of the adsorbed polyions dangle into the bulk phase, inducing a small steric force. If polycations and poyanions are adsorbed on top of each other, a strong short range attractive force is seen due to ion-pair formation after crossing a large repulsive electrostatic/steric barrier. (iii) Obviously, after polyelectrolyte adsorption, there are still nonoccupied b…
Layer-by-layer assembled protein/polymer hybrid films: nanoconstruction via specific recognition
Abstract In the present study it is shown that streptavidin-containing multilayer films with varying numbers of polyelectrolyte spacer layers can be fabricated reproducibly using optimized deposition conditions. Direct alternation of streptavidin and PLB leads to multilayer systems with an average streptavidin thickness of 5.3 nm which is in good agreement with the dimensions of the protein. When the streptavidin layers are spacered by more polyelectrolyte layers the distance between the protein sheets is increased up to e.g. 6.5 nm in the case of (PLB/PSS/PAH/PSS/PLB) as spacer layer. X-ray reflectivity reveals that streptavidin increases the surface roughness of the films probably due to …