PubMed Health⌕ Search

Biomedical subjects

Paul M Chaikin

Publications and source records attributed to Paul M Chaikin.

7 recordsLinked to original sources

Shear alignment of sphere-morphology block copolymer thin films with viscous fluid flow.

The effect of shear on crystalline order is interesting fundamentally, as well as technologically, for producing long-range alignment of micron- and nanoscale structures. We study the influence of shear on a sphere-forming diblock copolymer thin film consisting of a stack of two to six hexagonal layers, using a stress-controlled rheometer to transmit the stress through a viscous fluid layer. Above a threshold stress, the hexagonal layers align macroscopically in the "easy shear" direction. A simple phenomenological model with an orientation-dependent order-disorder temperature, T*(ODT)(deltatheta)=T(ODT)[1-(sigma/sigma(c))sin2(3 deltatheta)] and recrystallization describes the influence of stress level, temperature, and shearing time remarkably well.

Journal Article↗

Shear ordering in thin films of spherical block copolymer.

We have investigated shear-induced alignment of a bilayer of spherical diblock copolymer micelles within thin films using molecular dynamics simulations at two different levels of coarse-graining. At the microscopic level, the copolymers are modeled as bead and spring chains with specific interaction potentials which produce strongly segregated spherical micelles. The simulations qualitatively reveal that long-range shear-induced ordering of hexagonally arranged micelles arises because of the tendency of micelles to pursue trajectories of minimum frictional resistance against micelles in the opposing layer. This influences their alignment in the direction of shear without them breaking apart and reforming within the time scale of the simulations. As observed in experiments, the ordering is shown to be very sensitive to the film thickness and shearing rates. To access larger lengths and longer time scales, we further coarse-grain our system to a mesoscopic level where an individual micelle is represented by a spherical particle, which interacts with other micelles through an effective potential obtained from the microscopic simulations. This approach enables us to follow the time evolution of global order from locally ordered domains. An exponentially fast growth of the orientational correlation length of the hexagonal pattern at early times, followed by a crossover to linear growth, is found in the presence of shear, in contrast to the much slower power-law scalings observed in experiments without shear.

Journal Article↗

Ordering mechanisms in two-dimensional sphere-forming block copolymers.

We study the coarsening dynamics of two-dimensional hexagonal patterns formed by single microdomain layers of block copolymers, using numerical simulations. Our study is focused on the temporal evolution of the orientational correlation length, the interactions between topological defects, and the mechanisms of coarsening. We find no free disclinations in the system; rather, they are located on large-angle grain boundaries, commonly where such boundaries bifurcate. The correlation lengths determined from the scattering function, from the density of dislocations, and from the density of disclinations exhibit similar behavior and grow with time according to a power law. The orientational correlation length also grows following a power law, but with a higher exponent than the other correlation lengths. The orientational correlation length grows via annihilation of dislocations, through preferential annihilation of small-angle grain boundaries due to poor screening of the strain field around dislocations located on small-angle grain boundaries. Consequently, the patterns are characterized by large-angle grain boundaries. The most commonly observed mechanism of coarsening is the collapse of smaller grains residing on the boundary of two larger grains delimited by large-angle grain boundaries. Simulations agree remarkably well with experimental results recently obtained.

Journal Article↗

Reversible self-assembly and directed assembly of DNA-linked micrometer-sized colloids.

We present a technique for the directed assembly and self-assembly of micrometer-scale structures based on the control of specific DNA linkages between colloidal particles. The use of DNA links combined with polymer brushes provides an effective way to regulate the range and magnitude of addressable forces between pairs (and further combinations) of different particles. We demonstrate that the autoassembly of alternate microbeads as well as their directed assembly, by using laser tweezers, is reversible. The key to reversibility is preventing the particles from falling into their van der Waals well at close distances. This goal is achieved by the use of adsorbed polymers that limit the number of DNA bridges to one to three between adjacent particles.

Base Sequence↗

Dynamics of pattern coarsening in a two-dimensional smectic system.

We have followed the coarsening dynamics of a single layer of cylindrical block copolymer microdomains in a thin film. This system has the symmetry of a two-dimensional smectic. The orientational correlation length of the microdomains was measured by scanning electron microscopy and found to grow with the average spacing between +/-1/2 disclinations, following a power law xi2(t) approximately t(1/4). By tracking disclinations during annealing with time-lapse atomic force microscopy, we observe dominant mechanisms of disclination annihilation involving tripoles and quadrupoles (three and four disclinations, respectively). We describe how annihilation events involving multiple disclinations result in similarly reduced kinetic exponents as observed here. These results map onto a wide variety of physical systems that exhibit similarly striped patterns.

Journal Article↗

Nature of the divergence in low shear viscosity of colloidal hard-sphere dispersions.

Measurements of the low-shear viscosity eta(o) with a Zimm-Crothers viscometer for dispersions of colloidal hard spheres are reported as a function of volume fraction phi up to 0.56. Nonequilibrium theories based on solutions to the two-particle Smoluchoski equation or ideal mode coupling approximations do not capture the divergence. However, the nonhydrodynamic contribution to the relative viscosity Deltaeta(o) is correlated over a wide range of volume fractions by the Doolittle and Adam-Gibbs equations, indicating an exponential divergence at phi(m)=0.625+/-0.015. The data extend the previously proposed master curve, providing a test for improved theories for the many-body thermodynamic and hydrodynamic interactions that determine the viscosity of hard-sphere dispersions.

Journal Article↗

Correction for piezoelectric creep in scanning probe microscopy images using polynomial mapping.

We describe a method for using polynomial mapping to correct scanning probe microscope images for distortion due to piezoelectric creep. Because such distortion varies from image to image, this method can be used when the actual locations of some features within an image are known absolutely, or in a series of images in which the actual locations of some features are known not to vary. While the general case of polynomial mapping of degree N requires the determination of 2(N+ 1)2 matrix elements by regression, we find that by understanding the mechanism by which piezoelectric creep distorts scanning probe microscope images, we can fix most of these coefficients at 0 or 1 a priori, leaving only 2(N+ 1) coefficients to be determined by regression. We describe our implementation of this strategy using the Interactive Data Language (IDL) programming language, and demonstrate our technique on a series of atomic force microscopy (AFM) images of diblock copolymer microdomains. Using our simplified scheme, we are able to reduce the effects of distortion in an AFM image from 5% of the scan width to a single pixel, using only five reference points.

Journal Article↗