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Biomedical subjects

Steve Granick

Publications and source records attributed to Steve Granick.

28 records · Page 2Linked to original sources

Polymer lateral diffusion at the solid-liquid interface.

Measurements are presented of how polymer surface diffusion at the solid-liquid interface is controlled by surface coverage. The method of measurement was fluorescence correlation spectroscopy (FCS), and the system was poly(ethylene oxide) (PEG) adsorbed onto methyl-terminated self-assembled monolayers in buffered aqueous solution. The translational diffusion coefficient at first increased with increasing surface concentration, presumably because the number of adsorption sites per molecule decreased. Ultimately it slowed by 1 order of magnitude, presumably reflecting jamming by neighboring chains.

Journal Article↗

Noncontact temperature measurement in microliter-sized volumes using fluorescent-labeled DNA oligomers.

A new method of noncontact temperature measurement in microliter-sized volumes is demonstrated, based on the temperature sensitivity of the fluorescence lifetime of rhodamine-G when it is attached to a DNA oligomer. As temperature changes, the spacing between the fluorescent dye and a designed sequence of DNA bases is modulated by conformation changes of the DNA chain, and as a result the ability of dye molecules to fluoresce is also modulated according to differential quenching by bases on the DNA. In the system that we studied, the temperature sensitivity of the fluorescence lifetime was 36-42 ps/ degrees C depending on specific solution conditions. Although this strategy of temperature measurement is demonstrated using a specific sequence of DNA, it can also be generalized to a dye attached to any other intrinsic quencher of fluorescence whose conformation changes with temperature.

DNA, Single-Stranded↗

Slippery questions about complex fluids flowing past solids.

Viscous flow is familiar and useful, yet the underlying physics is surprisingly subtle and complex. Recent experiments and simulations show that the textbook assumption of 'no slip at the boundary' can fail greatly when walls are sufficiently smooth. The reasons for this seem to involve materials chemistry interactions that can be controlled--especially wettability and the presence of trace impurities, even of dissolved gases. To discover what boundary condition is appropriate for solving continuum equations requires investigation of microscopic particulars. Here, we draw attention to unresolved topics of investigation and to the potential to capitalize on 'slip at the wall' for purposes of materials engineering.

Friction↗

Materials science of the gel to fluid phase transition in a supported phospholipid bilayer.

We report the results of in situ AFM measurements examining the phase transition of bilayers formed from the zwitterionic phospholipid, DMPC, 1,2-dimyristoyl-sn-glycero-3-phosphocholine, supported on mica. The images show that the fluid to gel phase transition process features substantial tearing of the bilayer due to the density change between the two phases. The gel to fluid transition is strongly affected by the resultant stress introduced into the gel phase, which changes the degree of cooperativity, the shape of developing fluid phase regions, and the course of the transition.

Aluminum Silicates↗

Contrasting friction and diffusion in molecularly thin confined films.

We study, using fluorescence correlation spectroscopy, translational diffusion in molecularly thin liquids confined within a surface forces apparatus. The diffusion coefficient decreases exponentially from the edges towards the center of the Hertzian contact and further suggests the presence of a small number of distinct diffusion processes. This holds alike a crystallizable fluid (OMCTS) and a glass-former (1,2-propane diol), both of which displayed static friction. We conclude that friction, the average of an ensemble of molecules, masked massively heterogeneous molecular mobility.

Journal Article↗

Limits of the hydrodynamic no-slip boundary condition.

A controversial point in fluid dynamics is to distinguish the relative importance of surface roughness and fluid-surface intermolecular interactions in determining the boundary condition. Here hydrodynamic forces were compared for flow of Newtonian fluids past surfaces of variable roughness but similar, poorly wetted, surface chemistry. The critical shear stress and shear rate to observe deviations from predictions using the no-slip boundary condition increased nearly exponentially with increasing roughness and diverged at approximately 6 nm rms roughness. We conclude that local intermolecular interactions dominated when the surface was very smooth, but roughness dominated otherwise. This quantifies the limits of both ideas.

Journal Article↗

Hydrophobicity at a Janus interface.

Water confined between adjoining hydrophobic and hydrophilic surfaces (a Janus interface) is found to form stable films of nanometer thickness whose responses to shear deformations are extraordinarily noisy. The power spectrum of this noise is quantified. In addition, the frequency dependence of the complex shear modulus is a power law with slope one-half, indicating a distribution of relaxation processes rather than any dominant one. The physical picture emerges that whereas surface energetics encourage water to dewet the hydrophobic side of the interface, the hydrophilic side constrains water to be present, resulting in a flickering, fluctuating complex.

Journal Article↗

Phospholipid membranes as substrates for polymer adsorption.

A largely unsolved problem in soft materials is how surface reconstruction competes with the rate of adsorption. Here, supported phospholipid bilayers of DMPC (1,2-dimyristoyl-sn-glycero-3-phosphocholine) were employed as substrates for the adsorption of a weak polyelectrolyte, polymethacrylic acid, whose time-dependent ratio of charged to uncharged functional groups served to probe the local dielectric environment. Chains that encountered sparsely covered surfaces spread to maximize the number of segment-surface contacts at rates independent of the molar mass (which was varied by a factor of 30), but dependent on the phase of the lipid bilayer, gel or liquid crystal. Surface reconstruction rather than molar mass of the adsorbing molecules seemed to determine the rate of spreading. The significance of these findings is the stark contrast with well-known views of polymer adsorption onto surfaces having structures that are 'frozen' and unresponsive, and is relevant not just from biological and biophysical standpoints, but also in the formulation of many cosmetics and pharmaceutical products.

Adsorption↗