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R. Podgornik

Publications and source records attributed to R. Podgornik.

34 records · Page 2Linked to original sources

Electrostatic image effects for counter-ions between charged planar walls

We study the effect of dielectric inhomogeneities on the interaction between two planparallel charged surfaces with oppositely charged mobile charges in between. The dielectric constant between the surfaces is assumed to be different from the dielectric constant of the two semiinfinite regions bounded by the surfaces, giving rise to electrostatic image interactions. We show that on the weak coupling level the image charge effects are generally small, making their mark only in the second order fluctuation term. However, in the strong coupling limit, the image effects are large and fundamental. They modify the interactions between the two surfaces in an essential way. Our calculations are particularly useful in the regime of parameters where computer simulations would be difficult and extremely time consuming due to the complicated nature of the long range image potentials.

cond-mat.soft↗

Dielectric relaxation of DNA aqueous solutions

We report on a detailed characterization of complex dielectric response of Na-DNA aqueous solutions by means of low-frequency dielectric spectroscopy (40 Hz - 110 MHz). Results reveal two broad relaxation modes of strength 20<Δε_LF<100 and 5<Δε_HF<20, centered at 0.5 kHz<ν_LF<70 kHz and 0.1 MHz<ν_HF<15 MHz. The characteristic length scale of the LF process, 50<L_LF<750nm, scales with DNA concentration as c_DNA^{-0.29\pm0.04} and is independent of the ionic strength in the low added salt regime. Conversely, the measured length scale of the LF process does not vary with DNA concentration but depends on the ionic strength of the added salt as I_s^{-1} in the high added salt regime. On the other hand, the characteristic length scale of the HF process, 3<L_HF<50 nm, varyes with DNA concentration as c_DNA^{-0.5} for intermediate and large DNA concentrations. At low DNA concentrations and in the low added salt limit the characteristic length scale of the HF process scales as c_DNA^{-0.33}. We put these results in perspective regarding the integrity of the double stranded form of DNA at low salt conditions as well as regarding the role of different types of counterions in different regimes of dielectric dispersion. We argue that the free DNA counterions are primarily active in the HF relaxation, while the condensed counterions play a role only in the LF relaxation. We also suggest theoretical interpretations for all these length scales in the whole regime of DNA and salt concentrations and discuss their ramifications and limitations.

cond-mat.soft↗

Electrostatic Contribution to the Persistence Length of a Semiflexible Dipolar Chain

We investigate the electrostatic contribution to the persistence length of a semiflexible polymer chain whose segments interact via a screened Debye-H\" uckel dipolar interaction potential. We derive the expressions for the renormalized persistence length on the level of a 1/D-expansion method already successfully used in other contexts of polyelectrolye physics. We investigate different limiting forms of the renormalized persistence length of the dipolar chain and show that in general it depends less strongly on the screening length than in the context of a monopolar chain. We show that for a dipolar chain the electrostatic persistence length in the same regime of the parameter phase space as the original Odijk-Skolnick-Fixman (OSF) form for a monopolar chain depends logarithmically on the screening length rather than quadratically. This can be understood solely on the basis of a swifter decay of the dipolar interactions with separation compared to the monopolar electrostatic interactions. We comment also on the general contribution of higher multipoles on the electrostatic renormalization of the bending rigidity.

cond-mat.soft↗

Correlated and Decorrelated Positional and Orientational Order in the Nucleosomal Core Particle Mesophases

We investigate the orientational order of transverse polarization vectors of long columns of nucleosomal core particles and their coupling to positional order in high density mesophases discovered recently. Inhomogeneous polar ordering of these columns precipitates crystalization of the 2D sections with different orientations of the transverse polarization vector on each column in the unit cell. We propose possible scenarios for going from the 2D hexagonal phase into distorted lamellar and related phases observed experimentally.

cond-mat.soft↗

Van der Waals interactions across stratified media

Working at the Lifshitz level, we investigate the van der Waals interactions across a series of layers with a periodic motif. We derive the complete form of the van der Waals interaction as an explicit function of the number of periodic layers. We then compare our result with an approximation based on an anisotropic-continuum representation of the stratified medium. Satisfactory agreement between discrete-layer and continuum models is reached only for thicknesses of ten or more layers.

cond-mat.soft↗

Membrane pinning on a disordered substrate

We investigate interactions between an elastic membrane and a substrate characterized by quenched positional disorder in the height function. We show that the positional disorder transforms the standard secondary DLVO minimum into two separate states: the hovering state characterized by a planar membrane at a finite separation from the interface and a pinned state where the membrane follows closely the asperities of the substrate and is as a consequence quite corrugated. The transition between the two states is continuous and depends on the parameters of the underlying DLVO potential as well as the parameters describing the quenched height-height correlation function of the substrate.

cond-mat.soft↗

Electrons on the double helix: optical experiments on native DNA

Optical experiments on calf thymus DNA films subjected to different buffer environments are reported. The optical conductivity is that of a disordered or lightly doped semiconductor with a well-defined band-gap for charge excitations and low frequency transport determined by a small number of strongly localized electron states.

cond-mat.dis-nn↗

Positional, Reorientational and Bond Orientational Order in DNA Mesophases

We investigate the orientational order of transverse polarization vectors of long, stiff polymer molecules and their coupling to bond orientational and positional order in high density mesophases. Homogeneous ordering of transverse polarization vector promotes distortions in the hexatic phase, whereas inhomogeneous ordering precipitates crystalization of the 2D sections with different orientations of the transverse polarization vector on each molecule in the unit cell. We propose possible scenarios for going from the hexatic phase, through the distorted hexatic phase to the crystalline phase with an orthorhombic unit cell observed experimentally for the case of DNA.

cond-mat.soft↗

Casimir and pseudo-Casimir interactions in confined polyelectrolytes

We investigate the pseudo-Casimir force acting between two charged surfaces confining a single polyelectrolyte chain with opposite charge. We expand the exact free energy to the second order in the local electrostatic field as well as the replicated polymer density field around the mean-field (saddle-point) solution. The quadratic terms lead to a fluctuation interaction that is partly due to the (thermal) Casimir effect for the confined electrostatic field and partly due to the pseudo-Casimir effect due to the confined replicated polymer density field. We study the intersurface separation dependence of both effects and show that the pseudo-Casimir effect leads to a long range attraction between the surfaces that decays with an anomalous algebraic exponent of $\sim 1.7$, smaller than the standard exponent of 2 in the case of Casimir interactions.

cond-mat.soft↗

Equation of state for polymer liquid crystals: theory and experiment

The first part of this paper develops a theory for the free energy of lyotropic polymer nematic liquid crystals. We use a continuum model with macroscopic elastic moduli for a polymer nematic phase. By evaluating the partition function, considering only harmonic fluctuations, we derive an expression for the free energy of the system. We find that the configurational entropic part of the free energy enhances the effective repulsive interactions between the chains. This configurational contribution goes as the fourth root of the direct interactions. Enhancement originates from the coupling between bending fluctuations and the compressibility of the nematic array normal to the average director. In the second part of the paper we use osmotic stress to measure the equation of state for DNA liquid crystals in 0.1M to 1M NaCl solutions. These measurements cover 5 orders of magnitude in DNA osmotic pressure. At high osmotic pressures the equation of state, dominated by exponentially decaying hydration repulsion, is independent of the ionic strength. At lower pressures the equation of state is dominated by fluctuation enhanced electrostatic double layer repulsion. The measured equation of state for DNA fits well with our theory for all salt concentrations. We are able to extract the strength of the direct electrostatic double layer repulsion. This is a new and alternative way of measuring effective charge densities along semiflexible polyelectrolytes.

cond-mat.soft↗

Charge Fluctuation Forces Between Stiff Polyelectrolytes in Salt Solution: Pairwise Summability Re-examined

We formulate low-frequency charge-fluctuation forces between charged cylinders - parallel or skewed - in salt solution: forces from dipolar van der Waals fluctuations and those from the correlated monopolar fluctuations of mobile ions. At high salt concentrations forces are exponentially screened. In low-salt solutions dipolar energies go as $R^{-5}$ or $R^{-4}$; monopolar energies vary as $R^{-1}$ or $\ln{R}$, where $R$ is the minimal separation between cylinders. However, pairwise summability of rod-rod forces is easily violated in low-salt conditions. Perhaps the most important result is not the derivation of pair potentials but rather the demonstration that some of these expressions may not be used for the very problems that originally motivated their derivation.

cond-mat↗

Coupling between Smectic and Twist Modes in Polymer Intercalated Smectics

We analyse the elastic energy of an intercalated smectic where orientationally ordered polymers with an average orientation varying from layer to layer are intercalated between smectic planes. The lowest order terms in the coupling between polymer director and smectic layer curvature are added to the smectic elastic energy. Integration over the smectic degrees of freedom leaves an effective polymer twist energy that has to be included into the total polymer elastic energy leading to a fluctuational renormalization of the intercalated polymer twist modulus. If the polymers are chiral this in its turn leads to a renormalization of the cholesteric pitch.

cond-mat.soft↗

Bond Orientational Order, Molecular Motion and Free Energy of High Density DNA Mesophases

By equilibrating condensed DNA arrays against reservoirs of known osmotic stress and examining them with several structural probes, it has been possible to achieve a detailed thermodynamic and structural characterization of the change between two distinct regions on the liquid crystalline phase digram: a higher-density hexagonally packed region with long-range bond orientational order in the plane perpendicular to the average molecular direction; and a lower-density cholesteric region with fluid-like positional order. X-rays scattering on highly ordered DNA arrays at high density and with the helical axis oriented parallel to the incoming beam showed a six-fold azimuthal modulation of the first order diffraction peak that reflects the macroscopic bond-orientational order. Transition to the less-dense cholesteric phase through osmotically controlled swelling shows the loss of this bond orientational order that had been expected from the change in optical birefringence patterns and that is consistent with a rapid onset of molecular positional disorder. This change in motion was previously inferred from intermolecular force measurements and is now confirmed by $\rm ^{31}P$ NMR. Controlled reversible swelling and compaction under osmotic stress, spanning a range of densities between $\sim 120$ mg/ml to $\sim 600$ mg/ml, allows measurement of the free energy changes throughout each phase and at the phase transition, essential information for theories of liquid-crystalline states.

chem-ph↗

Orientational Ordering of Polymers on a Fluctuating Flexible Surface

Arguments are presented to the effect that embedding semi-flexible (wormlike) ideal polymers into a fluctuating, flexible surface leads to an effective attractive orientational interaction between polymer segments that precipitates an orientational ordering transition of the polymer chains on the surface even in the case of otherwise ideal (non-interacting) chains. The orientational interaction is analogous to the (zero order) Casimir force and is due to the energy change in surface conformational fluctuations in the presence of embedded semi-flexible chains.

cond-mat↗

Surface Polymer Network Model and Effective Membrane Curvature Elasticity

A microscopic model of a surface polymer network - membrane system is introduced, with contact polymer surface interactions that can be either repulsive or attractive and sliplinks of functionality four randomly distributed over the supporting membrane surface anchoring the polymers to it. For the supporting surface perturbed from a planar configuration and a small relative number of surface sliplinks, we investigate an expansion of the free energy in terms of the local curvatures of the surface and the surface density of sliplinks, obtained through the application of the Balian - Bloch - Duplantier multiple surface scattering method. As a result, the dependence of the curvature elastic modulus, the Gaussian modulus as well as of the spontaneous curvature of the "dressed" membrane, ~{\sl i.e.} polymer network plus membrane matrix, is obtained on the mean polymer bulk end to end separation and the surface density of sliplinks.

cond-mat↗

Parameterization invariance and shape equations of elastic axisymmetric vesicles

The issue of different parameterizations of the axisymmetric vesicle shape addressed by Hu Jian-Guo and Ou-Yang Zhong-Can [ Phys.Rev. E {\bf 47} (1993) 461 ] is reassesed, especially as it transpires through the corresponding Euler - Lagrange equations of the associated elastic energy functional. It is argued that for regular, smooth contours of vesicles with spherical topology, different parameterizations of the surface are equivalent and that the corresponding Euler - Lagrange equations are in essence the same. If, however, one allows for discontinuous (higher) derivatives of the contour line at the pole, the differently parameterized Euler - Lagrange equations cease to be equivalent and describe different physical problems. It nevertheless appears to be true that the elastic energy corresponding to smooth contours remains a global minimum.

cond-mat↗