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Bing-Sui Lu

Publications and source records attributed to Bing-Sui Lu.

26 records · Page 2Linked to original sources

Van der Waals interaction between polymers with sequence-specific polarizabilities: Stiff polymers and flexible Gaussian coils

We consider the van der Waals interaction between a pair of polymers with quenched heterogeneous sequences of local polarizabilities along their backbones, and study the effective pairwise interaction energy for both stiff polymers and flexible Gaussian coils. In particular, we focus on the cases where the pair of polarizability sequences are (i)~distinct and (ii)~identical. We find that the pairwise interaction energies of distinct and identical Gaussian coils are both isotropic and exhibit the same decay behavior for separations larger than the gyration radius, in contradistinction to the orientationally anisotropic interaction energies of distinct and identical stiff polymers. For both Gaussian coils and stiff polymers, the attractive interaction between identical polymers is enhanced if the polarizability sequence is more heterogeneous.

cond-mat.soft↗

Effective interactions between fluid membranes

A self-consistent theory is proposed for the general problem of interacting undulating fluid membranes subject to the constraint that they do not interpenetrate. We implement the steric constraint via an exact functional integral representation, and through the use of a saddle-point approximation transform it into a novel effective steric potential. The steric potential is found to consist of two contributions: one generated by zero mode fluctuations of the membranes, and the other by thermal bending fluctuations. For membranes of cross-sectional area $S$, we find that the bending fluctuation part scales with the inter-membrane separation $d$ as $d^{-2}$ for $d \ll \sqrt{S}$, but crosses over to $d^{-4}$ scaling for $d \gg \sqrt{S}$, whereas the zero mode part of the steric potential always scales as $d^{-2}$. For membranes interacting exclusively via the steric potential, we obtain closed-form expressions for the effective interaction potential and for the rms undulation amplitude $σ$, which becomes small at low temperatures $T$ and/or large bending stiffnesses $κ$. Moreover, $σ$ scales as $d$ for $d \ll \sqrt{S}$, but saturates at $\sqrt{k_{\rm B} T S/κ}$ for $d \gg \sqrt{S}$. In addition, using variational Gaussian theory, we apply our self-consistent treatment to study inter-membrane interactions subject to three different types of potential: (i)~the Moreira-Netz potential for a pair of strongly charged membranes with an intervening solution of multivalent counterions, (ii)~an attractive square well, (iii)~the Morse potential, and (iv)~a combination of hydration and van der Waals interactions.

cond-mat.soft↗

Molecular recognition by van der Waals interaction between polymers with sequence-specific polarizabilities

We analyze van der Waals interactions between two rigid polymers with sequence-specific, anisotropic polarizabilities along the polymer backbones, so that the dipole moments fluctuate parallel to the polymer backbones. Assuming that each polymer has a quenched-in polarizability sequence which reflects, for example, the polynucleotide sequence of a double-stranded DNA molecule, we study the van der Waals interaction energy between a pair of such polymers with rod-like structure for the cases where their respective polarizability sequences are (i) distinct and (ii) identical, with both zero and non-zero correlation length of the polarizability correlator along the polymer backbones in the latter case. For identical polymers, we find a novel $r^{-5}$ scaling behavior of the van der Waals interaction energy for small inter-polymer separation $r$, in contradistinction to the $r^{-4}$ scaling behavior of distinct polymers, with furthermore a pronounced angular dependence favoring attraction between sufficiently aligned identical polymers. Such behavior can assist the molecular recognition between polymers.

cond-mat.soft↗

The Correlation Potential of a Test Ion Near a Strongly Charged Plate

We analytically calculate the correlation potential of a test ion near a \emph{strongly} charged plate inside a dilute $m:-n$ electrolyte. We do this by calculating the electrostatic Green's function in the presence of a nonlinear background potential, the latter having been obtained using the nonlinear Poisson-Boltzmann theory. We consider the general case where the dielectric constants of the plate and the electrolyte are distinct. The following generic results emerge from our analyses: (1) If the distance to the plate $Δz$ is much larger than a Gouy-Chapman length, the plate surface will behave effectively as an infinitely charged surface, and the dielectric constant of the plate effectively plays no role. (2) If $Δz$ is larger than a Gouy-Chapman length but shorter than a Debye length, the correlation potential can be interpreted in terms of an image charge that is three times larger than the source charge. This behavior is independent of the valences of the ions. (3) The Green's function vanishes inside the plate if the surface charge density is infinitely large; hence the electrostatic potential is constant there. In this respect, a strongly charged plate behaves like a conductor plate. (4) If $Δz$ is smaller than a Gouy-Chapman length, the correlation potential is dominated by the conventional image charge due to the dielectric discontinuity at the interface. (5) If $Δz$ is larger than a Debye length, the leading order behavior of the correlation potential will depend on the valences of the ions in the electrolyte. Furthermore, inside an \emph{asymmetric} electrolyte, the correlation potential is \emph{singly} screened, i.e., it undergoes exponential decay with a decay width equal to the Debye length.

cond-mat.soft↗

Generalized Deam-Edwards Approach to the Statistical Mechanics of Randomly Crosslinked Systems

We address the statistical mechanics of randomly and permanently crosslinked networks. We develop a theoretical framework (vulcanization theory) which can be used to systematically analyze the correlation between the statistical properties of random networks and their histories of formation. Generalizing the original idea of Deam and Edwards, we consider an instantaneous crosslinking process, where all crosslinkers (modeled as Gaussian springs) are introduced randomly at once in an equilibrium liquid state, referred to as the preparation state. The probability that two functional sites are crosslinked by a spring exponentially decreases with their distance squared. After formally averaging over network connectivity, we obtained an effective theory with all degrees of freedom replicated 1 + n times. Two thermodynamic ensembles, the preparation ensemble and the measurement ensemble, naturally appear in this theory. The former describes the thermodynamic fluctuations in the state of preparation, while the latter describes the thermodynamic fluctuations in the state of measurement. We classify various correlation functions and discuss their physical significances. In particular, the memory correlation functions characterize how the properties of networks depend on their history of formation, and are the hallmark properties of all randomly crosslinked materials. We clarify the essential difference between our approach and that of Deam-Edwards, discuss the saddle-point order parameters and its physical significance. Finally we also discuss the connection between saddle-point approximation of vulcanization theory, and the classical theory of rubber elasticity as well as the neo-classical theory of nematic elastomers.

cond-mat.stat-mech↗

Statistical physics of isotropic-genesis nematic elastomers: I. Structure and correlations at high temperatures

Isotropic-genesis nematic elastomers (IGNEs) are liquid crystalline polymers (LCPs) that have been randomly, permanently cross-linked in the high-temperature state so as to form an equilibrium random solid. Thus, instead of being free to diffuse throughout the entire volume, as they would be in the liquid state, the constituent LCPs in an IGNE are mobile only over a finite length-scale controlled by the density of cross-links. We address the effects that such network-induced localization have on the liquid-crystalline characteristics of an IGNE, as probed via measurements made at high temperatures. In contrast with the case of uncross-linked LCPs, for IGNEs these characteristics are determined not only by thermal fluctuations but also by the quenched disorder associated with the cross-link constraints. To study IGNEs, we consider a microscopic model of dimer nematogens in which the dimers interact via orientation-dependent excluded volume forces. The dimers are, furthermore, randomly, permanently cross-linked via short Hookean springs, the statistics of which we model by means of a Deam-Edwards type of distribution. We show that at length-scales larger than the size of the nematogens this approach leads to a recently proposed phenomenological Landau theory of IGNEs [Lu et al., Phys. Rev. Lett. 108, 257803 (2012)], and hence predicts a regime of short-ranged oscillatory spatial correlations in the nematic alignment, of both thermal and glassy types. In addition, we consider two alternative microscopic models of IGNEs: (i) a wormlike chain model of IGNEs that are formed via the cross-linking of side-chain LCPs; and (ii) a jointed chain model of IGNEs that are formed via the cross-linking of main-chain LCPs. At large length-scales, both of these models give rise to liquid-crystalline characteristics that are qualitatively in line with those predicted by the dimer-and-springs model.

cond-mat.soft↗

Phenomenological Theory of Isotropic-Genesis Nematic Elastomers

We consider the impact of the elastomer network on the structure and fluctuations in the isotropic-genesis nematic elastomer, via a phenomenological model that underscores the role of network compliance. The model contains a network-mediated nonlocal interaction as well as a new kind of random field, which reflects the memory of the nematic order present at cross-linking, and also encodes local anisotropy due to localized polymers. Thus, we predict a regime of short-ranged oscillatory spatial correlations (both thermal and glassy) in the nematic alignment trapped into the network.

cond-mat.soft↗

Polydomain structure and its origins in isotropic-genesis nematic elastomers

We address the physics of nematic liquid crystalline elastomers randomly crosslinked in the isotropic state. To do this, we construct a phenomenological effective replica Hamiltonian in terms of two order-parameter fields: one for the vulcanization, the other for nematic alignment. Using a Gaussian variational approach, we analyze both thermal and quenched fluctuations of the local nematic order, and find that, even for low temperatures, the macroscopically isotropic polydomain state is stabilized by the network heterogeneity. For sufficiently strong disorder and low enough temperature, our theory predicts unusual, short-range oscillatory structure in (i.e., anti-alignment of) the local nematic order. The present approach, which naturally takes into account the compliant, thermally fluctuating and heterogeneous features of elastomeric networks, can also be applied to other types of randomly crosslinked solids.

cond-mat.soft↗