arXiv subjects

Jens-Uwe Sommer

Publications and source records attributed to Jens-Uwe Sommer.

At least 37 records · Page 2Linked to original sources

arXiv2021

The Formation and Structure of Olympic Gels

Different methods for creating Olympic gels are analyzed using computer simulations. First ideal reference samples are obtained from freely interpenetrating semi-dilute solutions and melts of cyclic polymers. The distribution of pairwise concatenations per cyclic molecule is given by a Poisson-distribution and can be used to describe the elastic structure of the gels. Several batches of linear chains decorated with different selectively binding groups at their ends are mixed in the "DNA Origami" technique and network formation is realized. While the formation of cyclic molecules follows mean field predictions below overlap of the precursor molecules, an enhanced ring formation above overlap is found that is not explained by mean field arguments. The "progressive construction" method allows to create Olympic gels with a single reaction step from a concentrated mixture of large compressed rings with a low weight fraction short chains that are below overlap concentration. This method, however, is limited by the difficulty to obtain a sufficiently high degree of polymerization of the large rings.

cond-mat.soft↗

arXiv2021

Effect of Topology on the Conformations of Ring Polymers

The bond fluctuation method is used to simulate both non-concatenated entangled and interpenetrating melts of ring polymers. We find that the swelling of interpenetrating rings upon dilution follows the same laws as for linear chains. Knotting and linking probabilities of ring polymers in semi-dilute solution are analyzed using the HOMFLY polynomial. We find an exponential decay of the knotting probability of rings. The correlation length of the semi-dilute solution can be used to superimpose knotting data at different concentrations. A power law dependence $f_{n}\simϕR^{2}\simϕ^{0.77}N$ for the average number $f_{n}$ of linked rings per ring at concentrations larger than the overlap volume fraction of rings $ϕ^{*}$ is determined from the simulation data. The fraction of non-concatenated rings displays an exponential decay $P_{OO}\sim\exp(-f_{n})$, which indicates $f_{n}$ to provide the entropic effort for not forming concatenated conformations. Based upon this results we find four different regimes for the conformations of rings in melts that are separated by a critical lengths $N_{OO}$, $N_{C}$ and $N^{*}$. $N_{OO}$ describes the onset of the effect of non-concatenation below which topological effects are not important, $N_{C}$ is the cross-over between weak and strong compression of rings, and $N^{*}$ is defined by the cross-over from a non-concatenation contribution $f_{n}\simϕR^{2}$ to an overlap dominated concatenation contribution $f_{n}\simϕN^{1/2}$ at $N>N^{*}$. For $N_{OO}<N<N_{C}$, the scaling of ring sizes $R\sim N^{2/5}$ results from balancing non-concatenation with weak compression of rings. For $N_{C}<N<N^{*}$, non-concatenation and strong compression imply $R\sim N^{3/8}$. Our simulation data for non-interpenetrating rings up to $N=1024$ are in good agreement with the prediction for weakly compressed rings.

cond-mat.soft↗

arXiv2021

On the Structure of Star-Polymer Networks

Using the bond fluctuation model we study polymer networks obtained by endlinking of symmetric 4-arm star polymers. We consider two types of systems. Solutions of one type (A) of star polymers and solution of two types (A,B) of star polymer where A-type polymers can only crosslink with B-type polymers. We find that network defects in $A$ networks are dominated by short dangling loops close to overlap concentration $c^{*}$. $AB$ networks develop a more perfect network structure, since loop sizes involving an odd number of stars are impossible, and thus, the most frequent dangling loop with largest impact on the phantom modulus is absent. The analysis of the pair-correlation and scattering function reveals that there is an amorphous packing of $A$ and $B$ type stars with a homogenization of $A$ and $B$ concentrations upon cross-linking at intermediate length scales in contrast to the previously suggested crystalline like order of $A$ and $B$ components at $c^{*}$. This result is corroborated by the coincidence of the probabilities of the shortest loop structures (which is impossible upon the previously suggested packing of stars) in both types of networks. Furthermore, we derive the vector order parameters associated with the most frequent network structures based on the phantom model. In particular, for $AB$ networks we can show that there is a dominating cyclic defect with a clearly separated order parameter that could be used to analyze cyclic network defects.

cond-mat.soft↗

arXiv2021

Short Cyclic Structures in Polymer Model Networks: A Test of Mean Field Approximation by Monte Carlo Simulations

A mean field rate theory description of the homo- and co-polymerization of $f$-functional molecules is developed, which contains the formation of short cyclic structures inside the network. The predictions of this model are compared with Monte-Carlo simulations of cross-linking of star polymers in solution. We find that homo-polymerizations are well captured by mean-field models at concentrations larger than one quarter of the geometrical overlap concentration. All simulation data can be fit using a single geometric parameter for cyclization. The simulation data reveal that within the range of parameters of the present study correlations among multiply connected molecules can be neglected. Thus, mean-field treatments of homopolymerizations are reasonable approximations, if short cycles are properly addressed. Co-polymerization is considered in the case of strict A-B reactions, where all reactive groups of individual molecules are either of type A or B. For these systems we find a clear influence of the local intermixing of A and B groups for all concentrations investigated. In consequence, mean-field models are less appropriate to describe the simulation data. The lack of ring structures containing an odd number of molecules as compared to homopolymerizations at the same extent of reaction allows for the formation of stable AB networks at concentrations one order of magnitude below the geometrical overlap concentration.

cond-mat.soft↗

arXiv2021

The Swelling of Olympic Gels

The swelling equilibrium of Olympic gels, which are composed of entangled cyclic polymers, is studied by Monte Carlo Simulations. In contrast to chemically crosslinked polymer networks, we observe that Olympic gels made of chains with a \emph{larger} degree of polymerization, $N$, exhibit a \emph{smaller} equilibrium swelling degree, $Q\propto N^{-0.28}ϕ_{0}^{-0.72}$, at the same polymer volume fraction $ϕ_{0}$ at network preparation. This observation is explained by a desinterspersion process of overlapping non-concatenated rings upon swelling.

cond-mat.soft↗

arXiv2021

Olympic Gels: Concatenation and Swelling

Concatenation and equilibrium swelling of Olympic gels, which are composed of entangled cyclic polymers, is studied by Monte Carlo Simulations. The average number of concatenated molecules per cyclic polymers, $f_n$, is found to depend on the degree of polymerization, $N$, and polymer volume fraction at network preparation, $ϕ_0$, as $f_n ~ ϕ_0^{ν/(3ν-1)}N$ with scaling exponent $ν = 0.588$. In contrast to chemically cross-linked polymer networks, we observe that Olympic gels made of longer cyclic chains exhibit a smaller equilibrium swelling degree, $Q ~ N^{-0.28} ϕ_0^{-0.72}$, at the same polymer volume fraction $ϕ_0$. This observation is explained by a desinterspersion process of overlapping non-concatenated rings upon swelling, which is tested directly by analyzing the change in overlap of the molecules upon swelling.

cond-mat.soft↗

arXiv2020

Chemotaxis of cargo-carrying self-propelled particles

Active particles with their characteristic feature of self-propulsion are regarded as the simplest models for motility in living systems. The accumulation of active particles in low activity regions has led to the general belief that chemotaxis requires additional features and at least a minimal ability to process information and to control motion. We show that self-propelled particles display chemotaxis and move into regions of higher activity, if the particles perform work on passive objects, or cargo, to which they are bound. The origin of this cooperative chemotaxis is the exploration of the activity gradient by the active particle when bound to a load, resulting in an average excess force on the load in the direction of higher activity. Using a minimalistic theoretical model, we capture the most relevant features of these active-passive dimers and in particular we predict the crossover between anti-chemotactic and chemotactic behaviour. Moreover we show that merely connecting active particles to chains is sufficient to obtain the crossover from anti-chemotaxis to chemotaxis with increasing chain length. Such an active complex is capable of moving up a gradient of activity such as provided by a gradient of fuel and to accumulate where the fuel concentration is at its maximum. The observed transition is of significance to proto-forms of life enabling them to locate a source of nutrients even in the absence of any supporting sensomotoric apparatus.

cond-mat.soft↗

arXiv2020

Correlations in multithermostat Brownian systems with Lorentz force

We study the motion of a Brownian particle subjected to Lorentz force due to an external magnetic field. Each spatial degree of freedom of the particle is coupled to a different thermostat. We show that the magnetic field results in correlation between different velocity components in the stationary state. Integrating the velocity autocorrelation matrix, we obtain the diffusion matrix that enters the Fokker-Planck equation for the probability density. The eigenvectors of the diffusion matrix do not align with the temperature axes. As a consequence the Brownian particle performs spatially correlated diffusion. We further show that in the presence of an isotropic confining potential, an unusual, flux-free steady state emerges which is characterized by a non-Boltzmann density distribution, which can be rotated by reversing the magnetic field. The nontrivial steady state properties of our system result from the Lorentz force induced coupling of the spatial degrees of freedom which cease to exist in equilibrium corresponding to a single-temperature system.

cond-mat.stat-mech↗

arXiv2020

Unusual stationary state in Brownian systems with Lorentz force

In systems with overdamped dynamics, the Lorentz force reduces the diffusivity of a Brownian particle in the plane perpendicular to the magnetic field. The anisotropy in diffusion implies that the Fokker-Planck equation for the probabiliy distribution of the particle acquires a tensorial coefficient. The tensor, however, is not a typical diffusion tensor due to the antisymmetric elements which account for the fact that Lorentz force curves the trajectory of a moving charged particle. This gives rise to unusual dynamics with features such as additional Lorentz fluxes and a nontrivial density distribution, unlike a diffusive system. The equilibrium properties are, however, unaffected by the Lorentz force. Here we show that by stochastically resetting the Brownian particle, a nonequilibrium steady state can be created which preserves the hallmark features of dynamics under Lorentz force. We then consider a minimalistic example of spatially inhomogeneous magnetic field, which shows how Lorentz fluxes fundamentally alter the boundary conditions giving rise to an unusual stationary state.

cond-mat.stat-mech↗

arXiv2019

Pseudo-chemotaxis of active Brownian particles competing for food

Using Brownian dynamics simulations, the motion of active Brownian particles (ABPs) in the presence of fuel (or 'food') sources is studied. It is an established fact that within confined stationary systems, the activity of ABPs generates density profiles that are enhanced in regions of low activity, which is generally referred to as 'anti-chemotaxis'. We demonstrate that -- contrary to common believes -- in non-stationary setups, emerging here as a result of short fuel bursts, our model ABPs do instead exhibit signatures of chemotactic behavior. In direct competition with inactive, but otherwise identical Brownian particles (BPs), the ABPs are shown to fetch a larger amount of food. From a biological perspective, the ability to turn active would, despite of the absence of sensoric devices, encompass an evolutionary advantage.

physics.bio-ph↗

arXiv2019

Pseudochemotaxis in inhomogeneous active Brownian systems

We study dynamical properties of confined, self-propelled Brownian particles in an inhomogeneous activity profile. Using Brownian dynamics simulations, we calculate the probability to reach a fixed target and the mean first passage time to the target of an active particle. We show that both these quantities are strongly influenced by the inhomogeneous activity. When the activity is distributed such that high-activity zone is located between the target and the starting location, the target finding probability is increased and the passage time is decreased in comparison to a uniformly active system. Moreover, for a continuously distributed profile, the activity gradient results in a drift of active particle up the gradient bearing resemblance to chemotaxis. Integrating out the orientational degrees of freedom, we derive an approximate Fokker-Planck equation and show that the theoretical predictions are in very good agreement with the Brownian dynamics simulations.

cond-mat.soft↗

arXiv2019

Nondiffusive Fluxes in Brownian System with Lorentz Force

The Fokker-Planck equation provides complete statistical description of a particle undergoing random motion in a solvent. In the presence of Lorentz force due to an external magnetic field, the Fokker-Planck equation picks up a tensorial coefficient, which reflects the anisotropy of the particle's motion. This tensor, however, can not be interpreted as a diffusion tensor; there are antisymmetric terms which give rise to fluxes perpendicular to the density gradients. Here, we show that for an inhomogeneous magnetic field these nondiffusive fluxes have finite divergence and therefore affect the density evolution of the system. Only in the special cases of a uniform magnetic field or carefully chosen initial condition with the same symmetry as the magnetic field can these fluxes be ignored in the density evolution.

cond-mat.stat-mech↗

arXiv2019

Lorentz forces induce inhomogeneity and fluxes in active systems

We consider the nonequilibrium dynamics of a charged active Brownian particle in the presence of a space dependent magnetic field. It has recently been shown that the Lorentz force induces a particle flux perpendicular to density gradients, thus preventing a diffusive description of the dynamics. Whereas a passive system will eventually relax to an equilibrium state, unaffected by the magnetic field, an active system subject to a spatially varying Lorentz force settles into a nonequilibrium steady state characterized by an inhomogeneous density and divergence-free bulk fluxes. A macroscopic flux of charged active particles is induced by the gradient of the magnetic field only and does not require additional symmetric breaking such as density or potential gradients. This stands in marked contrast to similar phenomena in condensed matter such as the classical Hall effect. In a confined geometry we observe circulating fluxes, which can be reversed by inverting the direction of the magnetic field. Our theoretical approach, based on coarse-graining of the Fokker-Planck equation, yields analytical results for the density, fluxes, and polarization in the steady state, all of which are validated by direct computer simulation. We demonstrate that passive tracer particles can be used to measure the essential effects of the Lorentz force on the active particle bath, and we discuss under which conditions the effects of the flux could be observed experimentally.

cond-mat.soft↗

arXiv2017

Influence of weak reversible cross-linkers on entangled polymer melt dynamics

In this paper we study a system of entangled chains that bear reversible cross-links in a melt state. The cross-links are tethered uniformly on the backbone of each chain. A slip-link type model for the system is presented and solved for the relaxation modulus. The effects of entanglements and reversible cross-linkers are modelled as discrete form of constraints that influence the motion of the primitive path. In contrast to a non-associating entangled system the model calculations demonstrate that the elastic modulus has a much higher first plateau and a delayed terminal relaxation. These effects are attributed to the evolution of the entangled chains as influenced by tethered reversible linkers. The model is solved for the case when linker survival time $τ_s$ is greater than the entanglement time $τ_e$ but less than the Rouse time $τ_R$.

cond-mat.soft↗

arXiv2012

Critical adsorption controls translocation of polymer chains through lipid bilayers and permeation of solvent

Monte Carlo simulations using an explicit solvent model indicate a new pathway for translocation of a polymer chain through a lipid bilayer. We consider a polymer chain composed of repeat units with a given hydrophobicity and a coarse-grained model of a lipid bilayer in the self-organized liquid state. By varying the degree of hydrophobicity the chain undergoes an adsorption transition with respect to the lipid bilayer. Close to the transition point, at a properly balanced hydrophobicity of the chain, the membrane becomes transparent with respect to the chain. At the same time the solvent permeability of the bilayer is strongly increased in the region close to adsorbed chain. Our results indicate that the critical point of adsorption of the polymer chain interacting with the fluctuating lipid bilayer could play a key role for the translocation of molecules though biological membranes.

cond-mat.soft↗

arXiv2008

Nano-scale brushes: How to build a smart surface coating

Via computer simulations, we demonstrate how a densely grafted layer of polymers, a {\it brush}, could be turned into an efficient switch through chemical modification of some of its end-monomers. In this way, a surface coating with reversibly switchable properties can be constructed. We analyze the fundamental physical principle behind its function, a recently discovered surface instability, and demonstrate that the combination of a high grafting density, an inflated end-group size and a high degree of monodispersity are conditions for an optimal functionality of the switch.

cond-mat.soft↗

arXiv1999

Localization transition of random copolymers at interfaces

We consider adsorption of random copolymer chains onto an interface within the model of Garel et al. Europhysics Letters 8, 9 (1989). By using the replica method the adsorption of the copolymer at the interface is mapped onto the problem of finding the ground state of a quantum mechanical Hamiltonian. To study this ground state we introduce a novel variational principle for the Green's function, which generalizes the well-known Rayleigh-Ritz method of Quantum Mechanics to nonstationary states. Minimization with an appropriate trial Green's function enables us to find the phase diagram for the localization-delocalization transition for an ideal random copolymer at the interface.

cond-mat.soft↗

arXiv1997

Random copolymers at a selective interface: many chains with excluded volume interactions

We investigate numerically, using the bond-fluctuation model, the adsorption of many random AB--copolymers with excluded volume interactions at the interface between two solvents. We find two regimes, controlled by the total number of polymers. In the first (dilute) regime, the copolymers near the interface extend parallel to it, while in the second regime they extend perpendicular to it. The density at the interface and the density in the bulk depend differently on the total number of copolymers: In the first regime the density at the interface increases more rapidly then in the bulk, whereas the opposite is true in the second regime.

cond-mat.soft↗