Entanglement Length Scale Separates Threading from Branching of Unknotted and Non-concatenated Ring Polymers in Melts
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ABSTRACT:
SUBMITTER: Ubertini M
PROVIDER: S-EPMC9753756 | biostudies-literature | 2022 Nov
REPOSITORIES: biostudies-literature
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Project description:Entanglement-assisted concatenated quantum codes (EACQCs), constructed by concatenating two quantum codes, are proposed. These EACQCs show significant advantages over standard concatenated quantum codes (CQCs). First, we prove that, unlike standard CQCs, EACQCs can beat the nondegenerate Hamming bound for entanglement-assisted quantum error-correction codes (EAQECCs). Second, we construct families of EACQCs with parameters better than the best-known standard quantum error-correction codes (QECCs) and EAQECCs. Moreover, these EACQCs require very few Einstein-Podolsky-Rosen (EPR) pairs to begin with. Finally, it is shown that EACQCs make entanglement-assisted quantum communication possible, even if the ebits are noisy. Furthermore, EACQCs can outperform CQCs in entanglement fidelity over depolarizing channels if the ebits are less noisy than the qubits. We show that the error-probability threshold of EACQCs is larger than that of CQCs when the error rate of ebits is sufficiently lower than that of qubits. Specifically, we derive a high threshold of 47% when the error probability of the preshared entanglement is 1% to that of qubits.
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Project description:The motion of nanoparticles (NPs) in entangled melts of linear polymers and nonconcatenated ring polymers are compared by large-scale molecular dynamics simulations. The comparison provides a paradigm for the effects of polymer architecture on the dynamical coupling between NPs and polymers in nanocomposites. Strongly suppressed motion of NPs with diameter d larger than the entanglement spacing a is observed in a melt of linear polymers before the onset of Fickian NP diffusion. This strong suppression of NP motion occurs progressively as d exceeds a and is related to the hopping diffusion of NPs in the entanglement network. In contrast to the NP motion in linear polymers, the motion of NPs with d > a in ring polymers is not as strongly suppressed prior to Fickian diffusion. The diffusion coefficient D decreases with increasing d much slower in entangled rings than in entangled linear chains. NP motion in entangled nonconcatenated ring polymers is understood through a scaling analysis of the coupling between NP motion and the self-similar entangled dynamics of ring polymers.
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Project description:A scaling model of self-similar conformations and dynamics of nonconcatenated entangled ring polymers is developed. Topological constraints force these ring polymers into compact conformations with fractal dimension df = 3 that we call fractal loopy globules (FLGs). This result is based on the conjecture that the overlap parameter of subsections of rings on all length scales is the same and equal to the Kavassalis-Noolandi number OKN ≈ 10-20. The dynamics of entangled rings is self-similar and proceeds as loops of increasing sizes are rearranged progressively at their respective diffusion times. The topological constraints associated with smaller rearranged loops affect the dynamics of larger loops through increasing the effective friction coefficient but have no influence on the entanglement tubes confining larger loops. As a result, the tube diameter defined as the average spacing between relevant topological constraints increases with time t, leading to "tube dilation". Analysis of the primitive paths in molecular dynamics simulations suggests a complete tube dilation with the tube diameter on the order of the time-dependent characteristic loop size. A characteristic loop at time t is defined as a ring section that has diffused a distance equal to its size during time t. We derive dynamic scaling exponents in terms of fractal dimensions of an entangled ring and the underlying primitive path and a parameter characterizing the extent of tube dilation. The results reproduce the predictions of different dynamic models of a single nonconcatenated entangled ring. We demonstrate that traditional generalization of single-ring models to multi-ring dynamics is not self-consistent and develop a FLG model with self-consistent multi-ring dynamics and complete tube dilation. This selfconsistent FLG model predicts that the longest relaxation time of nonconcatenated entangled ring polymers scales with their degree of polymerization N as τrelax ~ N7/3, while the diffusion coefficient of these rings scales as D3d ~ N-5/3. For the entangled solutions and melts of rings, we predict power law stress relaxation function G(t) ~ t-3/7 at t < τrelax without a rubbery plateau and the corresponding viscosity scaling with the degree of polymerization N as η ~ N4/3. These theoretical predictions are in good agreement with recent computer simulations and are consistent with experiments of melts of nonconcatenated entangled rings.
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Project description:Unconcatenated ring polymers in concentrated solutions and melt are remarkably well described as double-folded conformations on randomly branched primitive trees. This picture though contrasts recent evidence for extensive intermingling between close-by rings in the form of long-lived topological constraints or threadings. Here, we employ the concept of ring minimal surface to quantify the extent of threadings in polymer solutions of the double-folded rings vs rings in equilibrated molecular dynamics computer simulations. Our results show that the double-folded ring polymers are significantly less threaded compared to their counterparts at equilibrium. Second, threadings form through a slow process whose characteristic time-scale is of the same order of magnitude as that of the diffusion of the rings in solution. These findings are robust, being based on universal (model-independent) observables as the average fraction of threaded length or the total penetrations between close-by rings and the corresponding distribution functions.
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Project description:We use computer simulations to study a system of two unlinked ring polymers, whose length and bending stiffness are systematically varied. We derive the effective potentials between the rings, calculate the areas of minimal surfaces of the same, and characterize the threading between them. When the two rings are of the same kind, threading of a one ring through the surface of the other is immanent for small ring-ring separations. Flexible rings pierce the surface of the other ring several times but only shallowly, as compared to the stiff rings which pierce less frequently but deeply. Typically, the ring that is being threaded swells and flattens up into an oblate-like conformation, while the ring that is threading the other takes a shape of an elongated prolate. The roles of the threader and the threaded ring are being dynamically exchanged. If, on the other hand, the rings are of different kinds, the symmetry is broken and the rings tend to take up roles of the threader and the threaded ring with unequal probabilities. We propose a method how to predict these probabilities based on the parameters of the individual rings. Ultimately, our work captures the interactions between ring polymers in a coarse-grained fashion, opening the way to large-scale modelling of materials such as kinetoplasts, catenanes or topological brushes.
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Project description:Abnormally slower diffusional processes than its internal structure relaxation have been observed in ring polymeric melt systems recently. A key structural feature in ring polymer melts is topological constraints which allow rings to assume a threading configuration in the melt phase. In this work, we constructed a lattice model under the assumption of asymmetric diffusivity between two threading rings, and investigated a link between the structural correlation and its dynamic behavior via Monte Carlo simulations. We discovered that the hierarchical threading configurations render the whole system to exhibit abnormally slow dynamics. By analyzing statistical distributions of timescales of threading configurations, we found that the decoupling between internal structure relaxation and diffusion is crucial to understand the threading effects on the dynamics of a ring melt. In particular, in the limit of small but threaded rings, scaling exponents of the diffusion coefficient D and timescale τ diff with respect to the degree of polymerization N agree well with that of the annealed tree model as well as our mean-field analysis. As N increases, however, the ring diffusion abruptly slows down to the glassy behavior, which is supported by a breakdown of the Stokes⁻Einstein relation.
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Project description:We have measured the linear rheology of critically purified ring polyisoprenes, polystyrenes and polyethyleneoxides of different molar masses. The ratio of the zero-shear viscosities of linear polymer melts η0,linear to their ring counterparts η0,ring at isofrictional conditions is discussed as function of the number of entanglements Z. In the unentangled regime η0,linear/η0,ring is virtually constant, consistent with the earlier data, atomistic simulations, and the theoretical expectation η0,linear/η0,ring=2. In the entanglement regime, the Z-dependence of rings viscosity is much weaker than that of linear polymers, in qualitative agreement with predictions from scaling theory and simulations. The power-law extracted from the available experimental data in the rather limited range 1<Z<20, η0,linear/η0,ring ~ Z1.2±0.3, is weaker than the scaling prediction (η0,linear/η0,ring ~ Z1.6±0.3 ) and the simulations (η0,linear/η0,ring ~ Z2.0±0.3 ). Nevertheless, the present collection of state-of-the- art experimental data unambiguously demonstrates that rings exhibit a universal trend clearly departing from that of their linear counterparts, and hence it represents a major step toward resolving a 30-year old problem.
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Project description:We present Monte Carlo computer simulations for melts of semiflexible randomly knotted and randomly concatenated ring polymers on the fcc lattice and in slit confinement. Through systematic variation of the slit width at fixed melt density, we explore the influence of confinement on single-chain conformations and interchain interactions. We demonstrate that confinement makes chains globally larger and more elongated while enhancing both contacts and knottedness propensities. As for multichain properties, we show that ring-ring contacts decrease with the confinement, yet neighboring rings overlap more as confinement grows. These aspects are accompanied by a marked decrease in the links formed between pairs of neighboring rings. In connection with the quantitative relation between links and entanglements in polymer melts recently established by us [Ubertini M. A.; Rosa A.Macromolecules2023, 56, 3354-3362], we propose that confinement can be used to set polymer networks that act softer under mechanical stress and suggest a viable experimental setup to validate our results.
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Project description:The relationship between polymer topology and bulk rheology remains a key question in soft matter physics. Architecture-specific constraints (or threadings) are thought to control the dynamics of ring polymers in ring-linear blends, which thus affects the viscosity to range between that of the pure rings and a value larger, but still comparable to, that of the pure linear melt. Here we consider qualitatively different systems of linear and ring polymers, fused together in "chimeric" architectures. The simplest example of this family is a "tadpole"-shaped polymer, a single ring fused to the end of a single linear chain. We show that polymers with this architecture display a threading-induced dynamical transition that substantially slows chain relaxation. Our findings shed light on how threadings control dynamics and may inform design principles for chimeric polymers with topologically tunable bulk rheological properties.
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