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1.
Phys Rev E ; 100(2-1): 022501, 2019 Aug.
Article in English | MEDLINE | ID: mdl-31574720

ABSTRACT

We study the relaxation dynamics of the polymer networks that are constructed based on a degree distribution specific to small-world networks. The employed building algorithm generates polymers with a large variety of architectures, thus allowing for a detailed study of the structural transition from a pure linear chain to dendritic polymer networks. This is done by varying a single parameter p, which measures the randomness in the degree of the network's nodes. The dynamics is investigated in the framework of the generalized Gaussian structures model by monitoring the influence of the parameter p and of the stiffness parameter q on the behavior of the relaxation quantities: averaged monomer displacement, storage modulus, and loss modulus. The structure properties of the constructed polymers are described by the mean-square radius of gyration. In the absence of stiffness, in the intermediate frequencies domain of the dynamical quantities we encounter different behaviours, such as a dendritic behavior followed by a linear one for very small values of p or a single well-marked dendritic behavior for higher values of p. The stiffness parameter q influences drastically the relaxation dynamics of these polymer networks and in general no evident scaling regions were encountered. However, for some values of the parameter set (p,q), such as (0.8,0.4), an extremely short constant slope region, less than one order of magnitude, was found.

2.
Sci Rep ; 8(1): 3731, 2018 Feb 27.
Article in English | MEDLINE | ID: mdl-29487316

ABSTRACT

We focus on treelike generalized scale-free polymer networks, whose geometries depend on a parameter, γ, that controls their connectivity and on two modularity parameters: the minimum allowed degree, K min , and the maximum allowed degree, K max . We monitor the influence of these parameters on the static and dynamic properties of the achieved generalized scale-free polymer networks. The relaxation dynamics is studied in the framework of generalized Gaussian structures model by employing the Rouse-type approach. The dynamical quantities on which we focus are the average monomer displacement under external forces and the mechanical relaxation moduli (storage and loss modulus), while for the static and structure properties of these networks we concentrate on the eigenvalue spectrum, diameter, and degree correlations. Depending on the values of network's parameters we were able to switch between distinct hyperbranched structures: networks with more linearlike segments or with a predominant star or dendrimerlike topology. We have observed a stronger influence on K min than on K max . In the intermediate time (frequency) domain, all physical quantities obey power-laws for polymer networks with γ = 2.5 and K min = 2 and we prove additionally that for networks with γ ≥ 2.5 new regions with constant slope emerge by a proper choice of K min . Remarkably, we show that for certain values of the parameter set one may obtain self-similar networks.

3.
Polymers (Basel) ; 10(2)2018 Feb 08.
Article in English | MEDLINE | ID: mdl-30966200

ABSTRACT

In this paper, we focus on the mechanical relaxation of a multilayer polymer network built by connecting identical layers that have, as underlying topologies, the dual Sierpinski gasket and the regular dendrimer. Additionally, we analyze the dynamics of dipolar energy transfer over a system of chromophores arranged in the form of a multilayer network. Both dynamical processes are studied in the framework of the generalized Gaussian structure (GSS) model. We develop a method whereby the whole eigenvalue spectrum of the connectivity matrix of the multilayer network can be determined iteratively, thereby rendering possible the analysis of the dynamics of networks consisting of a large number of layers. This fact allows us to study in detail the crossover from layer-like behavior to chain-like behavior. Remarkably, we highlight the existence of two bulk-like behaviors. The theoretical findings with respect to the decomposition of the intermediate domain of the relaxation quantities, as well as the chain-like behavior, are well supported by experimental results.

4.
Polymers (Basel) ; 10(7)2018 Jul 18.
Article in English | MEDLINE | ID: mdl-30960712

ABSTRACT

In this paper, we focus on the relaxation dynamics of a polymer network modeled by a fractal cactus. We perform our study in the framework of the generalized Gaussian structure model using both Rouse and Zimm approaches. By performing real-space renormalization transformations, we determine analytically the whole eigenvalue spectrum of the connectivity matrix, thereby rendering possible the analysis of the Rouse-dynamics at very large generations of the structure. The evaluation of the structural and dynamical properties of the fractal network in the Rouse type-approach reveals that they obey scaling and the dynamics is governed by the value of spectral dimension. In the Zimm-type approach, the relaxation quantities show a strong dependence on the strength of the hydrodynamic interaction. For low and medium hydrodynamic interactions, the relaxation quantities do not obey power law behavior, while for slightly larger interactions they do. Under strong hydrodynamic interactions, the storage modulus does not follow power law behavior and the average displacement of the monomer is very low. Remarkably, the theoretical findings with respect to scaling in the intermediate domain of the relaxation quantities are well supported by experimental results from the literature.

5.
J Chem Phys ; 146(3): 034902, 2017 Jan 21.
Article in English | MEDLINE | ID: mdl-28109236

ABSTRACT

In this work, we study the relaxation dynamics of a multihierarchical polymer network built by replicating the Vicsek fractal in dendrimer shape. The relaxation dynamics is investigated in the framework of the generalized Gaussian structure model by employing both Rouse and Zimm approaches. In the Rouse-type approach, we show the iterative procedure whereby the whole eigenvalue spectrum of the connectivity matrix of the multihierarchical structure can be obtained. Remarkably, the general picture that emerges from both approaches, even though we have a mixed growth algorithm, is that the obtained multihierarchical structure preserves the individual relaxation behaviors of its components. The theoretical findings with respect to the splitting of the intermediate domain of the relaxation quantities are well supported by experimental results.

6.
Polymers (Basel) ; 9(7)2017 Jun 24.
Article in English | MEDLINE | ID: mdl-30970922

ABSTRACT

In this paper we focus on the relaxation dynamics of a multihierarchical polymer network built through the replication of the dual Sierpinski gasket in the form of a regular dendrimer. The relaxation dynamics of this multihierarchical structure is investigated in the framework of the generalized Gaussian structure model using both Rouse and Zimm approaches. In the Rouse-type approach, we show a method whereby the whole eigenvalue spectrum of the connectivity matrix of the multihierarchical structure can be determined iteratively, thereby rendering possible the analysis of the Rouse-dynamics at very large generations. Remarkably, the general picture that emerges from both approaches, even though we have a mixed growth algorithm and the monomers interactions are taken into account specifically to the adopted approach, is that the multihierarchical structure preserves the individual relaxation behaviors of its constituent components. The theoretical findings with respect to the splitting of the intermediate domain of the relaxation quantities are well supported by experimental results.

7.
J Chem Phys ; 145(10): 104901, 2016 Sep 14.
Article in English | MEDLINE | ID: mdl-27634273

ABSTRACT

We focus on the relaxation dynamics of multilayer polymer structures having, as underlying topology, the Husimi cactus. The relaxation dynamics of the multilayer structures is investigated in the framework of generalized Gaussian structures model using both Rouse and Zimm approaches. In the Rouse type-approach, we determine analytically the complete eigenvalues spectrum and based on it we calculate the mechanical relaxation moduli (storage and loss modulus) and the average monomer displacement. First, we monitor these physical quantities for structures with a fixed generation number and we increase the number of layers, such that the linear topology will smoothly come into play. Second, we keep constant the size of the structures, varying simultaneously two parameters: the generation number of the main layer, G, and the number of layers, c. This fact allows us to study in detail the crossover from a pure Husimi cactus behavior to a predominately linear chain behavior. The most interesting situation is found when the two limiting topologies cancel each other. For this case, we encounter in the intermediate frequency/time domain regions of constant slope for different values of the parameter set (G, c) and we show that the number of layers follows an exponential-law of G. In the Zimm-type approach, which includes the hydrodynamic interactions, the quantities that describe the mechanical relaxation dynamics do not show scaling behavior as in the Rouse model, except the limiting case, namely, a very high number of layers and low generation number.

8.
J Chem Phys ; 145(21): 214901, 2016 Dec 07.
Article in English | MEDLINE | ID: mdl-28799361

ABSTRACT

In this paper, we focus on the relaxation dynamics of Sierpinski hexagon fractal polymer. The relaxation dynamics of this fractal polymer is investigated in the framework of the generalized Gaussian structure model using both Rouse and Zimm approaches. In the Rouse-type approach, by performing real-space renormalization transformations, we determine analytically the complete eigenvalue spectrum of the connectivity matrix. Based on the eigenvalues obtained through iterative algebraic relations we calculate the averaged monomer displacement and the mechanical relaxation moduli (storage modulus and loss modulus). The evaluation of the dynamical properties in the Rouse-type approach reveals that they obey scaling in the intermediate time/frequency domain. In the Zimm-type approach, which includes the hydrodynamic interactions, the relaxation quantities do not show scaling. The theoretical findings with respect to scaling in the intermediate domain of the relaxation quantities are well supported by experimental results.

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