Spatio-temporal heterogeneities in nanosegregated single-molecule polymeric nanoparticles

Bačová, Petra; Glynos, Emmanouil; Anastasiadis, Spiros H.; Harmandaris, Vagelis

doi:10.1039/d0sm00079e

Cited by 7 publications

(4 citation statements)

References 34 publications

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“…[44] Identical structure of the kernel was used before in the simulations of mikto-arm stars. [38][39][40] In Figure 1, we present a schematic illustration of the kernels for f = 8 and f = 32. The kernel is composed of carbon units which we consider as united atoms.…”

Section: Modelmentioning

confidence: 99%

“…The initial configuration of the star was created by attaching fully stretched arms to the kernel under a certain angle, minimizing the overlap of the atoms, following the protocol reported for mikto-arm stars model systems. [38][39][40] Then, a series of energy minimization (EM) runs together with very short MD simulations with a reduced time step (of 0.1 fs) were performed to eliminate overlaps. The bonds were constrained during the EM by the LINCS [48] algorithm, to avoid bond stretching.…”

Section: Modelmentioning

confidence: 99%

“…As showed in our previous studies on mikto-arm stars, the PS arms with their bulky groups occupy much bigger volume around the star core than the PEO arms, being thus adequate examples of two model polymers with distinct properties. [38][39][40] Both types of stars have been also studied experimentally. [41,42] With our realistic model, we aim to bridge the gap between the general, bead-spring type coarse-grained polymer models and experimentally relevant specific polymer star-like structures.…”

Section: Introductionmentioning

confidence: 99%

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Size and Shape Characteristics of Polystyrene and Poly(ethylene oxide) Star Polymer Melts Studied By Atomistic Simulations

Gkolfi

Bačová

Harmandaris

2020

Macro Theory & Simulations

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Here, atomistic molecular dynamics simulations are used to address the effect of different chemistry on the morphology, size, and shape characteristics of star polymers. The role of chemical details and features such as packing or flexibility on the structural properties of star‐like polymer melts is probed. Two types of symmetric unentangled homopolymer stars, the first consisting of atactic polystyrene (PS) and the second one of poly(ethylene oxide) (PEO) are studied. The star functionality f (i.e., the number of arms) is varied from f = 1 (linear chains) up to f = 32 and the shape and size characteristics are reported as a function of this main variable. The results from the monodisperse star‐like polymers are confronted with the theoretical predictions and with previously published simulations studies employing generic bead‐spring coarse‐grained models, with the aim to fill the gap between the systems studied experimentally and computationally.

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Section: Modelmentioning

confidence: 99%

Section: Modelmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Size and Shape Characteristics of Polystyrene and Poly(ethylene oxide) Star Polymer Melts Studied By Atomistic Simulations

Gkolfi

Bačová

Harmandaris

2020

Macro Theory & Simulations

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“…We followed a multi-stage equilibration protocol for the preparation of the stars, which has been used in previous atomistic simulation studies of mikto-arm stars. [35,64,65] In brief, first, we attached fully stretched arms to the atoms of the last generation of the kernel and run short runs to avoid overlaps and minimize the energy of the artificially created initial configuration. Second, when the initial single-star configuration was ready, N S stars were inserted randomly into a simulation box and equilibrated with a sequence of heating and equilibration runs.…”

Section: Simulation Detailsmentioning

confidence: 99%

Dynamical heterogeneities in non-entangled polystyrene and poly(ethylene oxide) star melts

Bačová,

Gkolfi,

Hawke

et al. 2020

Preprint

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The following article has been accepted by Physics of Fluids. After it is published, it will be found at: https://publishing.aip.org/resources/librarians/products/journals/.Star polymers can exhibit a heterogeneous dynamical behavior due to their internal structure. In this work we employ atomistic molecular dynamics simulations to study translational motion in non-entangled polystyrene and poly(ethylene oxide) star-shaped melts. We focus on the local heterogeneous dynamics originating from the multi-arm star-like architecture and quantify the intramolecular dynamical gradient. By examining the translational motion at length scales of the order of the Kuhn length, we aim to find common features for both studied chemistries and to provide a critical and direct comparison with theoretical models of polymer dynamics. We discuss the observed tendencies with respect to the continuous Rouse model adjusted for the star-like architectures. Two versions of the Rouse model are examined: one assuming uniform friction on every Rouse bead and another one considering larger branch point friction. Apart from chain connectivity between neighboring beads, both versions disregard interactions between the chains. Despite the tolerable description of the simulation data, neither model appears to reflect the mobility gradient accurately. The detailed quantitative atomistic models employed here bridge the gap between the theoretical and general, coarse-granined models of star-like polymers which lack the indispensable chemical details.

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Trifaceted Mickey Mouse Amphiphiles for Programmable Self‐Assembly, DNA Complexation and Organ‐Selective Gene Delivery

Carbajo-Gordillo

González-Cuesta

Blanco

et al. 2021

Chemistry A European J

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Instilling segregated cationic and lipophilic domains with an angular disposition in a trehalose-based trifaceted macrocyclic scaffold allows engineering patchy molecular nanoparticles leveraging directional interactions that emulate those controlling self-assembling processes in viral capsids. The resulting trilobular amphiphilic derivatives, featuring a Mickey Mouse architecture, can electrostatically interact with plasmid DNA (pDNA) and further engage in hydrophobic contacts to promote condensation into transfectious nanocomplexes. Notably, the topology and internal structure of the cyclooligosaccharide/pDNA co-assemblies can be molded by fine-tuning the valency and characteristics of the cationic and lipophilic patches, which strongly impacts the transfection efficacy in vitro and in vivo. Outstanding organ selectivities can then be programmed with no need of incorporating a biorecognizable motif in the formulation. The results provide a versatile strategy for the construction of fully synthetic and perfectly monodisperse nonviral gene delivery systems uniquely suited for optimization schemes by making cyclooligosaccharide patchiness the focus.

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Spatio-temporal heterogeneities in nanosegregated single-molecule polymeric nanoparticles

Abstract: Nanoparticles with nanosegregated, dynamically heterogeneous domains can be designed by combining incompatible dynamically asymmetric polymers of different glass transition temperature in a mikto-arm architecture.

Cited by 7 publications

References 34 publications

Size and Shape Characteristics of Polystyrene and Poly(ethylene oxide) Star Polymer Melts Studied By Atomistic Simulations

Size and Shape Characteristics of Polystyrene and Poly(ethylene oxide) Star Polymer Melts Studied By Atomistic Simulations

Dynamical heterogeneities in non-entangled polystyrene and poly(ethylene oxide) star melts

Trifaceted Mickey Mouse Amphiphiles for Programmable Self‐Assembly, DNA Complexation and Organ‐Selective Gene Delivery

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