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In concentrated solutions, bridged and interpenetrated nanocylinders emerge with distinct structure and rheology, featuring reentrant melting and enhanced elasticity and yield stress.",{"@graph":14,"@context":73},[15,34,56],{"@type":16,"itemListElement":17},"BreadcrumbList",[18,23,27,31],{"item":19,"name":20,"@type":21,"position":22},"https://docshare.wps.com","Home","ListItem",1,{"item":24,"name":25,"@type":21,"position":26},"https://docshare.wps.com/document/","Document",2,{"item":28,"name":29,"@type":21,"position":30},"https://docshare.wps.com/document/research-report/","Research & 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Nanocylinders from Self-Assembled Star Block Copolymers  \nEsmaeel Moghimi, Iurii Chubak, Konstantinos Ntetsikas, Georgios Polymeropoulos, Xin Wang, Consiglia Carillo, Antonia Statt, Luca Cipelletti, Kell Mortensen, Nikos Hadjichristidis, Athanassios Z. Panagiotopoulos, Christos N. Likos, and Dimitris Vlassopoulos *  \n Cite This: Macromolecules 2024, 57, 926−939  \nRead Online  \nDownloaded via COPENHAGEN UNIV LIBRARY on February 24, 2024 at 10:17:03 (UTC) . See [https://pubs.acs.org/sharingguidelines](https://pubs.acs.org/sharingguidelines) for options on how to legitimately share published articles.  \nACCESS  \n Metrics & More  \n Article Recommendations  \n*sı   \nSupporting Information  \nABSTRACT: The design of functional polymeric materials with tunable response requires a synergetic use of macromolecular architecture and interactions. Here, we combine experiments with computer simulations to demonstrate how physical properties of gels can be tailored at the molecular level, using star block copolymers with alternating block sequences as a paradigm. Telechelic star polymers containing attractive outer blocks self-assemble into soft patchy nanoparticles, whereas their mirror-image inverted architecture with inner attractive blocks yields micelles. In concentrated solutions, bridged and interpenetrated hexagonally packed nanocylinders are formed, respectively, with distinct structural and rheological properties. The phase diagrams exhibit a peculiar reentrance where the hexagonal phase melts upon both heating and cooling because of solvent−block and block−block interactions. The bridged nanostructure is characterized by similar deformability, extended structural coherence, enhanced elasticity, and yield stress compared to micelles or typical colloidal gels, which make them promising and versatile materials for diverse applications.  \nI. INTRODUCTION  \nHierarchical self-assembly, the fundamental mechanism to form reversible multiscale material structures, is ubiquitous in modern technology since the properties of new products depend on the type of building blocks.1 Introducing directional interactions to building blocks via patchiness greatly enriches the realm of possibilities in material science.1,2 The anisotropic nature of patchy interactions limits the number of valences that each particle can have, which allows the formation of lowdensity gels,3 open crystals,4,5 and cluster phases.6,7 DNAcoated colloidal particles are one popular example of such soft patchy building blocks. In such suspensions, colloidal particles aggregate when the temperature is reduced below a certain system-dependent value as a result of interparticle binding.8−14 An appropriate deposition (or programming) of DNA-coated particles allows for the coupling of inter- and intraparticle binding.15 The fine-tuning of such competing interactions can lead to complex self-assembled structures with rich phase behavior characterized by colloidal crystallization 15 or gelation16, 17 on cooling, followed by re-entrant melting on  \nfurther cooling. However, DNA technology is often complex, and among the many outstanding challenges for applications, combining simplicity, versatility, and responsiveness stands out. 18, 19 Moreover, introducing intraparticle associations requires complex grafting of DNA strands on binary mixtures of colloidal particles. A simpler way to introduce competitive interactions can be achieved by combining macromolecular architecture and enthalpic interactions and is implemented with a special class of star polymers, the telechelic star polymers (TSPs).20−22 TSPs are macromolecules made of fdiblock copolymers grafted on a central anchoring point. Each diblock arm has a fraction α of solvophobic (at the outside) and 1 − α of solvophilic monomers. The dual nature of their  \n\n| Received: October 11, 2023\u003Cbr>Revised: January 5, 2024\u003Cbr>Accepted: Januar","cbCaigmcIGAJFQo8","https://ap.wps.com/l/cbCaigmcIGAJFQo8","pdf",6943686,14,"English","# Abstract\n# I. Introduction","[{\"question\":\"What material system does the study focus on?\",\"answer\":\"The study focuses on self-assembled star block copolymers with alternating block sequences, using telechelic star polymers as a paradigm.\"},{\"question\":\"How do different star architectures affect the assembled structures?\",\"answer\":\"Telechelic stars with attractive outer blocks self-assemble into soft patchy nanoparticles, while inverted architectures with inner attractive blocks yield micelles.\"},{\"question\":\"What happens in concentrated solutions and how is it characterized?\",\"answer\":\"Concentrated solutions form bridged and interpenetrated hexagonally packed nanocylinders with distinct structural and rheological properties, including a reentrance where the hexagonal phase melts on heating and cooling.\"}]","Interpenetrated and Bridged Nanocylinders from Self-Assembled Star Block Copolymers | PDF",1790001713,35]