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      Use of complementary nucleobase-containing synthetic polymers to prepare complex self-assembled morphologies in water†

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          Abstract

          Amphiphilic block copolymers with synthetic nucleobase-containing blocks as the hydrophobic segments were successfully synthesized using RAFT polymerisation and then self-assembled via solvent switch in aqueous solutions.

          Abstract

          Amphiphilic nucleobase-containing block copolymers with poly(oligo(ethylene glycol) methyl ether methacrylate) as the hydrophilic block and nucleobase-containing blocks as the hydrophobic segments were successfully synthesized using RAFT polymerization and then self-assembled via solvent switch in aqueous solutions. Effects of the common solvent on the resultant morphologies of the adenine (A) and thymine (T) homopolymers, and A/T copolymer blocks and blends were investigated. These studies highlighted that depending on the identity of the common solvent, DMF or DMSO, spherical micelles or bicontinuous micelles were obtained. We propose that this is due to the presence of A–T interactions playing a key role in the morphology and stability of the resultant nanoparticles, which resulted in a distinct system compared to individual adenine or thymine polymers. Finally, the effects of annealing on the self-assemblies were explored. It was found that annealing could lead to better-defined spherical micelles and induce a morphology transition from bicontinuous micelles to onion-like vesicles, which was considered to occur due to a structural rearrangement of complementary nucleobase interactions resulting from the annealing process.

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          Most cited references 48

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          Simple analytical expression for the peak-frequency shifts of plasmonic resonances for sensing

          We derive a closed-form expression that accurately predicts the peak frequency-shift and broadening induced by tiny perturbations of plasmonic nanoresonators without critically relying on repeated electrodynamic simulations of the spectral response of nanoresonator for various locations, sizes or shapes of the perturbing objects. The force of the present approach, in comparison with other approaches of the same kind, is that the derivation is supported by a mathematical formalism based on a rigorous normalization of the resonance modes of nanoresonators consisting of lossy and dispersive materials. Accordingly, accurate predictions are obtained for a large range of nanoparticle shapes and sizes, used in various plasmonic nanosensors, even beyond the quasistatic limit. The expression gives quantitative insight, and combined with an open-source code, provides accurate and fast predictions that are ideally suited for preliminary designs or for interpretation of experimental data. It is also valid for photonic resonators with large mode volumes.
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            Toroidal triblock copolymer assemblies.

            A stable phase of toroidal, or ringlike, supramolecular assemblies was formed by combining dilute solution characteristics critical for both bundling of like-charged biopolymers and block copolymer micelle formation. The key to toroid versus classic cylinder micelle formation is the interaction of the negatively charged hydrophilic block of an amphiphilic triblock copolymer with a positively charged divalent organic counterion. This produces a self-attraction of cylindrical micelles that leads to toroid formation, a mechanism akin to the toroidal bundling of semiflexible charged biopolymers such as DNA. The toroids can be kinetically trapped or chemically cross-linked. Insight into the mechanism of toroid formation can be gained by observation of intermediate structures kinetically trapped during film casting.
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              PASCal: A principal-axis strain calculator for thermal expansion and compressibility determination

              We describe a web-based tool (PASCal; Principal Axis Strain Calculator) aimed at simplifying the determination of principal coefficients of thermal expansion and compressibilities from variable-temperature and variable-pressure lattice parameter data. In a series of three case studies, we use PASCal to re-analyse previously-published lattice parameter data and show that additional scientific insight is obtainable in each case. First, the two-dimensional metal-organic framework Cu-SIP-3 is found to exhibit the strongest area-negative thermal expansion (NTE) effect yet observed; second, the widely-used explosive HMX exhibits much stronger mechanical anisotropy than had previously been anticipated, including uniaxial NTE driven by thermal changes in molecular conformation; and, third, the high-pressure form of the mineral malayaite is shown to exhibit a strong negative linear compressibility (NLC) effect that arises from correlated tilting of SnO6 and SiO4 coordination polyhedra.
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                Author and article information

                Journal
                Polym Chem
                Polym Chem
                Polymer Chemistry
                Royal Society of Chemistry
                1759-9954
                1759-9962
                28 April 2016
                6 April 2016
                : 7
                : 16
                : 2836-2846
                Affiliations
                [a ] Department of Chemistry , University of Warwick , Gibbet Hill Road , Coventry , CV4 7AL , UK . Email: Rachel.OReilly@ 123456warwick.ac.uk
                [b ] School of Life Sciences , University of Warwick , Gibbet Hill Road , Coventry , CV4 7AL , UK
                [c ] Australian Synchrotron , 800 Blackburn Road , Clayton Vic 3168 , Australia
                Article
                c6py00263c
                10.1039/c6py00263c
                4894073
                27358655
                3879ebf0-99b1-4846-9d7e-5e1977013994
                This journal is © The Royal Society of Chemistry 2016

                This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License ( http://creativecommons.org/licenses/by-nc/2.0/uk/) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.

                Categories
                Chemistry

                Notes

                †Electronic supplementary information (ESI) available: Characterization of monomers, polymers and particles: NMR, SEC, TEM, SAXS, and DLS. See DOI: 10.1039/c6py00263c

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