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000014581 084__ $$2WoS$$aChemistry, Physical
000014581 084__ $$2WoS$$aMaterials Science, Multidisciplinary
000014581 084__ $$2WoS$$aPhysics, Multidisciplinary
000014581 084__ $$2WoS$$aPolymer Science
000014581 1001_ $$0P:(DE-HGF)0$$aLund, R.$$b0
000014581 245__ $$aStructural and thermodynamic aspects of the cylinder-to-sphere transition in amphiphilic diblock copolymer micelles
000014581 260__ $$aCambridge$$bRoyal Society of Chemistry (RSC)$$c2011
000014581 300__ $$a1491 - 1500
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000014581 440_0 $$016881$$aSoft Matter$$v7$$x1744-683X$$y4
000014581 500__ $$aThe authors acknowledge the University of the Basque Country and Basque Country Government (Ref. No. IT-436-07, Depto. Educacion, Universidades e InvestigacionS, and iNANOGUNE research project within Etortek program) and the Spanish Minister of Education (Grant No. MAT 2007-63681) for their support. The support of the European Community within the SOFTCOMP Network of Excellence (NoE) program is also gratefully acknowledged.
000014581 520__ $$aThe structure of diblock copolymers micelles depends on a delicate balance of thermodynamic forces driving the system towards equilibrium and kinetic factors which limit the systems' exploration of the phase space. The factors governing the morphological transition between cylindrical and spherical micelles are related to a fine balance between entropic forces from chains within the micellar core and corona. In order to understand and control these structures, it is important to gain insight into the fundamental thermodynamic driving forces governing the structure and answer fundamental questions concerning its equilibrium nature. In this work we aim to understand the relationship between thermodynamics and morphological transitions by investigating the detailed structure of a system undergoing a cylinder-to-sphere transition. We focus on the structural properties of micelles constituted of poly(ethylene-alt-propylene)-poly(ethylene oxide) (PEP1-PEO1, the numbers indicate the molar mass in kg/mole) diblock copolymers in dimethylformamide (DMF)/water solvent mixtures. This system is ideal for fundamental studies as it represents a classical well-segregated block copolymer micelle system where the interfacial tension can be controlled in detail without significantly changing other thermodynamic properties. Using small-angle neutron scattering (SANS) it is shown that the system undergoes a cylinder-to-sphere transition upon addition of DMF which lowers the interfacial tension. By applying a detailed thermodynamic model we show that both the dependence of the structural parameters with the interfacial tension as well as the morphological transition can be quantitatively understood. The transition itself is governed by the interfacial tension which dictates the stretching of chains within both corona and core. At high interfacial tensions (in water-rich solutions) discrepancies between structural data and predictions from the thermodynamic model are observed. A qualitative comparison with some preliminary results on the chain exchange kinetics in the system show that these deviations coincide with the region where this equilibration mechanism is not active, i.e. when the kinetics are frozen at high interfacial tensions.
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000014581 7001_ $$0P:(DE-Juel1)VDB4339$$aPipich, V.$$b1$$uFZJ
000014581 7001_ $$0P:(DE-HGF)0$$aWillner, L.$$b2
000014581 7001_ $$0P:(DE-Juel1)VDB4342$$aRadulescu, A.$$b3$$uFZJ
000014581 7001_ $$0P:(DE-HGF)0$$aColmenero, J.$$b4
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000014581 773__ $$0PERI:(DE-600)2191476-X$$a10.1039/c0sm00894j$$gVol. 7, p. 1491 - 1500$$p1491 - 1500$$q7<1491 - 1500$$tSoft matter$$v7$$x1744-683X$$y2011
000014581 8567_ $$uhttp://dx.doi.org/10.1039/C0SM00894J
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