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000843966 1001_ $$00000-0002-7802-9407$$aKeidel, Rico$$b0$$eCorresponding author
000843966 245__ $$aTime-resolved structural evolution during the collapse of responsive hydrogels: The microgel-to-particle transition
000843966 260__ $$aWashington, DC [u.a.]$$bAssoc.$$c2018
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000843966 520__ $$aAdaptive hydrogels, often termed smart materials, are macromolecules whose structure adjusts to external stimuli. Responsive micro- and nanogels are particularly interesting because the small length scale enables very fast response times. Chemical cross-links provide topological constraints and define the three-dimensional structure of the microgels, whereas their porous structure permits fast mass transfer, enabling very rapid structural adaption of the microgel to the environment. The change of microgel structure involves a unique transition from a flexible, swollen finite-size macromolecular network, characterized by a fuzzy surface, to a colloidal particle with homogeneous density and a sharp surface. In this contribution, we determine, for the first time, the structural evolution during the microgel-to-particle transition. Time-resolved small-angle x-ray scattering experiments and computer simulations unambiguously reveal a two-stage process: In a first, very fast process, collapsed clusters form at the periphery, leading to an intermediate, hollowish core-shell structure that slowly transforms to a globule. This structural evolution is independent of the type of stimulus and thus applies to instantaneous transitions as in a temperature jump or to slower stimuli that rely on the uptake of active molecules from and/or exchange with the environment. The fast transitions of size and shape provide unique opportunities for various applications as, for example, in uptake and release, catalysis, or sensing.
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000843966 7001_ $$0P:(DE-Juel1)164360$$aGhavami, Ali$$b1
000843966 7001_ $$00000-0002-7539-3916$$aLugo, Dersy M.$$b2
000843966 7001_ $$00000-0001-7995-2693$$aLotze, Gudrun$$b3
000843966 7001_ $$0P:(DE-HGF)0$$aVirtanen, Otto$$b4
000843966 7001_ $$00000-0002-1012-3835$$aBeumers, Peter$$b5
000843966 7001_ $$00000-0002-7768-0206$$aPedersen, Jan Skov$$b6
000843966 7001_ $$0P:(DE-Juel1)172023$$aBardow, Andre$$b7
000843966 7001_ $$0P:(DE-Juel1)131039$$aWinkler, Roland G.$$b8$$eCorresponding author
000843966 7001_ $$0P:(DE-Juel1)IHRS-BioSoft-140012$$aRichtering, Walter$$b9$$eCorresponding author
000843966 773__ $$0PERI:(DE-600)2810933-8$$a10.1126/sciadv.aao7086$$gVol. 4, no. 4, p. eaao7086 -$$n4$$peaao7086$$tScience advances$$v4$$x2375-2548$$y2018
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