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Simon, Anna J.; Walls-Smith, Luke T.; Fredd, Matthew J.; Fong, Yi Fong; Gubala, Vladimir; Plaxco, Kevin W. (2016)
Publisher: American Chemical Society
Languages: English
Types: Article
Subjects: QD431, QD473
Recent years have seen increasing study of stimulus-responsive hydrogels constructed from aptamer-connected DNA building blocks. Presumably due to a lack of simple, quantitative tools with which to measure gel responsiveness, however, the literature describing these materials is largely qualitative. In response we demonstrate here simple, time-resolved, multiscale methods for measuring the response kinetics of these materials. Specifically, by employing trace amounts of fluorophore-quencher labeled crosslinkers and the rheology of entrapped fluorescent particles we simultaneously measure dissolution at molecular, hundred-nanometer, and hundred-micron length-scales. For our test-bed system, an adenine-responsive hydrogel, we find biphasic response kinetics dependent on both effector concentration and depth within the gel and a dissolution pattern uniform at scales longer than a few times the monomer-monomer distance. Likewise, we find that, in agreement with theoretical predictions, dissolution kinetics over the hundred nanometer length scale exhibit a power-law-like dependence on the fraction of disrupted crosslinks before a distinct crossover from solid-like to liquid-like behavior
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