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Although the assemblies formed by these peptide systems do not satisfy the assumption that particles should be spherical, we ran dynamic light scattering experiments to see the relative changes in particle sizes upon switching the pH and that the formation of peptide assemblies is supported even in the OPV3-4T mixtures (ESI, Fig. S8 and 9†). We have observed a dispersed distribution of sizes for basic solutions, which are consistently smaller than all the observed sizes for acidic solutions. This then supports the predominance of essentially dissolved structures in basic conditions, and the favored formation of assemblies under acidic conditions.
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The extreme pH conditions used (pH 2 and 10) were chosen to ensure that the majority of the OPV3 and/or 4T units are in their dissolved or self-assembled states but are not absolutely necessary to regulate the molecular-tonanostructure switch under the spectroscopic conditions employed here. No gelation was observed under such spectroscopic conditions, but gelation was observed for pure OPV3 and 9 mol% 4T at 1 wt% solutions.
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