Enhancing
DNA-Mediated Assemblies of Supramolecular
Cage Dimers through Tuning Core Flexibility and DNA LengthA
Combined Experimental–Modeling Study
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Abstract
Two complementary
small-molecule–DNA hybrid (SMDH) building
blocks have been combined to form well-defined supramolecular cage
dimers at DNA concentrations as high as 102 μM. This was made
possible by combining a flexible small-molecule core and three DNA
arms of moderate lengths (<20 base pairs). These results were successfully
modeled by coarse-grained molecular dynamics simulations, which also
revealed that the formation of ill-defined networks in the case of
longer DNA arms can be significantly biased by the presence of deep
kinetic traps. Notably, melting point studies revealed that cooperative
melting behavior can be used as a means to distinguish the relative
propensities for dimer versus network formation from complementary
flexible three-DNA-arm SMDH (fSMDH<sub>3</sub>) components: sharp,
enhanced melting transitions were observed for assemblies that result
mostly in cage dimers, while no cooperative melting behavior was observed
for assemblies that form ill-defined networks