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DNA nanostructures with programmable shape and interactions can be used asbuilding blocks for the self-assembly of crystalline materials with prescribednanoscale features, holding a vast technological potential. Structural rigidityand bond directionality have been recognised as key design features for DNAmotifs to sustain long-range order in 3D, but the practical challengesassociated with prescribing building-block geometry with sufficient accuracyhave limited the variety of available designs. We have recently introduced anovel platform for the one-pot preparation of crystalline DNA frameworkssupported by a combination of Watson-Crick base pairing and hydrophobic forces[Nano Lett., 17(5):3276-3281, 2017]. Here we use small angle X-ray scatteringand coarse-grained molecular simulations to demonstrate that, as opposed toavailable all- DNA approaches, amphiphilic motifs do not rely on structuralrigidity to support long-range order. Instead, the flexibility of amphiphilicDNA building-blocks is a crucial feature for successful crystallisation.

Flexibility defines structure in crystals of amphiphilic DNA nanostars