Journal
NATURE
Volume 610, Issue 7932, Pages -Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41586-022-05198-8
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Funding
- Paris Region (Region Ile-de-France) under the Blaise Pascal International Chairs of Excellence
- MRSEC programme of the National Science Foundation [NSF DMR-1420073, NSF PHY17-48958, NSF DMR-1710163]
- European Union [754387]
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By programming the interactions of colloidal droplet chains, specific geometric structures can be achieved through self-folding.
In the realm of particle self-assembly, it is possible to reliably construct nearly arbitrary structures if all the pieces are distinct(1-3), but systems with fewer flavours of building blocks have so far been limited to the assembly of exotic crystals(4-6). Here we introduce a minimal model system of colloidal droplet chains(7), with programmable DNA interactions that guide their downhill folding into specific geometries. Droplets are observed in real space and time, unravelling the rules of folding. Combining experiments, simulations and theory, we show that controlling the order in which interactions are switched on directs folding into unique structures, which we call colloidal foldamers(8). The simplest alternating sequences (ABAB...) of up to 13 droplets yield 11 foldamers in two dimensions and one in three dimensions. Optimizing the droplet sequence and adding an extra flavour uniquely encodes more than half of the 619 possible two-dimensional geometries. Foldamers consisting of at least 13 droplets exhibit open structures with holes, offering porous design. Numerical simulations show that foldamers can further interact to make complex supracolloidal architectures, such as dimers, ribbons and mosaics. Our results are independent of the dynamics and therefore apply to polymeric materials with hierarchical interactions on all length scales, from organic molecules all the way to Rubik's Snakes. This toolbox enables the encoding of large-scale design into sequences of short polymers, placing folding at the forefront of materials self-assembly.
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