Entropy Stabilizes Floppy Crystals of Mobile DNA-Coated Colloids
Ruiz, Pablo Sampedro
Date of Issue2018
School of Chemical and Biomedical Engineering
Grafting linkers with open ends of complementary single-stranded DNA makes a flexible tool to tune interactions between colloids, which facilitates the design of complex self-assembly structures. Recently, it has been proposed to coat colloids with mobile DNA linkers, which alleviates kinetic barriers without high-density grafting, and also allows the design of valency without patches. However, the self-assembly mechanism of this novel system is poorly understood. Using a combination of theory and simulation, we obtain phase diagrams for the system in both two and three dimensional spaces, and find stable floppy square and CsCl crystals when the binding strength is strong, even in the infinite binding strength limit. We demonstrate that these floppy phases are stabilized by vibrational entropy, and “floppy” modes play an important role in stabilizing the floppy phases for the infinite binding strength limit. This special entropic effect in the self-assembly of mobile DNA-coated colloids is very different from conventional molecular self-assembly, and it offers a new axis to help design novel functional materials using mobile DNA-coated colloids.
Physical Review Letters
© 2018 American Physical Society (APS). This paper was published in Physical Review Letters and is made available as an electronic reprint (preprint) with permission of American Physical Society (APS). The published version is available at: [http://dx.doi.org/10.1103/PhysRevLett.120.048003]. One print or electronic copy may be made for personal use only. Systematic or multiple reproduction, distribution to multiple locations via electronic or other means, duplication of any material in this paper for a fee or for commercial purposes, or modification of the content of the paper is prohibited and is subject to penalties under law.