Abstract
The possibility of prescribing local interactions between nano- and microscopic components that direct them to assemble in a predictable fashion is a central goal of nanotechnology research. In this article, we advance a new paradigm in which the self-assembly of DNA-functionalized colloidal particles is programmed using linker oligonucleotides dispersed in solution. We find a phase diagram that is surprisingly rich compared to phase diagrams typical of other DNA-functionalized colloidal particles that interact by direct hybridization, including a reentrant melting transition upon increasing linker concentration, and show that multiple linker species can be combined to prescribe many interactions simultaneously. A new theory predicts the observed phase behavior quantitatively without any fitting parameters. Taken together, these experiments and model lay the groundwork for future research in programmable self-assembly, enabling the possibility of programming the hundreds of specific interactions needed to assemble fully addressable, mesoscopic structures, while also expanding our fundamental understanding of the unique phase behavior possible in colloidal suspensions.Received 14 March 2019Revised 13 August 2019DOI:https://doi.org/10.1103/PhysRevX.9.041054Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasClassical statistical mechanicsPhase behaviorPhase diagramsSelf-assemblyPhysical SystemsColloidsDNAStatistical PhysicsCondensed Matter, Materials & Applied PhysicsPolymers & Soft Matter
Highlights
DNA-coated colloids are one of the most promising systems for designing complex self-assembling materials [1,2,3]
We find a phase diagram that is surprisingly rich compared to phase diagrams typical of other DNA-functionalized colloidal particles that interact by direct hybridization, including a reentrant melting transition upon increasing linker concentration, and show that multiple linker species can be combined to prescribe many interactions simultaneously
Our experiments reveal a rich phase diagram containing two previously unknown regions: (1) a reentrant melting transition that occurs upon increasing linker concentration and (2) a linker concentration at which coexistence between gas and solid is stable over a wide range of temperatures
Summary
DNA-coated colloids are one of the most promising systems for designing complex self-assembling materials [1,2,3]. DNA can encode these hundreds of interactions through careful design of the base sequences [10,11] This potential is nearly impossible to realize in systems of DNA-coated particles interacting through direct binding of their grafted strands: The steep temperature dependence of the interactions [12,13,14], the inherent uncertainty in predictions of the binding affinities [15], and the inability to tune the relative interactions without resynthesizing the particles [16] make matching hundreds of unique interactions intractable. We combine experiments and theory to explore the interactions and phase behavior that emerge when binding between DNA-grafted colloidal particles is encoded in soluble linker molecules. The combination of our experimental findings and new approaches to modeling shows that we can predict and program the interactions required to direct assembly of prescribed aperiodic structures
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