Simultaneous optimization of assembly time and yield in programmable self-assembly

Abstract

Rational design strategies for self-assembly require a detailed understanding of both the equilibrium state and the assembly kinetics. While the former is starting to be well understood, the latter remains a major theoretical challenge, especially in programmable systems and the so-called semiaddressable regime, where binding is often nondeterministic and the formation of off-target structures negatively influences the assembly. Here, we show that it is possible to simultaneously sculpt the assembly outcome and the assembly kinetics through the underexplored design space of binding energies and particle concentrations. By formulating the assembly process as a complex reaction network, we calculate and optimize the tradeoff between assembly speed and quality, and show that parameter optimization can speed up assembly by many orders of magnitude without lowering the yield of the target structure. Although the exact speedup varies from design to design, we find the largest speedups for nondeterministic systems where unoptimized assembly is the slowest, sometimes even making them assemble faster than optimized fully-addressable designs. Therefore, these results not only solve a key challenge in semiaddressable self-assembly, but further emphasize the utility of semiaddressability, where designs have the potential to be faster as well as cheaper (fewer particle species) and better (higher yield). More broadly, our results highlight the importance of parameter optimization in programmable self-assembly, and provide practical tools for simultaneous optimization of kinetics and yield in a wide range of systems.

References in corpus (15)

• The Statistical Mechanics of Dynamic Pathways to Self-assembly
• Equilibrium mechanisms of self-limiting assembly
• Mechanisms of kinetic trapping in self-assembly and phase transformation
• Multifarious Assembly Mixtures: Systems Allowing Retrieval of Diverse Stored Structures
• Brownian motion and the hydrodynamic friction tensor for colloidal particles of complex shape
• Geometrically programmed self-limited assembly of tubules using DNA origami colloids
• Designing patchy interactions to self-assemble arbitrary structures
• Designing the self-assembly of arbitrary shapes using minimal complexity building blocks
• The Information Capacity of Specific Interactions
• Hierarchical assembly may be a way to make large information-rich structures
• Economical routes to size-specific assembly of self-closing structures
• Physical interpretation of the partition function for colloidal clusters
• Close-to-equilibrium behaviour of quadratic reaction-diffusion systems with detailed balance
• Accessing Semi-Addressable Self Assembly with Efficient Structure Enumeration
• The polyhedral structure underlying programmable self-assembly