期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2022
卷号：119
期号：4
DOI：10.1073/pnas.2116373119
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：Significance
An important limiting factor for self-assembly processes is the time it takes to assemble large structures with high yield. While equilibrium self-assembly systems slowly relax toward a state of minimal free energy, nonequilibrium systems offer various ways to control assembly processes and to optimize their time efficiency. We show that these different control scenarios can informatively be characterized by their time complexity, i.e., their scaling of the assembly time with the structure size, analogous to algorithms for computational problems. Especially for large structures, differences in the time complexity of the scenarios lead to strongly diverging time efficiencies. Most significantly, we show that by effectively regulating the supply of constituents, high resource and time efficiency can be achieved for self-assembly processes.
Time efficiency of self-assembly is crucial for many biological processes. Moreover, with the advances of nanotechnology, time efficiency in artificial self-assembly becomes ever more important. While structural determinants and the final assembly yield are increasingly well understood, kinetic aspects concerning the time efficiency, however, remain much more elusive. In computer science, the concept of time complexity is used to characterize the efficiency of an algorithm and describes how the algorithm’s runtime depends on the size of the input data. Here we characterize the time complexity of nonequilibrium self-assembly processes by exploring how the time required to realize a certain, substantial yield of a given target structure scales with its size. We identify distinct classes of assembly scenarios, i.e., “algorithms” to accomplish this task, and show that they exhibit drastically different degrees of complexity. Our analysis enables us to identify optimal control strategies for nonequilibrium self-assembly processes. Furthermore, we suggest an efficient irreversible scheme for the artificial self-assembly of nanostructures, which complements the state-of-the-art approach using reversible binding reactions and requires no fine-tuning of binding energies.
关键词：ennonequilibrium self-assemblytime efficiencytime complexityself-assembly scenariosupply control
