期刊
JOURNAL OF CHEMICAL PHYSICS
卷 142, 期 2, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4905670
关键词
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资金
- Gates Cambridge Trust
- National Science Foundation Graduate Research Fellowship [DGE-1143678]
- European Research Council [227758]
- Engineering and Physical Sciences Research Council [EP/I001352/1]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- Engineering and Physical Sciences Research Council [EP/I001352/1, EP/I000844/1] Funding Source: researchfish
- EPSRC [EP/I001352/1, EP/I000844/1] Funding Source: UKRI
We present a technique for calculating free-energy profiles for the nucleation of multicomponent structures that contain as many species as building blocks. We find that a key factor is the topology of the graph describing the connectivity of the target assembly. By considering the designed interactions separately from weaker, incidental interactions, our approach yields predictions for the equilibrium yield and nucleation barriers. These predictions are in good agreement with corresponding Monte Carlo simulations. We show that a few fundamental properties of the connectivity graph determine the most prominent features of the assembly thermodynamics. Surprisingly, we find that polydispersity in the strengths of the designed interactions stabilizes intermediate structures and can be used to sculpt the free-energy landscape for self-assembly. Finally, we demonstrate that weak incidental interactions can preclude assembly at equilibrium due to the combinatorial possibilities for incorrect association. (C) 2015 AIP Publishing LLC.
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