Niblo Jessica K, Swartley Jacob R, Zhang Zhongmin, DuBay Kateri H
Department of Chemistry, University of Virginia, McCormick Road, PO Box 400319, Charlottesville, VA 22903-4319, USA.
Department of Chemistry, University of North Carolina at Chapel Hill, Campus Box 3290, Chapel Hill, NC 27599-3290, USA.
Soft Matter. 2024 Aug 28;20(34):6702-6713. doi: 10.1039/d4sm00455h.
Multiple dissipative self-assembly protocols designed to create novel structures or to reduce kinetic traps have recently emerged. Specifically, temporal oscillations of particle interactions have been shown effective at both aims, but investigations thus far have focused on systems of simple colloids or their binary mixtures. In this work, we expand our understanding of the effect of temporally oscillating interactions to a two-dimensional coarse-grained viral capsid-like model that undergoes a self-limited assembly. This model includes multiple intrinsic relaxation times due to the internal structure of the capsid subunits and, under certain interaction regimes, proceeds a two-step nucleation mechanism. We find that oscillations much faster than the local intrinsic relaxation times can be described a time averaged inter-particle potential across a wide range of interaction strengths, while oscillations much slower than these relaxation times result in structures that adapt to the attraction strength of the current half-cycle. Interestingly, oscillation periods similar to these relaxation times shift the interaction window over which orderly assembly occurs by enabling error correction during the half-cycles with weaker attractions. Our results provide fundamental insights to non-equilibrium self-assembly on temporally variant energy landscapes.
最近出现了多种旨在创建新型结构或减少动力学陷阱的耗散自组装协议。具体而言,粒子相互作用的时间振荡已被证明在这两个目标上都是有效的,但迄今为止的研究主要集中在简单胶体系统或其二元混合物上。在这项工作中,我们将对时间振荡相互作用效果的理解扩展到一个经历自限组装的二维粗粒化病毒衣壳样模型。由于衣壳亚基的内部结构,该模型包含多个固有弛豫时间,并且在某些相互作用机制下,会经历两步成核机制。我们发现,比局部固有弛豫时间快得多的振荡可以用广泛相互作用强度范围内的时间平均粒子间势来描述,而比这些弛豫时间慢得多的振荡会导致结构适应当前半周期的吸引强度。有趣的是,与这些弛豫时间相似的振荡周期通过在吸引力较弱的半周期内实现误差校正,从而改变了有序组装发生的相互作用窗口。我们的结果为非平衡自组装在时间变化的能量景观上提供了基本见解。