期刊
ACS NANO
卷 15, 期 5, 页码 8466-8473出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c10874
关键词
self-assembly; reconfigurable materials; solid-solid transition; DNA-functionalized particles; molecular dynamic simulations; coarse-grained model
类别
资金
- US Department of Energy, Office of Science, Basic Energy Sciences Award [DE-SC00013979]
- National Energy Research Scientific Computing Center resources, a DOE Office of Science User Facility [DE-AC02-05CH11231]
- National Science Foundation [TG-MCB120014]
This study investigates the nature of diffusionless transformations during the assembly of DNA-functionalized particles (DFPs) and demonstrates that reversible structural rearrangements between BCC and FCC structures can be driven by changing temperature. The findings have important implications for the design of reconfigurable crystalline materials and are applicable to experimentally realizable systems.
The presence of diffusionless transformations during the assembly of DNA-functionalized particles (DFPs) is highly significant in designing reconfigurable materials whose structure and functional properties are tunable with controllable variables. In this paper, we first use a variety of computational models and techniques (including free energy methods) to address the nature of such transformations between face-centered cubic (FCC) and body-centered cubic (BCC) structures in a three-dimensional binary system of multiflavored DFPs. We find that the structural rearrangements between BCC and FCC structures are thermodynamically reversible and dependent on crystallite size. Smaller nuclei favor nonclose-packed BCC structures, whereas close-packed FCC structures are observed during the growth stage once the crystallite size exceeds a threshold value. Importantly, we show that a similar reversible transformation between BCC/FCC structures can be driven by changing temperature without introducing additional solution components, highlighting the feasibility of creating reconfigurable crystalline materials. Lastly, we validate this thermally responsive switching behavior in a DFP system with explicit DNA (un)hybridization, demonstrating our findings' applicability to experimentally realizable systems.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据