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Tunable Orientation and Assembly of Polymer-Grafted Nanocubes at Fluid–Fluid Interfaces
ACS Nano ( IF 15.8 ) Pub Date : 2022-04-22 , DOI: 10.1021/acsnano.1c10416 Yilong Zhou 1 , Tsung-Yeh Tang 2 , Brian Hyun-Jong Lee 1 , Gaurav Arya 1
ACS Nano ( IF 15.8 ) Pub Date : 2022-04-22 , DOI: 10.1021/acsnano.1c10416 Yilong Zhou 1 , Tsung-Yeh Tang 2 , Brian Hyun-Jong Lee 1 , Gaurav Arya 1
Affiliation
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Self-assembly of faceted nanoparticles is a promising route for fabricating nanomaterials; however, achieving low-dimensional assemblies of particles with tunable orientations is challenging. Here, we demonstrate that trapping surface-functionalized faceted nanoparticles at fluid–fluid interfaces is a viable approach for controlling particle orientation and facilitating their assembly into unique one- and two-dimensional superstructures. Using molecular dynamics simulations of polymer-grafted nanocubes in a polymer bilayer along with a particle-orientation classification method we developed, we show that the nanocubes can be induced into face-up, edge-up, or vertex-up orientations by tuning the graft density and differences in their miscibility with the two polymer layers. The orientational preference of the nanocubes is found to be governed by an interplay between the interfacial area occluded by the particle, the difference in interactions of the grafts with the two layers, and the stretching and intercalation of grafts at the interface. The resulting orientationally constrained nanocubes are then shown to assemble into a variety of unusual architectures, such as rectilinear strings, close-packed sheets, bilayer ribbons, and perforated sheets, which are difficult to obtain using other assembly methods. Our work thus demonstrates a versatile strategy for assembling freestanding arrays of faceted nanoparticles with possible applications in plasmonics, optics, catalysis, and membranes, where precise control over particle orientation and position is required.
中文翻译：
流体-流体界面聚合物接枝纳米立方体的可调取向和组装
多面纳米粒子的自组装是制造纳米材料的一条很有前途的途径；然而，实现具有可调方向的低维粒子组装具有挑战性。在这里，我们证明了在流体-流体界面捕获表面功能化的多面纳米粒子是控制粒子方向并促进它们组装成独特的一维和二维超结构的可行方法。使用聚合物双层中聚合物接枝纳米立方体的分子动力学模拟以及我们开发的粒子取向分类方法，我们表明可以通过调整接枝将纳米立方体诱导成面朝上、边朝上或顶点朝上的方向密度和它们与两个聚合物层的混溶性差异。发现纳米立方体的取向偏好受粒子遮挡的界面区域、接枝与两层相互作用的差异以及接枝在界面处的拉伸和插入之间的相互作用控制。由此产生的方向受限的纳米立方体随后被证明可以组装成各种不寻常的结构，例如直线串、密排板、双层带和穿孔板，这些是使用其他组装方法难以获得的。因此，我们的工作展示了一种多功能策略，用于组装独立的多面纳米粒子阵列，可能应用于等离子体、光学、催化和膜，这些领域需要精确控制粒子方向和位置。
更新日期：2022-04-22
中文翻译：
流体-流体界面聚合物接枝纳米立方体的可调取向和组装
多面纳米粒子的自组装是制造纳米材料的一条很有前途的途径；然而，实现具有可调方向的低维粒子组装具有挑战性。在这里，我们证明了在流体-流体界面捕获表面功能化的多面纳米粒子是控制粒子方向并促进它们组装成独特的一维和二维超结构的可行方法。使用聚合物双层中聚合物接枝纳米立方体的分子动力学模拟以及我们开发的粒子取向分类方法，我们表明可以通过调整接枝将纳米立方体诱导成面朝上、边朝上或顶点朝上的方向密度和它们与两个聚合物层的混溶性差异。发现纳米立方体的取向偏好受粒子遮挡的界面区域、接枝与两层相互作用的差异以及接枝在界面处的拉伸和插入之间的相互作用控制。由此产生的方向受限的纳米立方体随后被证明可以组装成各种不寻常的结构，例如直线串、密排板、双层带和穿孔板，这些是使用其他组装方法难以获得的。因此，我们的工作展示了一种多功能策略，用于组装独立的多面纳米粒子阵列，可能应用于等离子体、光学、催化和膜，这些领域需要精确控制粒子方向和位置。
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