Interfacial directed assembly and attachment of interconnected nanoparticle networks

互连纳米粒子网络的界面定向组装和附着

• 批准号: 1803878
• 负责人: Tobias Hanrath
• 金额: $ 37.5万
• 依托单位: Cornell University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-08-01 至 2022-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1803878&HistoricalAwards=false
• 关键词: Interfacial; directed; assembly; attachment; interconnected

Nanoparticles are particles with diameters roughly one thousandth the width of a human hair. This award supports research to investigate how nanoparticles assemble and attach at the surface of a fluid. The process is not unlike how some fine powders can form a layer that floats on top of the surface of quiescent water. Nanoparticle building blocks with programmable size, shape, and composition have become available thanks to recent advances in chemistry. Connecting these building blocks to each other to form "sheets" can give rise to new classes of materials and devices with emergent properties that have intrigued scientists and engineers alike. Unfortunately, assembly instructions are not yet available. This project will close this knowledge gap with a combination of experiments and computer models. This synergistic approach will unveil key details of the mechanism by which the building blocks self-assemble and attach. Hence, the results will lead to strategies to design new building blocks that assemble into desirable patterns with minimal defects. This project will produce new knowledge of scientific and societal importance and may lead to the development of new nanostructured materials. Graduate students will receive extensive training in advanced experimental and modeling approaches, and research opportunities will be provided for undergraduates. Interactive learning modules for local K-12 programs will also be developed.The combination of self-assembly and directed attachment of colloidal nanoparticles at fluid interfaces presents scientifically interesting and technologically important research challenges. Remarkable strides have been made in the synthesis of polyhedral nanoparticle building blocks with precisely defined shapes and their self-assembly into highly ordered superstructures. Recent advances have revealed intriguing synergies between interfacial self-assembly and directed epitaxial attachment into ordered and connected superstructures. Access to superstructures with programmable symmetry opens new opportunities to create materials with properties by design. The main goal of this work is to attain a better understanding of the basic kinetic and thermodynamic factors governing the interplay of self-assembly and directed-attachment. The investigators hypothesize that the key to predicting and creating coupled assemblies with programmable structures lies in understanding and controlling the nanoparticle orientation at the fluid interface as well as the interactions among particles. The nanoparticle orientation at the liquid-liquid interface and subsequent directed attachment is a complex function of the interfacial energies, the nature of multi-particle interactions and the coupled dynamics of interfacial nanoparticle diffusion, ligand displacement from the nanoparticle surface and epitaxial fusion of adjacent nanoparticles through mutually exposed facets. The mechanism describing how the nanoparticle assembly transforms into an epitaxially connected superstructure presents an interesting unresolved scientific question, and competing hypotheses will be tested via a combination of experiments and simulations. In fact, this provides both a challenge and an opportunity to closely integrate in-situ X-ray structure analysis with multi-scale modeling. The proposal presents a hypothesis-driven collaborative approach with two objectives that aim to understand: (1) how specific nanoparticle superlattice polymorphs assemble at fluid interfaces and (2) how directed attachment can transform the assembled superlattice into an epitaxially connected quasi-2D solid.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

纳米颗粒是直径约为人类头发宽度千分之一的颗粒。 该奖项支持研究纳米粒子如何在流体表面组装和附着。 这个过程与一些细粉末形成一层漂浮在静止水面上的过程没有什么不同。 由于化学的最新进展，具有可编程尺寸、形状和成分的纳米粒子构建块已经成为可能。将这些构件相互连接形成“片材”可以产生具有新兴特性的新型材料和设备，这些特性引起了科学家和工程师的兴趣。不幸的是，组装说明尚不可用。该项目将通过实验和计算机模型的结合来缩小这一知识差距。 这种协同方法将揭示构建块自组装和附着机制的关键细节。 因此，研究结果将导致设计新的构建块的策略，这些构建块可以组装成具有最小缺陷的理想图案。该项目将产生具有科学和社会重要性的新知识，并可能导致新型纳米结构材料的开发。研究生将接受高级实验和建模方法的广泛培训，并将为本科生提供研究机会。 还将开发用于当地 K-12 项目的交互式学习模块。自组装和胶体纳米粒子在流体界面上的定向附着的结合提出了科学上有趣且技术上重要的研究挑战。在具有精确定义的形状的多面体纳米粒子构建块的合成以及它们自组装成高度有序的超结构方面已经取得了显着的进步。最近的进展揭示了界面自组装和定向外延附着到有序和连接的上部结构之间的有趣的协同作用。具有可编程对称性的上层结构为通过设计创造具有特性的材料提供了新的机会。这项工作的主要目标是更好地理解控制自组装和定向附着相互作用的基本动力学和热力学因素。研究人员假设，预测和创建具有可编程结构的耦合组件的关键在于理解和控制流体界面处的纳米颗粒方向以及颗粒之间的相互作用。液-液界面处的纳米颗粒取向和随后的定向附着是界面能量、多颗粒相互作用的性质以及界面纳米颗粒扩散、配体从纳米颗粒表面的位移以及相邻纳米颗粒的外延融合的耦合动力学的复杂函数。通过相互暴露的面。描述纳米粒子组装体如何转变为外延连接的上层结构的机制提出了一个有趣的未解决的科学问题，并且将通过实验和模拟相结合来测试相互竞争的假设。事实上，这为将原位 X 射线结构分析与多尺度建模紧密结合提供了挑战和机遇。该提案提出了一种假设驱动的协作方法，其两个目标旨在理解：（1）特定纳米颗粒超晶格多晶型物如何在流体界面处组装；（2）定向附着如何将组装的超晶格转变为外延连接的准二维固体。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

An Implicit-Solvent Model for the Interfacial Configuration of Colloidal Nanoparticles and Application to the Self-Assembly of Truncated Cubes

胶体纳米颗粒界面构型的隐式溶剂模型及其在截断立方体自组装中的应用

• DOI: 10.1021/acs.jctc.0c00283
• 发表时间: 2020-09
• 期刊: Journal of Chemical Theory and Computation
• 影响因子: 5.5
• 作者: Gupta, U.;Escobedo, F. A.
• 通讯作者: Escobedo, F. A.

Fundamental Processes and Practical Considerations of Lead Chalcogenide Mesocrystals Formed via Self-Assembly and Directed Attachment of Nanocrystals at a Fluid Interface

通过纳米晶体在流体界面自组装和定向附着形成铅硫族化物介晶的基本过程和实际考虑

• DOI: 10.1021/acs.chemmater.1c02910.s001
• 发表时间: 2021-12-16
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: Jessica Cimada daSilva;D. Balazs;Tyler A. Dunbar;T. Hanrath
• 通讯作者: T. Hanrath

Ligand Interactions and Nanoparticle Shapes Guide the Pathways toward Interfacial Self-Assembly

配体相互作用和纳米颗粒形状引导界面自组装途径

• DOI: 10.1021/acs.langmuir.1c02804
• 发表时间: 2022-02
• 期刊: Langmuir
• 影响因子: 3.9
• 作者: Gupta, U.;Escobedo, F. A.
• 通讯作者: Escobedo, F. A.

The Role of Dimer Formation in the Nucleation of Superlattice Transformations and Its Impact on Disorder

二聚体形成在超晶格转变成核中的作用及其对无序的影响

• DOI: 10.1021/acsnano.0c03800
• 发表时间: 2020-09
• 期刊: ACS Nano
• 影响因子: 17.1
• 作者: Chen, Isaiah Y.;Cimada daSilva, Jessica;Balazs, Daniel M.;Smeaton, Michelle A.;Kourkoutis, Lena F.;Hanrath, Tobias;Clancy, Paulette
• 通讯作者: Clancy, Paulette

Mechanistic Insights into Superlattice Transformation at a Single Nanocrystal Level Using Nanobeam Electron Diffraction

使用纳米束电子衍射对单纳米晶体水平的超晶格转变进行机理洞察

• DOI: 10.1021/acs.nanolett.0c01579
• 发表时间: 2020-07
• 期刊: Nano Letters
• 影响因子: 10.8
• 作者: daSilva, Jessica Cimada;Smeaton, Michelle A.;Dunbar, Tyler A.;Xu, Yuanze;Balazs, Daniel M.;Kourkoutis, Lena F.;Hanrath, Tobias
• 通讯作者: Hanrath, Tobias