Inverse Design of Self Assembling Nanocrystals: Low Coordinated Superlattices via Isotropic Potentials

PI：TRUSKETT，托马斯提案编号：1403768机构：德克萨斯大学奥斯汀分校标题：自组装纳米晶体的逆向设计：通过各向同性势能实现低配位超晶格目前人们对制造纳米颗粒(NP)的晶体(组件)很感兴趣，由于这些超晶格具有用作独特的光开关器件或用于传感的潜力，因此可以被认为是‘超晶格’。传统的纳米材料开发大多是一种自上而下的方法，即首先发现新的纳米材料和结构，然后确定它们的性质并展望其应用前景，而PI提出了一种按设计材料的方法，据此他们将设计并实验验证一个理论框架，以合理地设计配体封顶的NPs，使其以低配位自组装成特定的目标结构(超晶格)。他们选择球形纳米粒子(NPs)作为待测试的模型系统，而不是更难制造各向异性NPs，这将增加他们成功的机会。这是一个深思熟虑、集成良好的提案，旨在测试和验证自组装纳米晶体反向设计的新理论框架。这项研究的结果将具有广泛的适用性，为合理设计新型自组装结构的相互作用开辟了可能性。PI建议扩展他在最近的CBET赠款0165357中开发的逆统计-力学(SM)优化方法，并建议通过调整粒子间的势来探索在简单的单组分球形粒子系统中组装各种晶格(六边形、立方体等)的方法。他计划进一步模拟库什NP形成的平衡相图和动力学。然后，实验Co-PI将使用模拟的结果来制备和表征选定的配体封顶的纳米晶体，这些纳米晶体已经在电子计算机模拟中进行了优化。他们的计划包括三个主要活动：1)使用基于XM的逆优化来确定有利于目标超晶格的相互作用参数。2)使用分子模拟，结合相互作用势，确定平衡和动力学相行为(发现设计规则)。3)综合和研究最佳候选模型，并使用掠入射小角X射线散射(GISAXS)等技术对系统进行表征。

PI: Truskett, Thomas Proposal Number: 1403768 Institution: University of Texas at Austin Title: Inverse Design of Self Assembling Nanocrystals: Low Coordinated Superlattices via Isotropic Potentials There is currently much interest in making crystals (assemblies) of nanoparticles (NPs), which can be considered 'superlattices' due to the potential of these superlattices to be used as unique optical switching devices or for sensing. While traditional nano-materials development is mostly a top-down approach, whereby novel nanomaterials and structures are first discovered and then their properties are determined and applications envisioned, the PIs propose a materials-by-design approach, whereby they will devise and experimentally validate a theoretical framework to rationally design ligand-capped NPs to self-assemble into specific targeted structures (superlattices) with low coordination. Their choice of spherical nanoparticles (NPs) as the model system to be tested, rather than the harder to make anisotropic NPs, will increase their chances of being successful. This is a well-thought, well-integrated proposal to test and validate a new theoretical framework for the inverse design of self-assembling nanocrystals. Results from the research will have broad applicability, opening up the possibilities of rationally designing interactions for novel self-assembling structures.The PI proposes to extend the inverse statistic-mechanical (SM) optimization method developed in his recent CBET grant 0165357 and suggests ways to explore, in-silico, the assembly of various lattices (hexagonal, cubic, etc) in a simple one component system of spherical particles by just adjusting inter-particle potentials. He plans further to simulate the equilibrium phase diagrams and dynamics of cush NP formation. The experimental Co-PI will then use the results of the simulation to fabricate and characterize selected ligand-capped nanocrystals, which had been optimized in the in-silico simulations. Their plan comprises three major activities: 1) Use the XM-based inverse optimization to determine interaction parameters that favor targetted superlattices. 2) Use molecular simulations, together with the interaction potentials, to determine equilibrium and kinetic phase behaviors (discover design rules). 3) Synthesize and investigate the best candidate models and characterize the systems using techniques such as grazing-incidence small-angle x-ray scattering (GISAXS).