Computational design and atomic layer deposition synthesis of stereochemically active multifunctional oxide nanostructures

该奖项支持一项研究计划，致力于探索新型多功能含锡氧化物材料，其中锡的2+氧化态与电子“孤对”的存在有关。由这些具有空间活性但化学惰性的电子引起的大的离子位移导致大的弹性变形和强的极性性质。pi的协同方法包括材料理论和计算，以及作为项目基本相互关联部分的生长和表征。利用这些工具的组合，pi将：(a)在锡基氧化物的体、薄膜和纳米结构形式中研究复杂的耦合现象——包括弹性、极性和电子现象；(b)确定在这些化合物中实现增强或未知的新特性的合理途径，这些特性将导致先进的功能；(c)开发利用原子层/化学气相沉积来生长锡基氧化物的合成工艺，以及将其纳入各种纳米结构的加工技术。该项目是康涅狄格大学和伊利诺伊大学芝加哥分校的合作项目，包括与阿贡国家实验室的合作。pi将使用一种独特的原子层/化学气相沉积反应器来制造新的多功能氧化物材料，其尺寸范围从体状的多微米到纳米，同时保持高度的结构一致性。这些材料的相关电活性和电化学性能将不仅作为组成和结构的功能来研究，而且还将作为从微米长度尺度到原子、亚纳米尺度的薄膜厚度的功能来研究。利用从原子/分子尺度到中尺度建立信息流的综合模拟方法，将为实验生长和表征工作提供支持和指导。理论和模拟任务包括合成候选结构的初始选择，其性质的预测评估，最佳生长条件的确定以及由这些材料制成的不同形状和尺寸的纳米结构的功能行为的粗粒度评估。该研究项目将通过对本科生和研究生进行实验和计算材料科学技术的培训，并将研究成果纳入凝聚态物理和材料科学课程，从而整合到本科生和研究生的教育和指导经验中。这两所PI机构都位于少数民族学生人数众多的地区，并提供完善的项目，以新的物理、化学和工程模块的形式，或通过一系列科学、数学和技术研讨会，向初高中学生和教师传播研究成果和方法。这些项目将利用这两种途径，鼓励来自代表性不足的少数群体的学生参与与本项目有关的科技活动。该奖项支持一项研究计划，致力于探索新型多功能含锡氧化物材料，旨在作为铅基化合物的环保替代品，用于各种技术应用，包括能量收集、存储和转换，例如在机械和电气形式之间的能量。pi的协同方法包括材料理论和计算的使用，以及作为项目基本相互关联部分的生长和表征。这些工具的结合将有助于研究大块、薄膜和纳米结构形式的锡基氧化物的弹性和电子特性，并开发合成工艺，通过逐层沉积技术和加工技术来生长这些结构，从而使其有可能融入各种电子设备。该项目是康涅狄格大学和伊利诺伊大学芝加哥分校的合作项目，包括与阿贡国家实验室的合作。一个独特的逐层生长室将用于制造尺寸从多微米到纳米的新型氧化锡化合物，同时保持高水平的材料质量。这些材料的电子和机械性能将作为化学成分和生长样品长度尺度的函数进行研究。计算机模拟将为实验生长和表征工作提供支持和指导。理论和模拟任务包括合成候选结构的初始选择，其性质的评估和最佳生长条件的确定。该研究项目将通过对本科生和研究生进行实验和计算材料科学技术的培训，并将研究成果纳入凝聚态物理和材料科学课程，从而整合到本科生和研究生的教育和指导经验中。所涉及的机构位于少数民族学生人数众多的地区，并提供完善的计划，以新的物理、化学和工程模块的形式，或通过一系列科学、数学和技术研讨会，向初高中学生和教师传播研究成果和方法。这两种途径都将用于鼓励来自代表性不足的少数群体的学生参加与新材料有关的科技活动。

Technical SummaryThis award supports a research program dedicated to exploring novel multifunctional tin-containing oxide materials, where the 2+ oxidation state of tin is associated with the presence of electron 'lone pairs.' Large ionic displacements induced by these sterically active, but chemically inert electrons lead to large elastic deformations and strong polar properties. The PIs' synergistic approach includes both materials theory and computation, and growth and characterization as essential interconnected parts of the project. Utilizing the combination of these tools, the PIs will: (a) investigate complex coupled phenomena - including elastic, polar and electronic ones - in bulk, thin-film and nanostructured forms of tin-based oxides, (b) identify rational pathways for achieving enhanced or yet unknown new properties in these compounds that will lead to advanced functionalities, (c) develop synthetic processes to grow tin-based oxides utilizing atomic layer / chemical vapor deposition as well as processing technologies to incorporate them into a variety of nanostructures.This project is a collaboration between the University of Connecticut and University of Illinois at Chicago, and includes a collaboration with Argonne National Laboratory. The PIs will use a unique atomic layer / chemical vapor deposition reactor to fabricate new multifunctional oxide materials with dimensions ranging from bulk-like multi-micron to nanometer, while preserving a high degree of structural conformality. The pertinent electroactive and electrochemical properties of these materials will be investigated as functions of not only composition and structure, but also film thickness from the micron length scale to the atomic, sub-nanometer regime. The utilization of an integrated simulation approach with established information flow from atomic / molecular scale to mesoscale will provide both support and guidance for the experimental growth and characterization efforts. Theory-and-simulation tasks include initial selection of candidate structures for synthesis, predictive evaluation of their properties, identification of optimal growth conditions and coarse-grained evaluation of functional behavior of nanostructures of different shapes and sizes made out of these materials. This research program will be integrated into educational and mentoring experiences for undergraduate and graduate students by training them in experimental and computational materials science techniques and incorporating the research results into courses in Condensed Matter Physics and Materials Science. Both PI institutions are located in areas with large populations of underrepresented minority students and provide well established programs for disseminating research findings and methodologies to middle and high school students and teachers either in the form of new physics, chemistry and engineering modules, or through series of workshops in science, math, and technology. The PIs will use both of these routes to encourage students from underrepresented minority groups to participate in science and technology activities related to this project.Nontechnical SummaryThis award supports a research program dedicated to exploring novel multifunctional tin-containing oxide materials, intended as environmentally benign replacements of lead-based compounds for a variety of technological applications including energy harvesting, storage and conversion, for example between mechanical and electrical forms of energy. The PIs' synergistic approach includes the use of materials theory and computation, and growth and characterization as essential interconnected parts of the project. The combination of these tools will help investigate elastic and electronic properties of bulk, thin-film and nanostructured forms of tin-based oxides, and develop synthetic processes to grow these structures with layer-by-layer deposition techniques as well as processing technologies for their potential incorporation into a variety of electronic devices.This project is a collaboration between the University of Connecticut and University of Illinois at Chicago, and includes a collaboration with Argonne National Laboratory. A unique layer-by-layer growth chamber will be used to fabricate new tin-oxide compounds with dimensions ranging from multi-micron to nanometer, while preserving a high degree of material quality. Electronic and mechanical properties of these materials will be investigated as functions of chemical composition and length scale of the grown samples. Computer simulations will provide support and guidance for the experimental growth and characterization efforts. Theory-and-simulation tasks include initial selection of candidate structures for synthesis, evaluation of their properties and identification of optimal growth conditions. This research program will be integrated into educational and mentoring experiences for undergraduate and graduate students by training them in the experimental and computational materials science techniques, and incorporating the research results into courses in Condensed Matter Physics and Materials Science. The institutions involved are located in with large populations of underrepresented minority students and provide well established programs for disseminating research findings and methodologies to middle and high school students and teachers either in the form of new physics, chemistry and engineering modules, or through series of workshops in science, math, and technology. Both these routes will be used to encourage students from underrepresented minority groups to participate in science and technology activities related to new materials.