Collaborative Research: Modeling & Model Systems for Adsorbate Behavior in Lateral Confinement

合作研究：建模

• 批准号: 1306969
• 负责人: Ludwig Bartels
• 金额: $ 15万
• 依托单位: University of California-Riverside
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-09-01 至 2018-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1306969&HistoricalAwards=false
• 关键词: Collaborative; Research; Modeling; & Model

In this project, funded by the Macromolecular, Supramolecular and Nanochemistry Program of theChemistry Division, Prof. Theodore L. Einstein of University of Maryland and Prof. Ludwig Bartels ofthe University of California, Riverside, and their students will use a combination of scanning tunnelingmicroscopy and methods of statistical mechanics, especially Monte Carlo simulations and lattice-gasmodeling, to understand the formation of large regular self-organized networks of acene-relatedmolecules on substrates with prominent metallic surface states and the role of the resulting nanoscalepores in providing boundaries that modify the arrangements and reactions of small adsorbates like COtherein. With international collaborators we will test theories of modification (from large surfaces) keyreaction rates because of altered entropy of mixing in the confined pores and will study the relation of thesuperstructure to the surface state on the close-packed face of the copper substrate and investigate thecorrections to a simple picture of dot-induced pore formation. We will also take advantage of research intwo dimensional (2D) materials dominated by electronic states with many similarities to metallic surfacestates.This project will provide state of the art modeling and/or laboratory experiences for graduate andundergraduate students who will be learning the techniques of scanning probe microscopy andcomplementary Monte Carlo simulations and calculations of correlation functions, as well as ab initioelectronic structure calculations to help parameterize the statistical mechanical studies. The projectconsists of an exploration of the formation of regular porous superstructures by organic molecules onsubstrates with slowly decaying 2D electronic states. The validation of the novel explanation of porestabilization by 2D quantum-dot-like states will be pursued. The impact of such states on the distributionof small adsorbates (especially carbon monoxide) within the pore will be scrutinized. Calculations ofassociated parameters will require use of the latest advances in incorporating van der Waals interactionsinto density functional theory computations. Through leadership by a theorist experienced in statisticalphysics, this project will foster systematic perspective, deeper understanding and faster testing of resultsfor phase and pattern formation and predictions promising alternative substrates and adsorbates. Theproposed work is expected to have impact on industrial methodologies and society at large by providingaccess to large arrays of identical nanoscale cells in which one can do the experimental equivalent ofparallel computation. Control of such structures will allow tuning of cell sizes to select for favorableconfigurations and enhance particular reactions, as well as to explore natural fluctuations. The work willalso provide opportunities for educational and outreach activities with proven broad national,international and societal impact.

在该项目中，由化学部高分子、超分子和纳米化学项目资助，马里兰大学Theodore L. Einstein教授和加州大学河滨分校Ludwig Bartels教授及其学生将结合使用扫描隧道显微镜和统计力学方法，特别是蒙特卡罗模拟和晶格气体模型， 了解并苯相关分子在具有显着金属表面态的基底上形成的大型规则自组织网络，以及由此产生的纳米级孔在提供改变小吸附物（如CO）的排列和反应的边界方面的作用。我们将与国际合作者一起测试由于受限孔中混合熵改变而导致的改性（从大表面）关键反应速率的理论，并将研究超结构与铜基板密排面上表面状态的关系，并研究对点诱导孔形成的简单图像的校正。我们还将利用以电子态为主的二维 (2D) 材料的研究，与金属表面态有许多相似之处。该项目将为研究生和本科生提供最先进的建模和/或实验室经验，他们将学习扫描探针显微镜技术、互补蒙特卡罗模拟和相关函数计算，以及从头开始电子结构计算，以帮助 参数化统计力学研究。该项目包括探索有机分子在具有缓慢衰减的二维电子态的基底上形成规则的多孔超结构。我们将继续验证二维类量子点态对孔隙稳定作用的新解释。将仔细研究这种状态对孔内小吸附物（尤其是一氧化碳）分布的影响。相关参数的计算将需要利用将范德华相互作用纳入密度泛函理论计算的最新进展。在统计物理学方面经验丰富的理论家的领导下，该项目将促进系统的视角、更深入的理解和更快的测试相和图案形成的结果以及有前途的替代底物和吸附物的预测。拟议的工作预计将对工业方法和整个社会产生影响，因为它提供了对相同纳米级单元的大型阵列的访问，在这些单元中人们可以进行相当于并行计算的实验。对此类结构的控制将允许调整细胞尺寸以选择有利的配置并增强特定反应，以及探索自然波动。这项工作还将为教育和外展活动提供机会，这些活动已被证明具有广泛的国家、国际和社会影响。