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

本课题由化学系高分子、超分子和纳米化学项目资助，西奥多L.马里兰州大学的爱因斯坦和滨江的加州大学的路德维希·巴特尔斯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拟，来理解并苯的大型规则自组织网络的形成，相关的分子在基板上突出的金属表面状态和所产生的nanoscalepores的作用，提供边界，修改小吸附物的安排和反应，如COTHIN。与国际合作者，他们将测试理论的修改（从大表面）关键反应速率，因为改变熵的混合在封闭的孔隙，并将研究的关系，结构的表面状态上的紧密堆积面的铜基板，并调查thecorrections到一个简单的图片点诱导孔的形成。他们还将利用研究在二维（2D）材料为主的电子状态与许多相似的金属surfacestates。这个项目将提供最先进的建模和/或实验室经验的研究生和本科生谁将学习扫描探针显微镜和互补蒙特卡罗模拟和相关函数的计算技术，以及从头算电子结构计算，以帮助参数化的统计力学研究。该项目包括探索有机分子在具有缓慢衰减的2D电子态的基底上形成规则的多孔超结构。验证的新的解释孔稳定的二维量子点状状态将被追求。这种状态对孔隙内小吸附物（特别是一氧化碳）分布的影响将被仔细研究。相关参数的计算将需要利用最新的进展，将货车德瓦尔斯相互作用纳入密度泛函理论计算。通过在物理学方面经验丰富的理论家的领导，该项目将促进系统的观点，更深入的理解和更快的测试相和图案形成的结果，并预测有希望的替代基板和吸附物。拟议的工作预计将对工业方法和社会的影响，通过提供访问相同的纳米级细胞的大阵列，其中一个可以做实验等效的并行计算。对这种结构的控制将允许调整细胞大小，以选择可互换的配置并增强特定的反应，以及探索自然波动。这项工作还将为教育和外联活动提供机会，并证明具有广泛的国家、国际和社会影响。

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 they 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. They 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.