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Spatio-Temporal and Site-Specific Chemical Dynamics at Interfaces

界面处的时空和特定位点化学动力学

基本信息

批准号：
1900188
负责人：
Steven Sibener
金额：
$ 49万
依托单位：
University of Chicago
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2019
资助国家：
美国
起止时间：
2019-08-01 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1900188&HistoricalAwards=false
关键词：
Spatio Temporal Site Specific Chemical

项目摘要

Chemical reactions at surfaces are everywhere, from the corrosion of metals to the fabrication of computer chips. However, compared with studying reactions in gases and solutions, chemical reactions at surfaces present unique challenges. The reactivity, for example, can depend on how fast reactant molecules collide with the surface, as well as the direction of approach. To complicate matters, surfaces are structurally imperfect at the atomic level and are littered with defects, including missing atoms, islands, and steps, each of which can react differently. Moreover, once the reaction occurs, it can shift nearby atoms around, changing the surface structure. With support from the Chemical Structure, Dynamics and Mechanism A program in the Division of Chemistry, Professor Steven J. Sibener at The University of Chicago is studying chemical reactions between highly reactive reagents such as oxygen and hydrogen atoms, as well as other energetic species, with metal and semiconductor surfaces. Working with his students, Professor Sibener directs atomic and molecular beams with known speed and direction at either bare surfaces, or surfaces decorated with molecules. The team then uses powerful microscopies capable of resolving individual atoms to monitor the reactivity at different sites, as well as how the surface structure changes in response to the reaction. Their discoveries could have broad implications for advanced materials fabrication, nanoscience, electronic materials, heterogeneous catalysis, combustion, and the design of protective coatings. The research team also participates in community outreach at local schools and museums to introduce the residents of Chicago's south-side to scientific issues that are essential for understanding our modern technological world. This program uses a combination of supersonic molecular beams, in situ scanning tunneling/atomic force microscopy, and surface spectroscopies to examine the site-specific chemical reactivity of clean and molecule decorated surfaces. Reactive scattering measurements are carried out with concurrent in situ atomic-level imaging. This program opens a direct path to understanding, with atomic resolution, spatio-temporal correlations in interfacial reactivity. It has focus on forefront issues in surface chemical dynamics that include adiabatic and non-adiabatic gas-surface interactions, atomically-resolved reactivity under non-equilibrium conditions, thin film growth and passivation, and geometry-constrained reaction studies with precise steric control over incident collision conditions. Such assessment of molecular reactivity as a function of known molecular orientation and local adsorption site is revealing remarkably detailed information on molecular reactivity and reaction potential energy surfaces suitable for quantitative comparison with theory and simulations.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.

从金属的腐蚀到计算机芯片的制造，表面的化学反应无处不在。然而，与研究气体和溶液中的反应相比，表面的化学反应提出了独特的挑战。例如，反应性可以取决于反应物分子与表面碰撞的速度以及接近的方向。更复杂的是，表面在原子水平上是结构不完美的，并且充满了缺陷，包括缺失的原子、岛和台阶，每一个都可能发生不同的反应。此外，一旦反应发生，它可以移动附近的原子，改变表面结构。在化学系化学结构，动力学和机制A计划的支持下，芝加哥大学的Steven J. Sibener教授正在研究高活性试剂（如氧原子和氢原子）以及其他高能物质与金属和半导体表面之间的化学反应。Sibener教授与他的学生一起工作，以已知的速度和方向将原子和分子束引导到裸露的表面或用分子装饰的表面。然后，该团队使用能够分辨单个原子的强大显微镜来监测不同位点的反应性，以及表面结构如何响应反应而变化。他们的发现可能对先进材料制造、纳米科学、电子材料、多相催化、燃烧和保护涂层的设计产生广泛的影响。研究小组还参加了当地学校和博物馆的社区外展活动，向芝加哥南部的居民介绍对理解我们现代技术世界至关重要的科学问题。该计划使用超声分子束，原位扫描隧道/原子力显微镜和表面光谱的组合来检查清洁和分子装饰表面的特定位点的化学反应性。反应散射测量进行了并发原位原子级成像。该计划为以原子分辨率理解界面反应性的时空相关性开辟了一条直接的道路。它专注于表面化学动力学的前沿问题，包括绝热和非绝热气体-表面相互作用，非平衡条件下的原子分辨反应性，薄膜生长和钝化，以及对入射碰撞条件进行精确空间控制的几何约束反应研究。这种分子反应性作为已知分子取向和局部吸附位点的函数的评估揭示了分子反应性和反应势能表面的非常详细的信息，适合与理论和模拟进行定量比较。该奖项反映了NSF的法定使命，并被认为值得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来支持。

项目成果

期刊论文数量（11）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Room temperature oxidation of GaAs(110) using high translational kinetic energy molecular beams of O2 visualized by STM

使用 STM 可视化的 O2 高平动动能分子束进行 GaAs(110) 的室温氧化

DOI：
10.1016/j.susc.2019.121516
发表时间：
2020
期刊：
Surface Science
影响因子：
1.9
作者：
Grabnic, Tim;Edel, Ross;Sibener, S.J.
通讯作者：
Sibener, S.J.

Chain-Length-Dependent Reactivity of Alkanethiolate Self-Assembled Monolayers with Atomic Hydrogen

烷硫醇自组装单分子层与原子氢的链长依赖性反应性

DOI：
10.1021/acs.jpcc.9b06809
发表时间：
2019
期刊：
The Journal of Physical Chemistry C
影响因子：
0
作者：
Sayler, Jeffrey D.;Brown, Sarah;Sibener, S. J.
通讯作者：
Sibener, S. J.

Influence of Structural Dynamics on the Kinetics of Atomic Hydrogen Reactivity with Low-Temperature Alkanethiolate Self-Assembled Monolayers

结构动力学对低温链烷硫醇自组装单层原子氢反应动力学的影响

DOI：
10.1021/acs.jpcc.1c07487
发表时间：
2021
期刊：
The Journal of Physical Chemistry C
影响因子：
0
作者：
Brown, Sarah;Sayler, Jeffrey D.;Sibener, S. J.
通讯作者：
Sibener, S. J.

Reverse water-gas shift chemistry inside a supersonic molecular beam nozzle

超音速分子束喷嘴内的逆水煤气变换化学

DOI：
10.1016/j.apsusc.2020.145985
发表时间：
2020
期刊：
Applied Surface Science
影响因子：
6.7
作者：
Thompson, Rebecca S.;Langlois, Grant G.;Li, Wenxin;Brann, Michelle R.;Sibener, S.J.
通讯作者：
Sibener, S.J.

Vapor-phase grafting of functional silanes on atomic layer deposited Al2O3

DOI：
10.1116/6.0002364
发表时间：
2023-04
期刊：
Journal of Vacuum Science & Technology A
影响因子：
0
作者：
Vepa Rozyyev;Rahul Shevate;R. Pathak;Julia G. Murphy;A. Mane;S. Sibener;J. Elam
通讯作者：
Vepa Rozyyev;Rahul Shevate;R. Pathak;Julia G. Murphy;A. Mane;S. Sibener;J. Elam