Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, MN 55455, USA.
Proc Natl Acad Sci U S A. 2011 Jan 18;108(3):965-70. doi: 10.1073/pnas.1006665107. Epub 2010 Nov 19.
Semiconductor nanocrystals are called artificial atoms because of their atom-like discrete electronic structure resulting from quantum confinement. Artificial atoms can also be assembled into artificial molecules or solids, thus, extending the toolbox for material design. We address the interaction of artificial atoms with bulk semiconductor surfaces. These interfaces are model systems for understanding the coupling between localized and delocalized electronic structures. In many perceived applications, such as nanoelectronics, optoelectronics, and solar energy conversion, interfacing semiconductor nanocrystals to bulk materials is a key ingredient. Here, we apply the well established theories of chemisorption and interfacial electron transfer as conceptual frameworks for understanding the adsorption of semiconductor nanocrystals on surfaces, paying particular attention to instances when the nonadiabatic Marcus picture breaks down. We illustrate these issues using recent examples from our laboratory.
半导体纳米晶体因其量子限域导致的类原子离散电子结构而被称为人造原子。人造原子也可以组装成人造分子或固体,从而扩展了材料设计的工具包。我们研究了人造原子与体半导体表面的相互作用。这些界面是理解局域和非局域电子结构之间耦合的模型体系。在许多被认为的应用中,如纳米电子学、光电学和太阳能转换,将半导体纳米晶体与体材料接口是一个关键要素。在这里,我们应用化学吸附和界面电子转移的成熟理论作为理解半导体纳米晶体在表面上吸附的概念框架,特别关注非绝热 Marcus 图像失效的情况。我们使用来自我们实验室的最新实例来说明这些问题。