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Vibrational Raman Spectroscopy on Adsorbate-Induced Low-Dimensional Surface Structures
Surface Science Reports ( IF 9.8 ) Pub Date : 2020-01-13 , DOI: 10.1016/j.surfrep.2020.100480
Eugen Speiser , Norbert Esser , Benedikt Halbig , Jean Geurts , Wolf Gero Schmidt , Simone Sanna

Low-dimensional self-organized surface structures, induced by (sub)monolayer metal adsorbates on semiconductor surfaces may give rise not only to a variety of emergent electronic properties, but also to a multitude of specific localized vibronic features. The focus of this review is on the analysis of these novel surface vibration eigenmodes. The application of in situ surface Raman spectroscopy under UHV conditions on clean semiconductor surfaces and those with self-ordered adsorbates, in close conjunction with the calculations of Raman spectra, based on the first-principles determination of the structural, electronic and vibronic properties, allows a consistent determination of the vibration eigenfrequencies, symmmetry properties, and elongation patterns of the systems of interest. The localized nature of the surface eigenmodes determines the surface sensitivity, independent of the high light penetration depth of light. The surface contribution can be selectively enhanced by employing resonance condition to surface electronic transitions. Moreover, surface and bulk contributions can be separated by taking difference spectra between various stages of surface preparation. The relevant surfaces are Ge and moreover Si with different orientations ((111) and vicinal (hhk)), on which the adsorption of various metal elements (Au, Sn, Pb, or In) gives rise to two- and quasi-one-dimensional structures (e.g. Au-(5×2)/Si(111)) with a variety of vibration modes. The Raman analysis of these modes does not only enable the distinction between different proposed structural models (e.g. for Au-(3×3)/Si(111)), but also gives access to the role of electron-phonon coupling in structural phase transitions (e.g. for In-(8×2)–(4×1)/Si(111)).



中文翻译:

吸附物诱导的低维表面结构的振动拉曼光谱

由(亚)单层金属吸附物在半导体表面上诱导的低维自组织表面结构不仅会产生各种新兴的电子特性,而且还会产生大量特定的局部振动特征。本文的重点是对这些新颖的表面振动本征模式的分析。原位应用在超高压条件下,在干净的半导体表面和具有自定序吸附物的表面上进行表面拉曼光谱,并结合拉曼光谱的计算,基于对结构,电子和振动性质的第一性原理的确定,感兴趣的系统的振动本征频率,对称性和伸长模式。表面本征模的局部性质决定了表面灵敏度,与光的高光穿透深度无关。通过对表面电子跃迁采用共振条件,可以选择性地提高表面贡献。此外,可以通过在表面准备的各个阶段之间获取差异光谱来分离表面和整体贡献。相关的表面是Ge以及取向不同的Si((111)和邻位(hhk)),各种金属元素(Au,Sn,Pb或In)的吸附会在表面上产生二和准一各种振动模式的三维结构(例如Au-(5×2)/ Si(111))。这些模式的拉曼分析不仅可以区分不同的提议结构模型(例如,对于Au-(3×3)/ Si(111)),但也可以访问电子-声子耦合在结构相变中的作用(例如,对于In-(8×2)–(4×1)/ Si(111))。

更新日期:2020-01-13
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