同位素工程石墨烯体系的拉曼光谱和原位拉曼光谱电化学
Raman spectroscopy and In-situ Raman spectroelectrochemistry of isotopically engineered graphene systems
摘要：
石墨烯的独特性质为许多科学领域的应用提供了巨大的机会，以及超出我们目前想象的社会需求。石墨烯的重要特征之一是其电子结构的相对简单的可调谐性，这是一种将石墨烯的可用性进一步扩展到现有经验之外的资产。将载流子直接注入到导带或价带中，即，掺杂，代表了一种可行的方法来移动费米能级。特别是，当需要更高的掺杂水平和需要严格控制实验条件时，电化学掺杂应该是选择的方法。在这个账户中，我们专注于石墨烯的电化学与原位拉曼光谱相结合，即，原位拉曼光谱电化学。这种方法的组合确实非常强大，因为拉曼光谱不仅可以容易地监测掺杂水平的变化，而且还可以提供有关材料中最终应力或无序的信息。然而，当采用拉曼光谱时，其主要优势之一在于在石墨烯样品的化学气相沉积（CVD）生长期间利用同位素工程。在各个层中具有巧妙设计的同位素组成的多层系统的原位拉曼光谱电化学研究可以提供关于以下相互作用的大量知识：（i）石墨烯层本身之间，（ii）石墨烯层与其直接相邻的环境（例如，衬底或电解质）之间，以及（iii）石墨烯层与其扩展环境之间，其通过一定数量的附加石墨烯层与该层分离。
英文摘要：
The unique properties of graphene offer immense opportunities for applications to many scientific fields, as well as societal needs, beyond our present imagination. One of the important features of graphene is the relatively simple tunability of its electronic structure, an asset which extends the usability of graphene even further beyond present experience. A direct injection of charge carriers into the conduction or valence bands, i.e., doping, represents a viable way of shifting the Fermi level. In particular, the electrochemical doping should be the method of choice, when higher doping levels are desired and when a firm control of experimental conditions is needed. In this Account, we focus on the electrochemistry of graphene in combination with in-situ Raman spectroscopy, i.e., the in-situ Raman spectroelectrochemistry. Such a combination of methods is indeed very powerful, since Raman spectroscopy can readily monitor not only the changes in the doping level, but it can give information also on eventual stress or disorder in the material. However, when employing Raman spectroscopy, one of its main strengths lies in the utilization of isotope engineering during the chemical vapor deposition (CVD) growth of the graphene samples. The in-situ Raman spectroelectrochemical study of multi-layered systems with smartly designed isotope compositions in individual layers can provide a plethora of knowledge about the mutual interactions: (i) between the graphene layers themselves, (ii) between graphene layers and their directly adjacent environment (e.g., substrate or electrolyte), and (iii) between graphene layers and their extended environment, which is separated from the layer by a certain number of additional graphene layers.
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