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Optically probing Al-O and O-H vibrations to characterize water adsorption and surface reconstruction on alpha-alumina: An experimental and theoretical study

  • Oxide/water interfaces are ubiquitous in a wide variety of applications and the environment. Despite this ubiquity, and attendant decades of study, gaining molecular level insight into water/oxide interaction has proven challenging. In part, this challenge springs from a lack of tools to concurrently characterize changes in surface structure (i.e., water/oxide interaction from the perspective of the solid) and O-H population and local environment (i.e., water/oxide interaction from the water perspective). Here, we demonstrate the application of surface specific vibrational spectroscopy to the characterization of the interaction of the paradigmatic alpha-Al2O3(0001) surface and water. By probing both the interfacial Al-O (surface phonon) and O-H spectral response, we characterize this interaction from both perspectives. Through electronic structure calculation, we assign the interfacial Al-O response and rationalize its changes on surface dehydroxylation and reconstruction. Because our technique is all-optical and interface specific,Oxide/water interfaces are ubiquitous in a wide variety of applications and the environment. Despite this ubiquity, and attendant decades of study, gaining molecular level insight into water/oxide interaction has proven challenging. In part, this challenge springs from a lack of tools to concurrently characterize changes in surface structure (i.e., water/oxide interaction from the perspective of the solid) and O-H population and local environment (i.e., water/oxide interaction from the water perspective). Here, we demonstrate the application of surface specific vibrational spectroscopy to the characterization of the interaction of the paradigmatic alpha-Al2O3(0001) surface and water. By probing both the interfacial Al-O (surface phonon) and O-H spectral response, we characterize this interaction from both perspectives. Through electronic structure calculation, we assign the interfacial Al-O response and rationalize its changes on surface dehydroxylation and reconstruction. Because our technique is all-optical and interface specific, it is equally applicable to oxide surfaces in vacuum, ambient atmospheres and at the solid/liquid interface. Application of this approach to additional alumina surfaces and other oxides thus seems likely to significantly expand our understanding of how water meets oxide surfaces and thus the wide variety of phenomena this interaction controls. (C) 2015 AIP Publishing LLC.show moreshow less

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Metadaten
Author:Yujin Tong, Jonas Wirth, Harald Kirsch, Martin Wolf, Peter SaalfrankORCiDGND, R. Kramer Campen
DOI:https://doi.org/10.1063/1.4906346
ISSN:0021-9606 (print)
ISSN:1089-7690 (online)
Pubmed Id:http://www.ncbi.nlm.nih.gov/pubmed?term=25662657
Parent Title (English):The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr
Publisher:American Institute of Physics
Place of publication:Melville
Document Type:Article
Language:English
Year of first Publication:2015
Year of Completion:2015
Release Date:2017/03/27
Volume:142
Issue:5
Pagenumber:12
Funder:Deutsche Forschungsgemeinschaft through Collaborative Research Center 1109: Understanding of Metal Oxide/Water Systems at the Molecular Scale: Structural Evolution, Interfaces and Dissolution
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Peer Review:Referiert