TY - JOUR A1 - Tong, Yujin A1 - Wirth, Jonas A1 - Kirsch, Harald A1 - Wolf, Martin A1 - Saalfrank, Peter A1 - Campen, Richard Kramer T1 - Optically probing Al-O and O-H vibrations to characterize water adsorption and surface reconstruction on alpha-alumina: An experimental and theoretical study JF - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr N2 - 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. Y1 - 2015 U6 - https://doi.org/10.1063/1.4906346 SN - 0021-9606 SN - 1089-7690 VL - 142 IS - 5 PB - American Institute of Physics CY - Melville ER -