Surface Chemistry of GaP(001) and InP(001) in Contact with Water

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• 作者：Brandon C. Wood ; Eric Schwegler ; Woon Ih Choi ; Tadashi Ogitsu
• 刊名：Journal of Physical Chemistry C
• 出版年：2014
• 出版时间：January 16, 2014
• 年：2014
• 卷：118
• 期：2
• 页码：1062-1070
• 全文大小：409K
• ISSN：1932-7455

文摘

We report the results of total-energy density functional theory and ab initio molecular dynamics simulations of (001) surfaces of InP and GaP in contact with gas-phase and liquid water. Both pristine and oxygen-rich surfaces (representing a submonolayer native surface oxide) are considered. We find that gas-phase binding of water on pristine mixed-dimer 未(2脳4) reconstructions of InP/GaP(001) is comparable to the solvation energy of liquid water, and that the barriers for room-temperature dissociation are high. In the presence of a submonolayer surface oxide, water binding and dissociation instead become strongly exothermic and proceed with almost no barrier. In this case, the surface chemistry at the interface with liquid water differs significantly from that of gas-phase water adsorption due to the formation of strong, low-barrier hydrogen bonds between surface adsorbates and water molecules. Water dissociation on the oxygen-rich surface is accompanied by extremely rapid local proton hopping between hydrogen-bonded surface adsorbates.