Partial dissociation of water on Fe${}_3$O${}_4$(001): adsorbate induced charge and orbital order

Abstract

The interaction of water with Fe${}_3$O${}_4$(001) is studied by density functional theory (DFT) calculations including an on-site Coulomb term. For isolated molecules dissociative adsorption is strongly promoted at surface defect sites, while at higher coverages a hydrogen-bonded network forms with alternating molecular and dissociated species. This mixed adsorption mode and a suppression of the $(\sqrt{2}\times \sqrt{2})R45^{\circ }$-reconstruction are confirmed by a quantitative low energy electron diffraction (LEED) analysis. Adsorbate induced electron transfer processes add a new dimension towards understanding the catalytic activity of magnetite(001).

arXiv comment5 pages, 4 figures; Physical Review Letters, in press

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• Charge and orbital order in Fe_3O_4
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• An efficient way to model complex magnetite: assessment of SCC-DFTB against DFT
• Oxygen vacancy induced site-selective mott transition in lanio3
• Self-limited Growth of an Oxyhydroxide Phase at the Fe3O4(001) Surface in Liquid and Ambient Pressure Water
• Order-disorder phase transition on the (100) surface of magnetite
• Competition of defect ordering and site disproportionation in strained LaCoO${}_3$ on SrTiO${}_3$(001)
• Insight into the interface between Fe${}_3$O${}_4$(001) surface and water overlayers through multiscale molecular dynamics simulations
• Parametrization of the Fe-Owater cross-interaction for a more accurate Fe3O4/water interface model and its application to a spherical Fe3O4 nanoparticle of realistic size
• Mechanism of spin ordering in Fe${}_3$O${}_4$ nanoparticles by surface coating with organic acids