The choice and quality of single-crystal substrates for epitaxial thin film growth drastically influence the properties of the synthesized films. Among them, high-quality substrates with a polar surface are particularly difficult to prepare due to their inherent structural instability against electrostatic forces of the polar discontinuity. As a commonly used insulating substrate, the (111) cut of MgO shows alternating planes of Mg2+ and O2− that form a hexagonal unit cell at the surface, which is useful for thin films with similar crystal symmetries. We present a method to prepare such a surface by first introducing (3×3)R30° reconstructed MgO (111) surface via face-to-face annealing in an O2 environment. We then dissolve the top layers in acid to achieve an unreconstructed and also passivated surface. The structure, stoichiometry, and stability of the resulting surfaces are characterized. This work provides an easy and reliable way to prepare a MgO (111) polar surface ready for subsequent epitaxial growth.

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