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Surfaces and interfaces of ferroelectric oxides exhibit enhancedfunctionality, and therefore serve as a platform for novel nano and quantumtechnologies. Experimental and theoretical challenges associated with examiningthe subtle electro-chemo-mechanical balance at metal-oxide surfaces havehindered the understanding and control of their structure and behavior. Here,we combine advanced electron-microscopy and first-principles thermodynamicsmethods to reveal the atomic-scale chemical and crystallographic structure ofthe surface of the seminal ferroelectric BaTiO3. We show that the surface iscomposed of a native < 2-nm thick TiOx rock-salt layer in epitaxial registrywith the BaTiO3. Using electron-beam irradiation, we successfully patternedartificially TiOx sites with sub-nanometer resolution, by inducing Ba escape.Therefore, our work offers electro-chemo-mechanical insights into ferroelectricsurface behavior in addition to a method for scalable high-resolutionbeam-induced chemical lithography for selectively driving surface phasetransitions, and thereby functionalizing metal-oxide surfaces.

Epitaxial TiOx Surface in Ferroelectric BaTiO3: Native Structure and Dynamic Patterning at the Atomic Scale