Oxygen control of atomic structure and physical properties of SrRuO3 surfaces.

Abstract

Complex oxide thin films and heterostructures have become one of the foci for condensed matter physics research due to a broad variety of properties they exhibit. Similar to the bulk, properties of oxide surfaces can be expected to be strongly affected by oxygen stoichiometry. Here we explore the coupling between atomic structure and physical properties of SrRuO3 (SRO), one of the most well-studied oxide materials. We perform a detailed in situ and ex situ experimental investigation of the surfaces of SRO thin films using a combination of scanning tunneling microscopy (STM), X-ray and ultraviolet photoelectron spectroscopy, SQUID magnetometry, and magnetotransport measurements, as well as ab initio modeling. A number of remarkable linear surface reconstructions were observed by STM and interpreted as oxygen adatoms, favorably adsorbed in a regular rectangular or zigzag patterns. The degree of oxygen coverage and different surface patterns change the work function of the thin films, and modify local electronic and magnetic properties of the topmost atomic layer. The ab initio modeling reveals that oxygen adatoms possess frustrated local spin moments with possible spin-glass behavior of the surface covered by adsorbed oxygen. Additionally, the modeling indicates presence of a pseudo gap on the topmost SrO layer on pristine SrO-terminated surface, suggesting possibility for realization of a surface half-metallic film.