2D nature of magnetic states at SnO2 surfaces: a combined experimental and theoretical study

Abstract

For undoped SnO₂, room temperature ferromagnetism could be seen uniquely in 2-dimensional configurations, particularly in ultra-thin films (whose thickness is ideally below 100 nm). Both bulk samples and nano-powders of pristine SnO₂ are diamagnetic, indicating that a 2D surface is a key point in shaping up the magnetic properties in SnO₂. As a complement to our experiments, we have performed a series of quantum-mechanical calculations for the bulk rutile-structure SnO₂ as well as its (001) and (101) surfaces. The calculations included several atomic configurations with and without vacancies in/under the studied surfaces. The stability of the non-magnetic ground state of rutile SnO₂ bulk was cross-checked and confirmed by its phonon spectrum computed within the harmonic approximation. Regarding the surfaces, the bulk-like (001) surface containing Sn vacancies has turned out to be ferromagnetic, while the shift of Sn vacancies under the surface resulted in a more complex ferrimagnetic state. The bulk-like (001) surface without vacancies and that with the O vacancies are predicted to be non-magnetic. Regarding the (101) surfaces, those terminated by a single layer of oxygen atoms and those terminated by tin atoms are non-magnetic, while a surface terminated by two layers of oxygen has turned out to be ferromagnetic.