We have investigated the effects of low-energy ion beam irradiations using argon clusters on the chemical and electronic properties of LaAlO3/SrTiO3 (LAO/STO) heterointerfaces by combining X-ray photoelectron spectroscopy (XPS) and electrical transport measurements. Due to its unique features, we show that a short-time cluster ion irradiation of the LAO surface induces indirect modifications in the chemical properties of the buried STO substrate, with (1) a lowering of Ti atoms oxidation states (from Ti4+ to Ti3+ and Ti2+) correlated to the formation of oxygen vacancies at the LAO surface and (2) the creation of new surface states for Sr atoms. Contrary to what is observed by using higher energy ion beam techniques, this leads to an increase of the electrical conductivity at the LAO/STO interface. Our XPS data clearly reveal the existence of dynamical processes on the titanium and strontium atoms, which compete with the effect of the cluster ion beam irradiation. These relaxation effects are in part attributed to the diffusion of the ion-induced oxygen vacancies in the entire heterostructure, since an increase of the interfacial metallicity is also evidenced far from the irradiated area. These results demonstrate that a local perturbation of the LAO surface can induce new properties at the interface and in the entire heterostructure. This study highlights the possibility of tuning the electronic properties of LAO/STO interfaces by surface engineering, confirming experimentally the intimate connection between LAO surface chemistry and electronic properties of LAO/STO interfaces.
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