The high-mobility conducting interface (CI) between LaAlO3 (LAO) and SrTiO3 (STO) has revealed many fascinating phenomena, including exotic magnetism and superconductivity. But, the formation mechanism of the CI has not been conclusively explained. Here, using in situ angle-resolved photoemission spectroscopy, we elucidated the mechanisms for the CI formation. In as-grown samples, we observed a built-in potential (Vbi) proportional to the polar LAO thickness starting from the first unit cell (UC) with CI formation appearing above 3 UCs. However, we found that the Vbi is removed by synchrotron ultraviolet (UV)-irradiation; The built-in potential is recovered by oxygen gas (O2(g))-exposure. Furthermore, after UV-irradiation, the CI appears even below 3UC of LAO. Our results demonstrate not only the Vbi-driven CI formation in as-grown LAO/STO, but also a new route to control of the interface state by UV lithographic patterning or other surface modification.

Two-dimensional electron gases (2DEGs) on the SrTiO3 (STO) surface or in STO-based heterostructures have exhibited many intriguing phenomena, which are strongly dependent on the 2DEG-carrier density. We report that the tunability of the 2DEG-carrier density is significantly enhanced by adding a monolayer LaTiO3 (LTO) onto the STO. Ultraviolet (UV) irradiation induced maximum carrier density of the 2DEG in LTO/STO is increased by a factor of ~4 times, compared to that of the bare STO. By oxygen gas exposure, it becomes 10 times smaller than that of the bare STO. This enhanced tunability is attributed to the drastic surface property change of a polar LTO layer by UV irradiation and O2 exposure. This indicates that the 2DEG controllability in LTO/STO is more reliable than that on the bare STO driven by defects, such an oxygen vacancy.

Pristine, single-crystalline graphene displays a unique collection of remarkable electronic properties that arise from its two-dimensional, honeycomb structure. Using in situ low-energy electron microscopy, we show that when deposited on the (111) surface of Au carbon forms such a structure. The resulting monolayer, epitaxial film is formed by the coalescence of dendritic graphene islands that nucleate at a high density. Over 95% of these islands can be identically aligned with respect to each other and to the Au substrate. Remarkably, the dominant island orientation is not the better lattice-matched 30° rotated orientation but instead one in which the graphene [01] and Au [011] in-plane directions are parallel. The epitaxial graphene film is only weakly coupled to the Au surface, which maintains its reconstruction under the slightly p-type doped graphene. The linear electronic dispersion characteristic of free-standing graphene is retained regardless of orientation. That a weakly interacting, non-lattice matched substrate is able to lock graphene into a particular orientation is surprising. This ability, however, makes Au(111) a promising substrate for the growth of single crystalline graphene films.