Comprehensive study on critical role of surface oxygen vacancies for 2DEG formation and annihilation in LaAlO3/SrTiO3 heterointerfaces

Here we report comprehensive study of 2DEG at a-LAO/STO interfaces in comparison with 2DEG at crystalline LaAlO3 (c-LAO)/STO interfaces. We observe that the oxygen deficient environment during the deposition of LAO overlayer is essentially required to create 2DEG at LAO/STO interface regardless of growth temperature from 25°C to 700°C, indicating that the oxygen-poor condition in the system is more important than the crystallinity of LAO layer. The critical thickness (2.6 nm) of 2DEG formation at a-LAO/STO heterostructure is thicker than (1.6 nm) that at c-LAO/STO. Upon ex-situ annealing at 300°C under 300 mTorr of oxygen pressure, 2DEG at a-LAO/STO interface is annihilated, while that in c-LAO/STO interface is still maintained. With combing these findings and scanning transmission electron microscope (STEM) analysis, we suggest that oxygen vacancies at the LAO surface is attributed to the origin of 2DEG formation at the LAO/STO and the crystallinity of the LAO overlayer plays a critical role in the annihilation of 2DEG at a-LAO/STO interface rather than in the formation of 2DEG. This work provides a framework to understand the importance of prohibiting the LAO surface from being oxidized for achieving thermally stable 2DEG at a-LAO/STO interface.