Nanosecond spin lifetimes in bottom-up fabricated bilayer graphene spin-valves with atomic layer deposited Al₂O₃ spin injection and detection barriers

We present spin transport studies on bi- and trilayer graphene non-local spin-valves which have been fabricated by a bottom-up fabrication method. By this technique, spin injection electrodes are first deposited onto Si$^{++}$/SiO$_2$ substrates with subsequent mechanical transfer of a graphene/hBN heterostructure. We showed previously that this technique allows for nanosecond spin lifetimes at room temperature combined with carrier mobilities which exceed 20,000 cm$^2$/(Vs). Despite strongly enhanced spin and charge transport properties, the MgO injection barriers in these devices exhibit conducting pinholes which still limit the measured spin lifetimes. We demonstrate that these pinholes can be partially diminished by an oxygen treatment of a trilayer graphene device which is seen by a strong increase of the contact resistance area products of the Co/MgO electrodes. At the same time, the spin lifetime increases from 1 ns to 2 ns. We believe that the pinholes partially result from the directional growth in molecular beam epitaxy. For a second set of devices, we therefore used atomic layer deposition of Al$_2$O$_3$ which offers the possibility to isotropically deposit more homogeneous barriers. While the contacts of the as-fabricated bilayer graphene devices are non-conductive, we can partially break the oxide barriers by voltage pulses. Thereafter, the devices also exhibit nanosecond spin lifetimes.