Graphene on two-dimensional hexagonal BN, AlN, and GaN: Electronic, spin-orbit, and spin relaxation properties

Abstract

We investigate the electronic structure of graphene on a series of 2D hexagonal nitride insulators hXN, X = B, Al, and Ga, with DFT calculations. A symmetry-based model Hamiltonian is employed to extract orbital parameters and spin-orbit coupling (SOC) from the low-energy Dirac bands of proximitized graphene. While commensurate hBN induces a staggered potential of about 10 meV into the Dirac bands, less lattice-matched hAlN and hGaN disrupt the Dirac point much less, giving a staggered gap below 100 $\mu$eV. Proximitized intrinsic SOC surprisingly does not increase much above the pristine graphene value of 12 $\mu$eV; it stays in the window of (1-16) $\mu$eV, depending strongly on stacking. However, Rashba SOC increases sharply when increasing the atomic number of the boron group, with calculated maximal values of 8, 15, and 65 $\mu$eV for B, Al, and Ga-based nitrides, respectively. The individual Rashba couplings also depend strongly on stacking, vanishing in symmetrically-sandwiched structures, and can be tuned by a transverse electric field. The extracted spin-orbit parameters were used as input for spin transport simulations based on Chebyshev expansion of the time-evolution of the spin expectation values, yielding interesting predictions for the electron spin relaxation. Spin lifetime magnitudes and anisotropies depend strongly on the specific (hXN)/graphene/hXN system, and they can be efficiently tuned by an applied external electric field as well as the carrier density in the graphene layer. A particularly interesting case for experiments is graphene/hGaN, in which the giant Rashba coupling is predicted to induce spin lifetimes of 1-10 ns, short enough to dominate over other mechanisms, and lead to the same spin relaxation anisotropy as observed in conventional semiconductor heterostructures: 50\%, meaning that out-of-plane spins relax twice as fast as in-plane spins.