This content will become publicly available on March 16, 2023

Electric fields and substrates dramatically accelerate spin relaxation in graphene
Electrons in graphene are theoretically expected to retain spin states much longer than most materials, making graphene a promising platform for spintronics and quantum information technologies. Here, we use first-principles density-matrix (FPDM) dynamics simulations to show that interaction with electric fields and substrates strongly enhances spin relaxation through scattering with phonons. Consequently, the relaxation time at room temperature reduces from microseconds in free-standing graphene to nanoseconds in graphene on the hexagonal boron nitride (hBN) substrate, which is the order of magnitude typically measured in experiments. Further, inversion symmetry breaking by hBN introduces a stronger asymmetry in electron and hole spin lifetimes than predicted by the conventional D'yakonov-Perel' (DP) model for spin relaxation. Deviations from the conventional DP model are stronger for in-plane spin relaxation, resulting in out-of-plane to in-plane lifetime ratios much greater than 1/2 with a maximum close to the Dirac point. These FPDM results, independent of symmetry-specific assumptions or material-dependent parameters, also validate recent modifications of the DP model to explain such deviations. Overall, our results indicate that spin-phonon relaxation in the presence of substrates may be more important in graphene than typically assumed, requiring consideration for graphene-based spin technologies at room temperature.
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Publication Date:
NSF-PAR ID:
10347316
Journal Name:
Physical review
Volume:
105
Page Range or eLocation-ID:
115122
ISSN:
2469-9985
The recently discovered spin-active boron vacancy (V$${}_{{{{{{{{\rm{B}}}}}}}}}^{-}$$${}_{B}^{-}$) defect center in hexagonal boron nitride (hBN) has high contrast optically-detected magnetic resonance (ODMR) at room-temperature, with a spin-triplet ground-state that shows promise as a quantum sensor. Here we report temperature-dependent ODMR spectroscopy to probe spin within the orbital excited-state. Our experiments determine the excited-state spin Hamiltonian, including a room-temperature zero-field splitting of 2.1 GHz and a g-factor similar to that of the ground-state. We confirm that the resonance is associated with spin rotation in the excited-state using pulsed ODMR measurements, and we observe Zeeman-mediated level anti-crossings in both the orbital ground- and excited-state. Our observation of a single set of excited-state spin-triplet resonance from 10 to 300 K is suggestive of symmetry-lowering of the defect system fromD3htoC2v. Additionally, the excited-state ODMR has strong temperature dependence of both contrast and transverse anisotropy splitting, enabling promising avenues for quantum sensing.