MoS2 and related metal dichalcogenides (MoSe2, WS2, WSe2) are layered two-dimensional materials that are promising for nanoelectronics and spintronics. For instance, large spin-orbit coupling and spin splitting in the valence band of single layer (SL) MoS2 could lead to enhanced spin lifetimes and large spin Hall angles. Understanding the nature of the contacts is a critical first step for realizing spin injection and spin transport in MoS2. Here, we have investigated Co contacts to SL MoS2 and find that the Schottky barrier height can be significantly decreased with the addition of a thin oxide barrier (MgO). Further, we show that the barrier height can be reduced to zero by tuning the carrier density with back gate. Therefore, the MgO could simultaneously provide a tunnel barrier to alleviate conductance mismatch while minimizing carrier depletion near the contacts. Such control over the barrier height should allow for careful engineering of the contacts to realize spin injection in these materials.

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Abstract:Graphene is an attractive material for spintronics due to theoretical predictions of long spin lifetimes arising from low spin-orbit and hyperfine couplings. In experiments, however, spin lifetimes in single layer graphene (SLG) measured via Hanle effects are much shorter than expected theoretically. Thus, the origin of spin relaxation in SLG is a major issue for graphene spintronics. Despite extensive theoretical and experimental work addressing this question, there is still little clarity on the microscopic origin of spin relaxation. By using organic ligand-bound nanoparticles as charge reservoirs to tune mobility between 2700 and 12000 cm 2 /Vs, we successfully isolate the effect of charged impurity scattering on spin relaxation in SLG. Our results demonstrate that while charged impurities can greatly affect mobility, the spin lifetimes are not affected by charged impurity scattering. Keywords:graphene; spintronics; spin relaxation; mobility; charged impurity scattering 2 Single layer graphene (SLG) is a promising material for spintronics due to theoretical predictions of long spin lifetimes based on its low intrinsic spin-orbit and hyperfine couplings [1][2][3][4][5] . However, spin lifetimes measured in SLG spin valves are much shorter (0.05 -1.2 ns) 6-9 than predicted (100 ns -1 s) [1][2][3][4][5] . Thus, the origin of spin relaxation in SLG has become a central issue for graphene spintronics and has motivated intense theoretical and experimental studies. Theoretical studies of spin relaxation include impurity scattering 10 , ripples 5 , spin orbit domains 11,12 , and substrate effects 13 , while experimental studies have investigated contact-induced spin relaxation 7, 9, 14 , ripples 15 , band structure effects 6,14,16 , edge effects 7 and charged impurity scattering 6, 8 .However, apart from recognizing the requirement for high quality tunneling contacts to suppress contact-induced spin relaxation 9 , there is little clarity regarding the origin of spin relaxation. To address the situation, it is crucial to develop experimental techniques that systematically isolate the various microscopic sources of spin relaxation.In this work, we successfully isolate the effect of charged impurity scattering on spin relaxation in SLG by exploiting the novel tunable mobility imparted by organic ligand-bound nanoparticles on the SLG surface 17 . The nanoparticles act as charge reservoirs that freely transfer charge with graphene at room temperature. At low temperature, the frozen charge distribution on the nanoparticles results in SLG mobility ranging from 2700 to 12000 cm 2 /Vs. This approach is able to isolate the effect of charged impurity scattering on spin relaxation more clearly than previous investigations based on adatom deposition 8 . This is because depositing adatoms to the graphene surface could introduce additional effects such as short-range scattering, lattice deformation, and/or spin-orbit coupling, whereas such effects should be minimized in the current approach. Additionally, we utilize tunne...

We have systematically introduced charged impurity scatterers in the form of Mg adsorbates to exfoliated single layer graphene and observe little variation of the spin relaxation times despite pronounced changes in the charge transport behavior. All measurements are performed on non-local graphene tunneling spin valves exposed in-situ to Mg adatoms, thus systematically introducing atomic-scale charged impurity scattering. While charge transport properties exhibit decreased mobility and decreased momentum scattering times, the observed spin lifetimes are not significantly affected indicating that charged impurity scattering is inconsequential in the present regime of spin relaxation times (∼1 ns).

Magnetism in graphene is an emerging field that has received much theoretical attention. In particular, there have been exciting predictions for induced magnetism through proximity to a ferromagnetic insulator as well as through localized dopants and defects. Here, we discuss our experimental work using molecular beam epitaxy (MBE) to modify the surface of graphene and induce novel spin-dependent phenomena. First, we investigate the epitaxial growth the ferromagnetic insulator EuO on graphene and discuss possible scenarios for realizing exchange splitting and exchange fields by ferromagnetic insulators. Second, we investigate the properties of magnetic moments in graphene originating from localized p z -orbital defects (i.e. adsorbed hydrogen atoms). The behavior of these magnetic moments is studied using non-local spin transport to directly probe the spin-degree of freedom of the defect-induced states. We also report the presence of enhanced electron g-factors caused by the exchange fields present in the system. Importantly, the exchange field is found to be highly gate dependent, with decreasing g-factors with increasing carrier densities.