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Giant Valley Splitting in Monolayer WS2 by Magnetic Proximity Effect (1902.05910v1)

Published 15 Feb 2019 in cond-mat.mes-hall

Abstract: Lifting the valley degeneracy of monolayer transition metal dichalcogenides (TMD) would allow versatile control of the valley degree of freedom. We report a giant valley exciton splitting of 18 meV/T for monolayer WS2, using the proximity effect from a ferromagnetic EuS substrate, which is enhanced by nearly two orders of magnitude from the 0.2 meV/T obtained by an external magnetic field. More interestingly, a sign reversal of the valley exciton splitting is observed as compared to that of WSe2 on EuS. Using first principles calculations, we investigate the complex behavior of exchange interactions between TMDs and EuS, that is qualitatively different from the Zeeman effect. The sign reversal is attributed to competing ferromagnetic (FM) and antiferromagnetic (AFM) exchange interactions for Eu- and S- terminated EuS surface sites. They act differently on the conduction and valence bands of WS2 compared to WSe2. Tuning the sign and magnitude of the valley exciton splitting offers opportunities for versatile control of valley pseudospin for quantum information processing.

Citations (189)

Summary

Giant Valley Splitting in Monolayer WS₂ by Magnetic Proximity Effect

This paper presents a robust analysis of valley exciton splitting in monolayers of transition metal dichalcogenides (TMDs), specifically focusing on WS₂, with magnetic proximity effects as the principal mechanism under examination. This mechanism substantially lifts valley degeneracy—in this instance, by 18 meV/T, which is almost two orders of magnitude above the 0.2 meV/T achieved by external magnetic fields. The researchers utilized first-principles calculations to probe the exchange interactions, attributing the noted reversal in sign of valley exciton splitting in WS₂, when juxtaposed with WSe₂, to the interaction dynamics between ferromagnetic (FM) and antiferromagnetic (AFM) states on the EuS substrate.

Key Findings

  • Valley Splitting Magnitude: The research explains that magnetic proximity enabled by EuS substrates can achieve a valley exciton splitting of 18 meV/T in WS₂, showcasing a stark contrast to the nominal 0.2 meV/T changes induced by external magnetic fields.
  • Sign Reversal: The paper identifies a sign reversal in valley exciton splitting between WS₂ and WSe₂ when interfaced with EuS. Through density functional theory calculations, this is attributed to the contrasting interactions of FM and AFM forces contingent on whether Eu or S termination occurs at the EuS surface.
  • Nonlinear Behavior: Results revealed nonlinear ΔE vs. B field relationships in the WS₂/EuS heterostructure, with an initial slope of -18 meV/T at low field strengths, illustrating a significant departure from linear Zeeman effect patterns seen on non-magnetic substrates.

Methodological Insights

The researchers employed magneto-reflectance spectroscopy to probe excitonic responses, calculating valley exciton shifts via the energy transitions at K and Kʹ valleys under variable magnetic field conditions. Their computational approach leverages density functional theory (DFT) to assess exchange interactions at the EuS-TMD interface, differing markedly from classic Zeeman effects in that it allows for magnetically tunable characteristics dependent on specific TMD-magnetic substrate pairings.

Implications and Future Directions

The paper highlights significant implications for quantum information processing, leveraging the tunable nature of the valley exciton splitting not just in magnitude but also in sign, allowing for more comprehensive control over valley pseudospins. Future prospects include the exploration of other TMD and magnetic substrate combinations to attain varied band alignments, further optimizing the valleytronic device applications.

The research also posits potential technological relevance in the ability to selectively control valley polarization using optical and electronic means. The robust correlation between magnetization of EuS and valley exciton splitting across various temperatures underlines the potential of integrating 2D magnetic materials with TMDs for advanced valleytronic applications. The paper suggests that combining these heterostructures with recent discoveries in 2D ferromagnetic materials could open new frontiers in information processing technologies.

Conclusion

The authors have elucidated a comprehensive framework for understanding and manipulating valley exciton behaviors using magnetic proximity effects in monolayer TMDs. This research not only aligns with contemporary interests in advancing spintronic and valleytronic technologies but also opens avenues for more tailored material design in heterostructures, pivotal for next-generation quantum computing and information applications.