Ferromagnetism emerged from non-ferromagnetic atomic crystals.

The recently emerged ferromagnetic two-dimensional (2D) materials provide unique platforms for compact spintronic devices down to the atomic-thin regime; however, the prospect is hindered by the limited number  of ferromagnetic 2D materials discovered with limited choices of magnetic properties. If 2D antiferromagnetism could be converted to 2D ferromagnetism, the range of 2D magnets and their potential applications would be significantly broadened. Here, we discovered emergent ferromagnetism by interfacing non-magnetic WS2 layers with the antiferromagnetic FePS3. The WS2 exhibits an order of magnitude enhanced Zeeman effect with a saturated interfacial exchange field ~38 Tesla. Given the pristine FePS3 is an intralayer antiferromagnet, the prominent interfacial exchange field suggests the formation of ferromagnetic FePS3 at interface. Furthermore, the enhanced Zeeman effect in WS2 is found to exhibit a strong WS2-thickness dependence, highlighting the layer-tailorable interfacial exchange coupling in WS2-FePS3 heterostructures, which is potentially attributed to the thickness-dependent interfacial hybridization.

Giant valley splitting in monolayer WS2 by magnetic proximity effect.

Lifting the valley degeneracy of monolayer transition metal dichalcogenides (TMDs) would allow versatile control of the valley degree of freedom. We report a giant valley exciton splitting of 16 meV/T for monolayer WS2, using the proximity effect from an EuS substrate, which is enhanced by nearly two orders of magnitude from that obtained by an external magnetic field. More interestingly, a sign reversal of the valley 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. 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 control of valley pseudospin for quantum information processing.

Enhanced valley splitting in monolayer WSe2 due to magnetic exchange field.

Exploiting the valley degree of freedom to store and manipulate information provides a novel paradigm for future electronics. A monolayer transition-metal dichalcogenide (TMDC) with a broken inversion symmetry possesses two degenerate yet inequivalent valleys, which offers unique opportunities for valley control through the helicity of light. Lifting the valley degeneracy by Zeeman splitting has been demonstrated recently, which may enable valley control by a magnetic field. However, the realized valley splitting is modest (∼0.2 meV T-1). Here we show greatly enhanced valley spitting in monolayer WSe2, utilizing the interfacial magnetic exchange field (MEF) from a ferromagnetic EuS substrate. A valley splitting of 2.5 meV is demonstrated at 1 T by magnetoreflectance measurements and corresponds to an effective exchange field of ∼12 T. Moreover, the splitting follows the magnetization of EuS, a hallmark of the MEF. Utilizing the MEF of a magnetic insulator can induce magnetic order and valley and spin polarization in TMDCs, which may enable valleytronic and quantum-computing applications.