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Register a new userValley Manipulation by Optically Tuning the Magnetic Proximity Effect in WSe$_2$/CrI$_3$ Heterostructures
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Monolayer valley semiconductors, such as tungsten diselenide (WSe$_2$), possess valley pseudospin degrees of freedom that are optically addressable but degenerate in energy. Lifting the energy degeneracy by breaking time-reversal symmetry is vital for valley manipulation. This has been realized by directly applying magnetic fields or via pseudo-magnetic fields generated by intense circularly polarized optical pulses. However, sweeping large magnetic fields is impractical for devices, and the pseudo-magnetic fields are only effective in the presence of ultrafast laser pulses. The recent rise of two-dimensional (2D) magnets unlocks new approaches to control valley physics via van der Waals heterostructure engineering. Here we demonstrate wide continuous tuning of the valley polarization and valley Zeeman splitting with small changes in the laser excitation power in heterostructures formed by monolayer WSe$_2$ and 2D magnetic chromium triiodide (CrI$_3$). The valley manipulation is realized via optical control of the CrI$_3$magnetization, which tunes the magnetic exchange field over a range of 20 T. Our results reveal a convenient new path towards optical control of valley pseudospins and van der Waals magnetic heterostructures.
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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.
Monolayer transition metal dichalcogenides (TMDs) hold great promise for future information processing applications utilizing a combination of electron spin and valley pseudospin. This unique spin system has led to observation of the valley Zeeman effect in neutral and charged excitonic resonances under applied magnetic fields. However, reported values of the trion valley Zeeman splitting remain highly inconsistent across studies. Here, we utilize high quality hBN encapsulated monolayer WSe$_2$ to enable simultaneous measurement of both intervalley and intravalley trion photoluminescence. We find the valley Zeeman splitting of each trion state to be describable only by a combination of three distinct g-factors, one arising from the exciton-like valley Zeeman effect, the other two, trion specific, g-factors associated with recoil of the excess electron. This complex picture goes significantly beyond the valley Zeeman effect reported for neutral excitons, and eliminates the ambiguity surrounding the magneto-optical response of trions in tungsten based TMD monolayers.
The Hall effect can be extended by inducing a temperature gradient in lieu of electric field that is known as the Nernst (-Ettingshausen) effect. The recently discovered spin Nernst effect in heavy metals continues to enrich the picture of Nernst effect-related phenomena. However, the collection would not be complete without mentioning the valley degree of freedom benchmarked by the observation of the valley Hall effect. Here we show the experimental evidence of its missing counterpart, the valley Nernst effect. Using millimeter-sized WSe$_{2}$ mono-multi-layers and the ferromagnetic resonance-spin pumping technique, we are able to apply a temperature gradient by off-centering the sample in the radio frequency cavity and address a single valley through spin-valley coupling. The combination of a temperature gradient and the valley polarization leads to the valley Nernst effect in WSe$_{2}$ that we detect electrically at room temperature. The valley Nernst coefficient is in very good agreement with the predicted value.
Van der Waals heterostructures composed of multiple few layer crystals allow the engineering of novel materials with predefined properties. As an example, coupling graphene weakly to materials with large spin orbit coupling (SOC) allows to engineer a sizeable SOC in graphene via proximity effects. The strength of the proximity effect depends on the overlap of the atomic orbitals, therefore, changing the interlayer distance via hydrostatic pressure can be utilized to enhance the interlayer coupling between the layers. In this work, we report measurements on a graphene/WSe$_2$ heterostructure exposed to increasing hydrostatic pressure. A clear transition from weak localization to weak anti-localization is visible as the pressure increases, demonstrating the increase of induced SOC in graphene.
Magnetic proximity effects are crucial ingredients for engineering spintronic, superconducting, and topological phenomena in heterostructures. Such effects are highly sensitive to the interfacial electronic properties, such as electron wave function overlap and band alignment. The recent emergence of van der Waals (vdW) magnets enables the possibility of tuning proximity effects via designing heterostructures with atomically clean interfaces. In particular, atomically thin CrI3 exhibits layered antiferromagnetism, where adjacent ferromagnetic monolayers are antiferromagnetically coupled. Exploiting this magnetic structure, we uncovered a layer-resolved magnetic proximity effect in heterostructures formed by monolayer WSe2 and bi/trilayer CrI3. By controlling the individual layer magnetization in CrI3 with a magnetic field, we found that the spin-dependent charge transfer between WSe2 and CrI3 is dominated by the interfacial CrI3 layer, while the proximity exchange field is highly sensitive to the layered magnetic structure as a whole. These properties enabled us to use monolayer WSe2 as a spatially sensitive magnetic sensor to map out layered antiferromagnetic domain structures at zero magnetic field as well as antiferromagnetic/ferromagnetic domains near the spin-flip transition in bilayer CrI3. Our work reveals a new way to control proximity effects and probe interfacial magnetic order via vdW engineering.
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