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تسجيل مستخدم جديدEnhanced valley splitting in monolayer WSe2 due to magnetic exchange field
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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 broken inversion symmetry possesses two degenerate yet inequivalent valleys, offering unique opportunities for valley control through 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). 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 magneto-reflectance measurements. Moreover, the splitting follows the magnetization of EuS, a hallmark of the MEF. Utilizing MEF of a magnetic insulator can induce magnetic order, and valley and spin polarization in TMDCs, which may enable valleytronic and quantum computing applications.
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Local energy extrema of the bands in momentum space, or valleys, can endow electrons in solids with pseudo-spin in addition to real spin. In transition metal dichalcogenides this valley pseudo-spin, like real spin, is associated with a magnetic momen
t which underlies the valley-dependent circular dichroism that allows optical generation of valley polarization, intervalley quantum coherence, and the valley Hall effect. However, magnetic manipulation of valley pseudospin via this magnetic moment, analogous to what is possible with real spin, has not been shown before. Here we report observation of the valley Zeeman splitting and magnetic tuning of polarization and coherence of the excitonic valley pseudospin, by performing polarization-resolved magneto-photoluminescence on monolayer WSe2. Our measurements reveal both the atomic orbital and lattice contributions to the valley orbital magnetic moment; demonstrate the deviation of the band edges in the valleys from an exact massive Dirac fermion model; and reveal a striking difference between the magnetic responses of neutral and charged valley excitons which is explained by renormalization of the excitonic spectrum due to strong exchange interactions.
Atomically thin crystals of transition metal dichalcogenides are ideally suited to study the interplay of light-matter coupling, polarization and magnetic field effects. In this work, we investiagte the formation of exciton-polaritons in a MoSe2 mono
layer, which is integrated in a fully-grown, monolithic microcavity. Due to the narrow linewidth of the polaritonic resonances, we are able to directly investigate the emerging valley Zeeman splitting of the hybrid light-matter resonances in the presence of a magnetic field. At a detuning of -54.5 meV (13.5 % matter constituent of the lower polariton branch), we find a Zeeman splitting of the lower polariton branch of 0.36 meV, which can be directly associated with an excitonic g factor of 3.94pm0.13. Remarkably, we find that a magnetic field of 6T is sufficient to induce a notable valley polarization of 15 % in our polariton system, which approaches 30% at 9T. Strikingly, this circular polarization degree of the polariton (ground) state exceeds the polarization of the exciton reservoir for equal magnetic field magnitudes by approximately 50%, as a consequence of enhanced relaxation of bosons in our monolayer-based system.
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.
Due to degeneracies arising from crystal symmetries, it is possible for electron states at band edges (valleys) to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseud
ospins, analogous to that routinely implemented using true spin, in the quest for quantum technologies. Here we show for the first time that SU(2) valley coherence can indeed be generated and detected. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley excitons and trions. We then reveal coherence between valley excitons through the observation of linearly polarized luminescence, whose orientation always coincides with that of any linearly polarized excitation. Since excitons in a single valley emit circularly polarized photons, linear polarization can only be generated through recombination of an exciton in a coherent superposition of the two valleys. In contrast, the corresponding photoluminescence from trions is not linearly polarized, consistent with the expectation that the emitted photon polarization is entangled with valley pseudospin. The ability to address coherence, in addition to valley polarization, adds a critical dimension to the quantum manipulation of valley index necessary for coherent valleytronics.
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