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Register a new userDirectional Interlayer Spin-Valley Transfer in Two-Dimensional Heterostructures
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Van der Waals heterostructures formed by two different monolayer semiconductors have emerged as a promising platform for new optoelectronic and spin/valleytronic applications. In addition to its atomically thin nature, a two-dimensional semiconductor heterostructure is distinct from its three-dimensional counterparts due to the unique coupled spin-valley physics of its constituent monolayers. Here, we report the direct observation that an optically generated spin-valley polarization in one monolayer can be transferred between layers of a two-dimensional MoSe2-WSe2 heterostructure. Using nondegenerate optical circular dichroism spectroscopy, we show that charge transfer between two monolayers conserves spin-valley polarization and is only weakly dependent on the twist angle between layers. Our work points to a new spin-valley pumping scheme in nanoscale devices, provides a fundamental understanding of spin-valley transfer across the two-dimensional interface, and shows the potential use of two-dimensional semiconductors as a spin-valley generator in 2D spin/valleytronic devices for storing and processing information.
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Moire superlattices provide a powerful way to engineer properties of electrons and excitons in two-dimensional van der Waals heterostructures. The moire effect can be especially strong for interlayer excitons, where electrons and holes reside in different layers and can be addressed separately. In particular, it was recently proposed that the moire superlattice potential not only localizes interlayer exciton states at different superlattice positions, but also hosts an emerging moire quasi-angular momentum (QAM) that periodically switches the optical selection rules for interlayer excitons at different moire sites. Here we report the observation of multiple interlayer exciton states coexisting in a WSe2/WS2 moire superlattice and unambiguously determine their spin, valley, and moire QAM through novel resonant optical pump-probe spectroscopy and photoluminescence excitation spectroscopy. We demonstrate that interlayer excitons localized at different moire sites can exhibit opposite optical selection rules due to the spatially-varying moire QAM. Our observation reveals new opportunities to engineer interlayer exciton states and valley physics with moire superlattices for optoelectronic and valleytronic applications.
Two dimensional heterostructures are likely to provide new avenues for the manipulation of magnetization that is crucial for spintronics or magnetoelectronics. Here, we demonstrate that optical spin pumping can generate a large effective magnetic field in two dimensional MoSe2/WSe2 heterostructures. We determine the strength of the generated field by polarization-resolved measurement of the interlayer exciton photoluminescence spectrum: the measured splitting exceeding 10 milli-electron volts (meV) between the emission originating from the two valleys corresponds to an effective magnetic field of ~ 30 T. The strength of this optically induced field can be controlled by the excitation light polarization. Our finding opens up new possibilities for optically controlled spintronic devices based on van der Waals heterostructures.
Van der Waals heterostructures give access to a wide variety of new phenomena that emerge thanks to the combination of properties brought in by the constituent layered materials. We show here that owing to an enhanced interaction cross section with electrons in a type I van der Waals heterostructure, made of single layer molybdenum disulphide and thin boron nitride films, electrons and holes created in boron nitride can be transferred to the dichalcogenide where they form electron-hole pairs yielding luminescence. This cathodoluminescence can be mapped with a spatial resolution far exceeding what can be achieved in a typical photoluminescence experiment, and is highly valuable to understand the optoelectronic properties at the nanometer scale. We find that in heterostructures prepared following the mainstream dry transfer technique, cathodoluminescence is locally extinguished, and we show that this extinction is associated with the formation of defects, that are detected in Raman spectroscopy and photoluminescence. We establish that to avoid defect formation induced by low-energy electron beams and to ensure efficient transfer of electrons and holes at the interface between the layers, flat and uniform interlayer interfaces are needed, that are free of trapped species, airborne ones or contaminants associated with sample preparation. We show that heterostructure fabrication using a pick-up technique leads to superior, intimate interlayer contacts associated with significantly more homogeneous cathodoluminescence.
Tunable magnetic interactions in high-mobility nonmagnetic semiconductor heterostructures are centrally important to spin-based quantum technologies. Conventionally, this requires incorporation of magnetic impurities within the two-dimensional (2D) electron layer of the heterostructures, which is achieved either by doping with ferromagnetic atoms, or by electrostatically printing artificial atoms or quantum dots. Here we report experimental evidence of a third, and intrinsic, source of localized spins in high-mobility GaAs/AlGaAs heterostructures, which are clearly observed in the limit of large setback distance (=80 nm) in modulation doping. Local nonequilibrium transport spectroscopy in these systems reveals existence of multiple spins, which are located in a quasi-regular manner in the 2D Fermi sea, and mutually interact at temperatures below 100 milliKelvin via the Ruderman-Kittel-Kasuya-Yosida (RKKY) indirect exchange. The presence of such a spin-array, whose microscopic origin appears to be disorder-bound, simulates a 2D lattice-Kondo system with gate-tunable energy scales.
Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and triplet interlayer excitons show giant valley-Zeeman splitting between the K and K valleys, a result of the large Lande g-factor of the singlet interlayer exciton and triplet interlayer exciton, which are experimentally determined to be ~ 10.7 and ~ 15.2, respectively, in good agreement with theoretical expectation. The PL from the singlet and triplet interlayer excitons show opposite helicities, determined by the atomic registry. Helicity-resolved photoluminescence excitation (PLE) spectroscopy study shows that both singlet and triplet interlayer excitons are highly valley-polarized at the resonant excitation, with the valley polarization of the singlet interlayer exciton approaches unity at ~ 20 K. The highly valley-polarized singlet and triplet interlayer excitons with giant valley-Zeeman splitting inspire future applications in spintronics and valleytronics.
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