Two-dimensional semiconductors such as MoS2 are an emerging material family with wide-ranging potential applications in electronics, optoelectronics, and energy harvesting. Large-area growth methods are needed to open the way to applications. Control over lattice orientation during growth remains a challenge. This is needed to minimize or even avoid the formation of grain boundaries, detrimental to electrical, optical, and mechanical properties of MoS2 and other 2D semiconductors. Here, we report on the growth of high-quality monolayer MoS2 with control over lattice orientation. We show that the monolayer film is composed of coalescing single islands with limited numbers of lattice orientation due to an epitaxial growth mechanism. Optical absorbance spectra acquired over large areas show significant absorbance in the high-energy part of the spectrum, indicating that MoS2 could also be interesting for harvesting this region of the solar spectrum and fabrication of UV-sensitive photodetectors. Even though the interaction between the growth substrate and MoS2 is strong enough to induce lattice alignment via van der Waals interaction, we can easily transfer the grown material and fabricate devices. Local potential mapping along channels in field-effect transistors shows that the single-crystal MoS2 grains in our film are well connected, with interfaces that do not degrade the electrical conductivity. This is also confirmed by the relatively large and length-independent mobility in devices with a channel length reaching 80 μm.

The band structure of transition metal dichalcogenides (TMDCs) with valence band edges at different locations in the momentum space could be harnessed to build devices that operate relying on the valley degree of freedom. To realize such valleytronic devices, it is necessary to control and manipulate the charge density in these valleys, resulting in valley polarization. While this has been demonstrated using optical excitation, generation of valley polarization in electronic devices without optical excitation remains difficult. Here, we demonstrate spin injection from a ferromagnetic electrode into a heterojunction based on monolayers of WSe2 and MoS2 and lateral transport of spin-polarized holes within the WSe2 layer. The resulting valley polarization leads to circularly polarized light emission that can be tuned using an external magnetic field. This demonstration of spin injection and magnetoelectronic control over valley polarization provides a new opportunity for realizing combined spin and valleytronic devices based on spin-valley locking in semiconducting TMDCs.

The observation of micrometer size spin relaxation makes graphene a promising material for applications in spintronics requiring long-distance spin communication. However, spin dependent scatterings at the contact/graphene interfaces affect the spin injection efficiencies and hence prevent the material from achieving its full potential. While this major issue could be eliminated by nondestructive direct optical spin injection schemes, graphene’s intrinsically low spin–orbit coupling strength and optical absorption place an obstacle in their realization. We overcome this challenge by creating sharp artificial interfaces between graphene and WSe2 monolayers. Application of circularly polarized light activates the spin-polarized charge carriers in the WSe2 layer due to its spin-coupled valley-selective absorption. These carriers diffuse into the superjacent graphene layer, transport over a 3.5 μm distance, and are finally detected electrically using Co/h-BN contacts in a nonlocal geometry. Polarization-dependent measurements confirm the spin origin of the nonlocal signal. We also demonstrate that such signal is absent if graphene is contacted to bilayer WSe2 where the inversion symmetry is restored.

Transition metal dichalcogenides (TMDCs), together with other two-dimensional (2D) materials, have attracted great interest due to the unique optical and electrical properties of atomically thin layers. In order to fulfill their potential, developing large-area growth and understanding the properties of TMDCs have become crucial. Here, we have used molecular beam epitaxy (MBE) to grow atomically thin MoSe2 on GaAs(111)B. No intermediate compounds were detected at the interface of as-grown films. Careful optimization of the growth temperature can result in the growth of highly aligned films with only two possible crystalline orientations due to broken inversion symmetry. As-grown films can be transferred onto insulating substrates, allowing their optical and electrical properties to be probed. By using polymer electrolyte gating, we have achieved ambipolar transport in MBE-grown MoSe2. The temperature-dependent transport characteristics can be explained by the 2D variable-range hopping (2D-VRH) model, indicating that the transport is strongly limited by the disorder in the film.

We report on the growth of molybdenum disulphide (MoS 2 ) using H 2 S as a gas-phase sulfur precursor that allows controlling the domain growth direction of domains in both vertical (perpendicular to the substrate plane) and horizontal (within the substrate plane), depending on the H 2 S:H 2 ratio in the reaction gas mixture and temperature at which they are introduced during growth. Optical and atomic force microscopy measurements on horizontal MoS 2 demonstrate the formation of monolayer triangular-shape domains that merge into a continuous film. Scanning transmission electron microscopy of monolayer MoS 2 shows a regular atomic structure with a hexagonal symmetry. Raman and photoluminescence spectra confirm the monolayer thickness of the material. Field-effect transistors fabricated on MoS 2 domains that are transferred onto Si/SiO 2 substrates show a mobility similar to previously reported exfoliated and chemical vapor deposition-grown materials.

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