The realization of long-range ferromagnetic order in two-dimensional van der Waals crystals, combined with their rich electronic and optical properties, could lead to new magnetic, magnetoelectric and magneto-optic applications. In two-dimensional systems, the long-range magnetic order is strongly suppressed by thermal fluctuations, according to the Mermin-Wagner theorem; however, these thermal fluctuations can be counteracted by magnetic anisotropy. Previous efforts, based on defect and composition engineering, or the proximity effect, introduced magnetic responses only locally or extrinsically. Here we report intrinsic long-range ferromagnetic order in pristine CrGeTe atomic layers, as revealed by scanning magneto-optic Kerr microscopy. In this magnetically soft, two-dimensional van der Waals ferromagnet, we achieve unprecedented control of the transition temperature (between ferromagnetic and paramagnetic states) using very small fields (smaller than 0.3 tesla). This result is in contrast to the insensitivity of the transition temperature to magnetic fields in the three-dimensional regime. We found that the small applied field leads to an effective anisotropy that is much greater than the near-zero magnetocrystalline anisotropy, opening up a large spin-wave excitation gap. We explain the observed phenomenon using renormalized spin-wave theory and conclude that the unusual field dependence of the transition temperature is a hallmark of soft, two-dimensional ferromagnetic van der Waals crystals. CrGeTe is a nearly ideal two-dimensional Heisenberg ferromagnet and so will be useful for studying fundamental spin behaviours, opening the door to exploring new applications such as ultra-compact spintronics.

Magnetism, originating from the moving charges and spin of elementary particles, has revolutionized important technologies such as data storage and biomedical imaging, and continues to bring forth new phenomena in emergent materials and reduced dimensions. The recently discovered two-dimensional (2D) magnetic van der Waals crystals provide ideal platforms for understanding 2D magnetism, the control of which has been fueling opportunities for atomically thin, flexible magneto-optic and magnetoelectric devices (such as magnetoresistive memories and spin field-effect transistors). The seamless integration of 2D magnets with dissimilar electronic and photonic materials opens up exciting possibilities for unprecedented properties and functionalities. We review the progress in this area and identify the possible directions for device applications, which may lead to advances in spintronics, sensors, and computing.

Density functional theory calculations are performed to unravel the nature of the contact between metal electrodes and monolayer MoS2. Schottky barriers are shown to be present for a variety of metals with the work functions spanning over 4.2-6.1 eV. Except for the p-type Schottky contact with platinum, the Fermi levels in all of the studied metal-MoS2 complexes are situated above the midgap of MoS2. The mechanism of the Fermi level pinning at metal-MoS2 contact is shown to be unique for metal-2D-semiconductor interfaces, remarkably different from the well-known Bardeen pinning effect, metal-induced gap states, and defect/disorder induced gap states, which are applicable to traditional metal-semiconductor junctions. At metal-MoS2 interfaces, the Fermi level is partially pinned as a result of two interface behaviors: first by a metal work function modification by interface dipole formation due to the charge redistribution, and second by the production of gap states mainly of Mo d-orbitals character by the weakened intralayer S-Mo bonding due to the interface metal-S interaction. This finding would provide guidance to develop approaches to form Ohmic contact to MoS2.

12Tunnel field effect transistors (TFETs) based on vertical stacking of two dimensional materials are 13 of interest for low-power logic devices. The monolayer transition metal dichalcogenides (TMDs) 14 with sizable band gaps show promise in building p-n junctions (couples) for TFET applications.

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A detailed in situ infrared spectroscopy analysis of single layer and multilayered graphene oxide (GO) thin films reveals that the normalized infrared absorption in the carbonyl region is substantially higher in multilayered GO upon mild annealing. These results highlight the fact that the reduction chemistry of multilayered GO is dramatically different from the single layer GO due to the presence of water molecules confined in the ∼1 nm spacing between sheets. IR spectroscopy, XPS analysis, and DFT calculations all confirm that the water molecules play a significant role interacting with basal plane etch holes through passivation, via evolution of CO(2) leading to the formation of ketone and ester carbonyl groups. Displacement of water from intersheet spacing with alcohol significantly changes the chemistry of carbonyl formation with temperature.

Metal-graphene contact is a key interface in graphene-based device applications, and it is known that two types of interfaces are formed between metal and graphene. In this paper, we apply first-principles calculations to twelve metal-graphene interfaces and investigate the detailed interface atomic and electronic structures of physisorption and chemisorption interfaces. For physisorption interfaces ͑Ag, Al, Cu, Cd, Ir, Pt, and Au͒, Fermi level pinning and Pauli-exclusion-induced energy-level shifts are shown to be two primary factors determining graphene's doping types and densities. For chemisorption interfaces ͑Ni, Co, Ru, Pd, and Ti͒, the combination of Pauli-exclusion-induced energy-level shifts and hybridized states' repulsive interactions lead to a band gap opening with metallic gap states. For practical applications, we show that external electric field can be used to modulate graphene's energy-levels and the corresponding control of doping or energy range of hybridization.

The understanding of the metal and transition metal dichalcogenide (TMD) interface is critical for future electronic device technologies based on this new class of two-dimensional semiconductors. Here, we investigate the initial growth of nanometer-thick Pd, Au, and Ag films on monolayer MoS2. Distinct growth morphologies are identified by atomic force microscopy: Pd forms a uniform contact, Au clusters into nanostructures, and Ag forms randomly distributed islands on MoS2. The formation of these different interfaces is elucidated by large-scale spin-polarized density functional theory calculations. Using Raman spectroscopy, we find that the interface homogeneity shows characteristic Raman shifts in E2g(1) and A1g modes. Interestingly, we show that insertion of graphene between metal and MoS2 can effectively decouple MoS2 from the perturbations imparted by metal contacts (e.g., strain), while maintaining an effective electronic coupling between metal contact and MoS2, suggesting that graphene can act as a conductive buffer layer in TMD electronics.