Magneto-optical Kerr effect microscopy is used to show that monolayer chromium triiodide is an Ising ferromagnet with out-of-plane spin orientation. The question of what happens to the properties of a material when it is thinned down to atomic-scale thickness has for a long time been a largely hypothetical one. In the past decade, new experimental methods have made it possible to isolate and measure a range of two-dimensional structures, enabling many theoretical predictions to be tested. But it has been a particular challenge to observe intrinsic magnetic effects, which could shed light on the longstanding fundamental question of whether intrinsic long-range magnetic order can robustly exist in two dimensions. In this issue of Nature, two groups address this challenge and report ferromagnetism in atomically thin crystals. Xiang Zhang and colleagues measured atomic layers of Cr2Ge2Te6 and observed ferromagnetic ordering with a transition temperature that, unusually, can be controlled using small magnetic fields. Xiaodong Xu and colleagues measured atomic layers of CrI3 and observed ferromagnetic ordering that, remarkably, was suppressed in double layers of CrI3, but restored in triple layers. The two studies demonstrate a platform with which to test fundamental properties of purely two-dimensional magnets. Since the discovery of graphene1, the family of two-dimensional materials has grown, displaying a broad range of electronic properties. Recent additions include semiconductors with spin–valley coupling2, Ising superconductors3,4,5 that can be tuned into a quantum metal6, possible Mott insulators with tunable charge-density waves7, and topological semimetals with edge transport8,9. However, no two-dimensional crystal with intrinsic magnetism has yet been discovered10,11,12,13,14; such a crystal would be useful in many technologies from sensing to data storage15. Theoretically, magnetic order is prohibited in the two-dimensional isotropic Heisenberg model at finite temperatures by the Mermin–Wagner theorem16. Magnetic anisotropy removes this restriction, however, and enables, for instance, the occurrence of two-dimensional Ising ferromagnetism. Here we use magneto-optical Kerr effect microscopy to demonstrate that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 kelvin is only slightly lower than that of the bulk crystal, 61 kelvin, which is consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phase, highlighting thickness-dependent physical properties typical of van der Waals crystals17,18,19. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect20, whereas in trilayer CrI3 the interlayer ferromagnetism observed in the bulk crystal is restored. This work creates opportunities for studying magnetism by harnessing the unusual features of atomically thin materials, such as electrical control for realizing magnetoelectronics12, and van der Waals engineering to produce interface phenomena15.

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Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit

Graphene is very popular because of its many fascinating properties, but its lack of an electronic bandgap has stimulated the search for 2D materials with semiconducting character. Transition metal dichalcogenides (TMDCs), which are semiconductors of the type MX2, where M is a transition metal atom (such as Mo or W) and X is a chalcogen atom (such as S, Se or Te), provide a promising alternative. Because of its robustness, MoS2 is the most studied material in this family. TMDCs exhibit a unique combination of atomic-scale thickness, direct bandgap, strong spin–orbit coupling and favourable electronic and mechanical properties, which make them interesting for fundamental studies and for applications in high-end electronics, spintronics, optoelectronics, energy harvesting, flexible electronics, DNA sequencing and personalized medicine. In this Review, the methods used to synthesize TMDCs are examined and their properties are discussed, with particular attention to their charge density wave, superconductive and topological phases. The use of TMCDs in nanoelectronic devices is also explored, along with strategies to improve charge carrier mobility, high frequency operation and the use of strain engineering to tailor their properties. Two-dimensional transition metal dichalcogenides (TMDCs) exhibit attractive electronic and mechanical properties. In this Review, the charge density wave, superconductive and topological phases of TMCDs are discussed, along with their synthesis and applications in devices with enhanced mobility and with the use of strain engineering to improve their properties.

2D transition metal dichalcogenides

The electronic and optical properties and the recent progress in applications of 2D semiconductor transition metal dichalcogenides with emphasis on strong excitonic effects, and spin- and valley-dependent properties are reviewed. Recent advances in the development of atomically thin layers of van der Waals bonded solids have opened up new possibilities for the exploration of 2D physics as well as for materials for applications. Among them, semiconductor transition metal dichalcogenides, MX2 (M = Mo, W; X = S, Se), have bandgaps in the near-infrared to the visible region, in contrast to the zero bandgap of graphene. In the monolayer limit, these materials have been shown to possess direct bandgaps, a property well suited for photonics and optoelectronics applications. Here, we review the electronic and optical properties and the recent progress in applications of 2D semiconductor transition metal dichalcogenides with emphasis on strong excitonic effects, and spin- and valley-dependent properties.

Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides

The isolation of graphene in 2004 from graphite was a defining moment for the “birth” of a field: two-dimensional (2D) materials In recent years, there has been a rapidly increasing number of papers focusing on non-graphene layered materials, including transition-metal dichalcogenides (TMDs), because of the new properties and applications that emerge upon 2D confinement Here, we review significant recent advances and important new developments in 2D materials “beyond graphene” We provide insight into the theoretical modeling and understanding of the van der Waals (vdW) forces that hold together the 2D layers in bulk solids, as well as their excitonic properties and growth morphologies Additionally, we highlight recent breakthroughs in TMD synthesis and characterization and discuss the newest families of 2D materials, including monoelement 2D materials (ie, silicene, phosphorene, etc) and transition metal carbide- and carbon nitride-based MXenes We then discuss the doping and functionalization of 2

Recent Advances in Two-Dimensional Materials beyond Graphene

Semiconductor technology is currently based on the manipulation of electronic charge; however, electrons have additional degrees of freedom, such as spin and valley, that can be used to encode and process information. Over the past several decades, there has been significant progress in manipulating electron spin for semiconductor spintronic devices, motivated by potential spin-based information processing and storage applications. However, experimental progress towards manipulating the valley degree of freedom for potential valleytronic devices has been limited until very recently. We review the latest advances in valleytronics, which have largely been enabled by the isolation of 2D materials (such as graphene and semiconducting transition metal dichalcogenides) that host an easily accessible electronic valley degree of freedom, allowing for dynamic control. The energy extrema of an electronic band are referred to as valleys. In 2D materials, two distinguishable valleys can be used to encode information and explore other valleytronic applications.

Valleytronics in 2D materials

Exciton binding energy and excited states in monolayers of tungsten diselenide (WSe(2)) are investigated using the combined linear absorption and two-photon photoluminescence excitation spectroscopy. The exciton binding energy is determined to be 0.37 eV, which is about an order of magnitude larger than that in III-V semiconductor quantum wells and renders the exciton excited states observable even at room temperature. The exciton excitation spectrum with both experimentally determined one- and two-photon active states is distinct from the simple two-dimensional (2D) hydrogenic model. This result reveals significantly reduced and nonlocal dielectric screening of Coulomb interactions in 2D semiconductors. The observed large exciton binding energy will also have a significant impact on next-generation photonics and optoelectronics applications based on 2D atomic crystals.

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Tightly bound excitons in monolayer WSe(2).

The superconducting properties of NbSe2 as it approaches the monolayer limit are investigated by means of magnetotransport measurements, uncovering evidence of spin–momentum locking.

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Ising pairing in superconducting NbSe2 atomic layers

The atomic thickness of two-dimensional materials provides a unique opportunity to control their electrical1 and optical2 properties as well as to drive the electronic phase transitions3 by electrostatic doping. The discovery of two-dimensional magnetic materials4–10 has opened up the prospect of the electrical control of magnetism and the realization of new functional devices11. A recent experiment based on the linear magneto-electric effect has demonstrated control of the magnetic order in bilayer CrI3 by electric fields12. However, this approach is limited to non-centrosymmetric materials11,13–16 magnetically biased near the antiferromagnet–ferromagnet transition. Here, we demonstrate control of the magnetic properties of both monolayer and bilayer CrI3 by electrostatic doping using CrI3–graphene vertical heterostructures. In monolayer CrI3, doping significantly modifies the saturation magnetization, coercive force and Curie temperature, showing strengthened/weakened magnetic order with hole/electron doping. Remarkably, in bilayer CrI3, the electron doping above ~2.5 × 1013 cm−2 induces a transition from an antiferromagnetic to a ferromagnetic ground state in the absence of a magnetic field. The result reveals a strongly doping-dependent interlayer exchange coupling, which enables robust switching of magnetization in bilayer CrI3 by small gate voltages. Electrostatic doping in vertical van der Waals CrI3–graphene heterostructures provides means to control the magnetic properties of monolayer and bilayer CrI3.

Controlling magnetism in 2D CrI 3 by electrostatic doping

Enhanced electron–phonon interactions in mono- and few-layer NbSe2 result in a significantly increased transition temperature of charge density waves compared with values in the bulk.

Strongly enhanced charge-density-wave order in monolayer NbSe2

The atomic thickness of two-dimensional (2D) materials provides a unique opportunity to control material properties and engineer new functionalities by electrostatic doping. Electrostatic doping has been demonstrated to tune the electrical and optical properties of 2D materials in a wide range, as well as to drive the electronic phase transitions. The recent discovery of atomically thin magnetic insulators has opened up the prospect of electrical control of magnetism and new devices with unprecedented performance. Here we demonstrate control of the magnetic properties of monolayer and bilayer CrI3 by electrostatic doping using a dual-gate field-effect device structure. In monolayer CrI3, doping significantly modifies the saturation magnetization, coercive force and Curie temperature, showing strengthened (weakened) magnetic order with hole (electron) doping. Remarkably, in bilayer CrI3 doping drastically changes the interlayer magnetic order, causing a transition from an antiferromagnetic ground state in the pristine form to a ferromagnetic ground state above a critical electron density. The result reveals a strongly doping-dependent interlayer exchange coupling, which enables robust switching of magnetization in bilayer CrI3 by small gate voltages.

Zefang Wang

Papers

Tightly bound excitons in monolayer WSe(2).

Ising pairing in superconducting NbSe2 atomic layers

Controlling magnetism in 2D CrI 3 by electrostatic doping

Strongly enhanced charge-density-wave order in monolayer NbSe2

Controlling magnetism in 2D CrI3 by electrostatic doping