Efrén Navarro-Moratalla

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

Since the discovery of graphene, the family of two-dimensional materials has grown, displaying a broad range of electronic properties. Recent additions include semiconductors with spin–valley coupling, Ising superconductors that can be tuned into a quantum metal, possible Mott insulators with tunable charge-density waves, and topological semimetals with edge transport. However, no two-dimensional crystal with intrinsic magnetism has yet been discovered; such a crystal would be useful in many technologies from sensing to data storage. Theoretically, magnetic order is prohibited in the two-dimensional isotropic Heisenberg model at finite temperatures by the Mermin–Wagner theorem. 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 crystals. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect, 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 magnetoelectronics, and van der Waals engineering to produce interface phenomena.

Enhanced superconductivity in atomically thin TaS2.

The ability to exfoliate layered materials down to the single layer limit has presented the opportunity to understand how a gradual reduction in dimensionality affects the properties of bulk materials. Here we use this top–down approach to address the problem of superconductivity in the two-dimensional limit. The transport properties of electronic devices based on 2H tantalum disulfide flakes of different thicknesses are presented. We observe that superconductivity persists down to the thinnest layer investigated (3.5 nm), and interestingly, we find a pronounced enhancement in the critical temperature from 0.5 to 2.2 K as the layers are thinned down. In addition, we propose a tight-binding model, which allows us to attribute this phenomenon to an enhancement of the effective electron–phonon coupling constant. This work provides evidence that reducing the dimensionality can strengthen superconductivity as opposed to the weakening effect that has been reported in other 2D materials so far.

Hybrid Magnetic/Superconducting Materials Obtained by Insertion of a Single‐Molecule Magnet into TaS2 Layers

N Among the hot topics in materials chemistry, the design of novel materials in which two or more physical properties of interest can be rationally combined into the same solid is currently attracting important attention. With this regard, the versatility of the molecular building-block approach, which relies on the combination of different molecular entities carrying specifi c functionalities into an extended molecule-based solid, has proven to be a very fruitful synthetic route. [ 1–5 ]

A MoTe 2 -based light-emitting diode and photodetector for silicon photonic integrated circuits

One of the current challenges in photonics is developing high-speed, power-efficient, chip-integrated optical communications devices to address the interconnects bottleneck in high-speed computing systems. Silicon photonics has emerged as a leading architecture, in part because of the promise that many components, such as waveguides, couplers, interferometers and modulators, could be directly integrated on silicon-based processors. However, light sources and photodetectors present ongoing challenges. Common approaches for light sources include one or few off-chip or wafer-bonded lasers based on III-V materials, but recent system architecture studies show advantages for the use of many directly modulated light sources positioned at the transmitter location. The most advanced photodetectors in the silicon photonic process are based on germanium, but this requires additional germanium growth, which increases the system cost. The emerging two-dimensional transition-metal dichalcogenides (TMDs) offer a path for optical interconnect components that can be integrated with silicon photonics and complementary metal-oxide-semiconductors (CMOS) processing by back-end-of-the-line steps. Here, we demonstrate a silicon waveguide-integrated light source and photodetector based on a p-n junction of bilayer MoTe2, a TMD semiconductor with an infrared bandgap. This state-of-the-art fabrication technology provides new opportunities for integrated optoelectronic systems.

Fast and reliable identification of atomically thin layers of TaSe2 crystals

Deposition of clean and defect-free atomically thin two-dimensional crystalline flakes on surfaces by mechanical exfoliation of layered bulk materials has proven to be a powerful technique, but it requires a fast, reliable and non-destructive way to identify the atomically thin flakes among a crowd of thick flakes. In this work, we provide general guidelines to identify ultrathin flakes of TaSe2 by means of optical microscopy and Raman spectroscopy. Additionally, we determine the optimal substrates to facilitate the optical identification of atomically thin TaSe2 crystals. Experimental realization and isolation of ultrathin layers of TaSe2 enables future studies on the role of the dimensionality in interesting phenomena such as superconductivity and charge density waves.Graphical abstract

Confined growth of cyanide-based magnets in two dimensions.

Herein we report the first hybrid magnetic material resulting from the intercalation of a cyanide-based molecular magnet into a solid-state layered host. More specifically, the use of a diamagnetic cationic Zn(II)-Al(lII) layered double hydroxide host allows for the formation of an anionic two-dimensional ferromagnetic Ni(II)-Cr(III) Prussian Blue analogue, from the templated assembly of its ionic molecular components in the confined interlamellar space offered by the inorganic host.

Intercalation of two-dimensional oxalate-bridged molecule-based magnets into layered double hydroxide hosts

Here we report the intercalation of a MnII–CrIII oxalate-bridged extended network into the interlamellar space offered by a ZnII–AlIII LDH host. This material exhibits ferrimagnetic ordering below 3 K from dominant antiferromagnetic interactions between metallic centres through the oxalate linker. Our result opens the door for the design of a completely new sort of hybrid magnetic multilayers from molecule-based magnets and layered inorganic flexible hosts, where the intrinsic properties of both sub-layers can be combined.

Strong enhancement of superconductivity at high pressures within the charge-density-wave states of 2H-TaS 2 and 2H-TaSe 2

We present measurements of the superconducting and charge density wave critical temperatures (Tc and TCDW) as a function of pressure in the transition metal dichalchogenides 2H-TaSe2 and 2H-TaS2. Resistance and susceptibility measurements show that Tc increases from temperatures below 1 K up to 8.5 K at 9.5 GPa in 2H-TaS2 and 8.2 K at 23 GPa in 2H-TaSe2. We observe a kink in the pressure dependence of TCDW at about 4 GPa that we attribute to the lock-in transition from incommensurate CDW to commensurate CDW. Above this pressure, the commensurate TCDW slowly decreases coexisting with superconductivity within our full pressure range.

Electrical control of 2D magnetism in bilayer CrI 3

Controlling magnetism via electric fields addresses fundamental questions of magnetic phenomena and phase transitions1–3, and enables the development of electrically coupled spintronic devices, such as voltage-controlled magnetic memories with low operation energy4–6. Previous studies on dilute magnetic semiconductors such as (Ga,Mn)As and (In,Mn)Sb have demonstrated large modulations of the Curie temperatures and coercive fields by altering the magnetic anisotropy and exchange interaction2,4,7–9. Owing to their unique magnetic properties10–14, the recently reported two-dimensional magnets provide a new system for studying these features15–19. For instance, a bilayer of chromium triiodide (CrI3) behaves as a layered antiferromagnet with a magnetic field-driven metamagnetic transition15,16. Here, we demonstrate electrostatic gate control of magnetism in CrI3 bilayers, probed by magneto-optical Kerr effect (MOKE) microscopy. At fixed magnetic fields near the metamagnetic transition, we realize voltage-controlled switching between antiferromagnetic and ferromagnetic states. At zero magnetic field, we demonstrate a time-reversal pair of layered antiferromagnetic states that exhibit spin-layer locking, leading to a linear dependence of their MOKE signals on gate voltage with opposite slopes. Our results allow for the exploration of new magnetoelectric phenomena and van der Waals spintronics based on 2D materials.Electrical control of magnetism in a bilayer of CrI3 enables the realization of an electrically driven magnetic phase transition and the observation of the magneto-optical Kerr effect in 2D magnets.

Ligand-field helical luminescence in a 2D ferromagnetic insulator

Bulk chromium tri-iodide (CrI3) has long been known as a layered van der Waals ferromagnet1. However, its monolayer form was only recently isolated and confirmed to be a truly two-dimensional (2D) ferromagnet2, providing a new platform for investigating light–matter interactions and magneto-optical phenomena in the atomically thin limit. Here, we report spontaneous circularly polarized photoluminescence in monolayer CrI3 under linearly polarized excitation, with helicity determined by the monolayer magnetization direction. In contrast, the bilayer CrI3 photoluminescence exhibits vanishing circular polarization, supporting the recently uncovered anomalous antiferromagnetic interlayer coupling in CrI3 bilayers2. Distinct from the Wannier–Mott excitons that dominate the optical response in well-known 2D van der Waals semiconductors3, our absorption and layer-dependent photoluminescence measurements reveal the importance of ligand-field and charge-transfer transitions to the optoelectronic response of atomically thin CrI3. We attribute the photoluminescence to a parity-forbidden d–d transition characteristic of Cr3+ complexes, which displays broad linewidth due to strong vibronic coupling and thickness-independent peak energy due to its localized molecular orbital nature.Atomically thin chromium tri-iodide is shown to be a 2D ferromagnetic insulator with an optical response dominated by ligand-field transitions, emitting circularly polarized photoluminescence with a helicity determined by the magnetization direction.