Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals.

Strongly Correlated Molecular Magnet with Curie Temperature above 60 K

Superconductivity has become a fascinating research field in condensed matter physics since its discovery in 1911. Nowadays, two-dimensional materials exhibit a variety of new physical phenomena, such as Ising superconductivity, topological superconductivity, and unconventional superconductivity. A number of two-dimensional van der Waals crystals exhibit superconductivity, which provide us with a broad research platform for exploring various physical effects and novel phenomena. In this review, we focus our attention on superconducting properties of two-dimensional van der Waals crystals, and highlight the recent progress of the state-of-the-art research on synthesis, characterization, and isolation of single and few layer nanosheets and the assembly of two-dimensional van der Waals superconductors. Finally we conclude the future research directions and prospects in two-dimensional materials with superconductivity.

The exfoliation and stacking of two-dimensional van der Waals crystals have created unprecedented opportunities in the discovery of quantum phases. A major obstacle to the advancement of this field is the limited spectroscopic access due to a mismatch in the sample sizes (10-6-10-5 m) and the wavelengths (10-4-10-3 m) of electromagnetic radiation relevant to their low-energy excitations. Here we introduce ferroelectric semiconductor NbOI2 as a two-dimensional van der Waals material capable of operating as a van der Waals terahertz emitter. We demonstrate intense and broadband terahertz generation from NbOI2 with an optical rectification efficiency that is more than one order of magnitude higher than that of ZnTe, the current standard terahertz emitter. Moreover, this NbOI2 terahertz emitter can be integrated into van der Waals heterostructures to enable on-chip near-field terahertz spectroscopy of a target van der Waals material and device. Our approach provides a general spectroscopic tool for two-dimensional van der Waals materials and quantum matter.

Materials research has driven the development of modern nano-electronic devices. In particular, research in magnetic thin films has revolutionized the development of spintronic devices1,2 because identifying new magnetic materials is key to better device performance and design. Van der Waals crystals retain their chemical stability and structural integrity down to the monolayer and, being atomically thin, are readily tuned by various kinds of gate modulation3,4. Recent experiments have demonstrated that it is possible to obtain two-dimensional ferromagnetic order in insulating Cr2Ge2Te6 (ref. 5) and CrI3 (ref. 6) at low temperatures. Here we develop a device fabrication technique and isolate monolayers from the layered metallic magnet Fe3GeTe2 to study magnetotransport. We find that the itinerant ferromagnetism persists in Fe3GeTe2 down to the monolayer with an out-of-plane magnetocrystalline anisotropy. The ferromagnetic transition temperature, Tc, is suppressed relative to the bulk Tc of 205 kelvin in pristine Fe3GeTe2 thin flakes. An ionic gate, however, raises Tc to room temperature, much higher than the bulk Tc. The gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2 opens up opportunities for potential voltage-controlled magnetoelectronics7-11 based on atomically thin van der Waals crystals.

Two-dimensional van der Waals (vdW) crystals can sustain various types of polaritons with strong electromagnetic confinements, making them highly attractive for nanoscale photonic and optoelectronic applications. While extensive experimental and numerical studies have been devoted to the polaritons of the vdW crystals, analytical models are sparse. Particularly, applying the model to describe polariton behaviors that are visualized by state of the art near-field optical microscopy requires further investigations. In this study, we develop an analytical waveguide model to describe polariton propagations in vdW crystals. The dispersion contours, dispersion relations, and localized electromagnetic field distributions of polariton waveguide modes are derived. The model is verified by real-space optical nano-imaging and numerical simulation of phonon polaritons in α-MoO3, which is a vdW biaxial crystal. Although we focus on α-MoO3, the proposed model is valid for other polaritonic crystals within the vdW family given the corresponding dielectric substitutions. Our model therefore provides an analytical rationale for describing and understanding the localized electromagnetic fields in vdW crystals that are associated with polaritons.

This study investigates the electronic band structure of chromium sulfur bromide (CrSBr) through comprehensive photoluminescence (PL) characterization. We clearly identify low-temperature optical transitions between two closely adjacent conduction-band states and two different valence-band states. The analysis on the PL data robustly unveils energy splittings, band gaps, and excitonic transitions across different thicknesses of CrSBr, from monolayer to bulk. Temperature-dependent PL measurements elucidate the stability of the band splitting below the Néel temperature, suggesting that magnons coupled with excitons are responsible for the symmetry breaking and brightening of the transitions from the secondary conduction band minimum (CBM2) to the global valence band maximum (VBM1). Collectively, these results not only reveal splitting in both the conduction and valence bands but also highlight a significant advance in our understanding of the interplay between the optical, electronic, and magnetic properties of antiferromagnetic two-dimensional van der Waals crystals.

Two-dimensional (2D) van der Waals (vdW) heterostructures have attracted much attention due to their unique properties in photocatalysis, electronics, and energy storage. This work comprehensively analyzed the electronic properties and photocatalytic efficiency properties of 2D vdW MoS2/Hf2CO2 heterostructure by first-principles calculations and molecular dynamics simulation. An ideal band gap of 1.44 eV was found for visible light absorption. Meanwhile, a high solar-to-hydrogen efficiency of 17.14% is obtained from the calculated band-edge positions, and a high power conversion efficiency of 13.84% is also confirmed by spectroscopy limited maximum efficiency simulation. We estimate the time scale for electron–hole transfer and recombination times using a combination of non-adiabatic molecular dynamics and time-dependent density functional theory. A suitable e-h recombination time of 1.86 ns and electron (hole) transfer time of 331 (978) fs are obtained in the 2D MoS2/Hf2CO2 heterostructure, which is expected to ensure high photocatalytic efficiency. Therefore, the constructed MoS2/Hf2CO2 heterostructures provide a new example for the prediction of high-performance nano optoelectronic devices.

Phonon polaritons (PhPs) in two-dimensional van der Waals crystals, such as hexagonal boron nitride (hBN) and α-phase molybdenum trioxide (α-MoO3), exhibit remarkable spatial confinement and extremely low optical losses, offering possibilities for the development of novel micro and nanophotonic devices at mid-infrared wavelengths. Here, we demonstrate the potential of the proposed Tamm structure to achieve dual-band high quality-factor perfect absorption within the mid-infrared range. This structure utilizes upper and lower spacer layers to isolate the anisotropic materials hBN and α-MoO3 from one-dimensional photonic crystals, where the Tamm phonon polaritons (TPhPs) are respectively excited at the interfaces, facilitating strong coupling with incident light and leading to significant dual-band perfect absorption phenomena. The results demonstrate that due to polariton resonances, the absorption peaks exhibit extremely narrow absorption bandwidths, with the maximum quality-factor reaching up to 297. In addition, tunable resonant wavelengths and polarization-dependent absorption properties are also demonstrated in the proposed Tamm structure. This study provides an alternative and straightforward approach for constructing dynamic and multifunctional optical devices such as optical modulators, tunable multi-band filters and biosensors.

The recent discovery of ferromagnetism in two-dimensional van der Waals crystals has provoked a surge of interest in the exploration of fundamental spin interaction in reduced dimensions. However, existing material candidates have several limitations, notably lacking intrinsic room-temperature ferromagnetic order and air stability. Here, motivated by the anomalously high Curie temperature observed in bulk diluted magnetic oxides, we demonstrate room-temperature ferromagnetism in Co-doped graphene-like Zinc Oxide, a chemically stable layered material in air, down to single atom thickness. Through the magneto-optic Kerr effect, superconducting quantum interference device and X-ray magnetic circular dichroism measurements, we observe clear evidences of spontaneous magnetization in such exotic material systems at room temperature and above. Transmission electron microscopy and atomic force microscopy results explicitly exclude the existence of metallic Co or cobalt oxides clusters. X-ray characterizations reveal that the substitutional Co atoms form Co2+ states in the graphitic lattice of ZnO. By varying the Co doping level, we observe transitions between paramagnetic, ferromagnetic and less ordered phases due to the interplay between impurity-band-exchange and super-exchange interactions. Our discovery opens another path to 2D ferromagnetism at room temperature with the advantage of exceptional tunability and robustness.

In spintronics, two-dimensional van der Waals crystals constitute a most promising material class for long-distance spin transport or effective spin manipulation at room temperature. To realize all-vdW-material-based spintronic devices, however, vdW materials with itinerant ferromagnetism at room temperature are needed for spin current generation and thereby serve as an effective spin source. We report theoretical design and experimental realization of a iron-based vdW material, Fe4GeTe2, showing a nearly room temperature ferromagnetic order, together with a large magnetization and high conductivity. These properties are well retained even in cleaved crystals down to seven layers, with notable improvement in perpendicular magnetic anisotropy. Our findings highlight Fe4GeTe2 and its nanometer-thick crystals as a promising candidate for spin source operation at nearly room temperature and hold promise to further increase T c in vdW ferromagnets by theory-guided material discovery.

The past decade has witnessed an explosion in the field of quantum materials, headlined by the predictions and discoveries of novel Landau-symmetry-broken phases in correlated electron systems, topological phases in systems with strong spin-orbit coupling, and ultra-manipulable materials platforms based on two-dimensional van der Waals crystals. Discovering pathways to experimentally realize quantum phases of matter and exert control over their properties is a central goal of modern condensed-matter physics, which holds promise for a new generation of electronic/photonic devices with currently inaccessible and likely unimaginable functionalities. In this Review, we describe emerging strategies for selectively perturbing microscopic interaction parameters, which can be used to transform materials into a desired quantum state. Particular emphasis will be placed on recent successes to tailor electronic interaction parameters through the application of intense fields, impulsive electromagnetic stimulation, and nanostructuring or interface engineering. Together these approaches outline a potential roadmap to an era of quantum phenomena on demand.

Flexible long period moiré superlattices form in two-dimensional van der Waals crystals containing layers that differ slightly in lattice constant or orientation. In this Letter we show theoretically that isolated flat moiré bands described by generalized triangular lattice Hubbard models are present in twisted transition metal dichalcogenide heterobilayers. The hopping and interaction strength parameters of the Hubbard model can be tuned by varying the twist angle and the three-dimensional dielectric environment. When the flat moiré bands are partially filled, candidate many-body ground states at some special filling factors include spin-liquid states, quantum anomalous Hall insulators, and chiral d-wave superconductors.

Semimetallic features in thermoelectric transport properties of 2H–3R phase niobium diselenide

Ambient humidity introduces water adsorption and intercalation at the surfaces and interfaces of low-dimensional materials. Our extensive molecular dynamics (MD) simulations reveal the completely opposite contributions of interfacial water to the peeling of monolayer graphene and hexagonal boron nitride (h-BN) sheets from graphite and BN substrates. For graphene, interfacial water decreases the peeling force, due to lower adhesion at the graphene/water interface. The peeling force of h-BN increases with an increase in the thickness of interfacial water, owing to stronger adhesion at the h-BN/water interface and the detachment of the water layer from the substrates. In this work, a theoretical model considering graphene/water and water/substrate interfacial adhesion energies is established, to predict the peeling forces of graphene and h-BN, which coincides well with the peeling forces predicted by the MD simulations. Our results should provide a deeper insight into the effect of interfacial water, induced by ambient humidity, on mechanical exfoliation and the transfer of two-dimensional van der Waals crystals.

Two-dimensional van der Waals crystals (2D vdW) are recognized as one of the potential materials to solve the physical limits caused by size scaling. Here, vdW metal oxide MoO3 is applied with the gate dielectric in a 2D field-effect transistor (FET). Due to its high dielectric constant and the good response of MoS2 to visible light, we obtained a field effect transistor for photodetection. In general, the device exhibits a threshold voltage near 0 V, Ion/Ioff ratio of 105, electron mobility about 85 cm2 V−1 s−1 and a good response to visible light, the responsivity is near 5 A/W at low laser power, which shows that MoO3 is a potential material as gate dielectric.