Two-dimensional itinerant ferromagnetism in atomically thin Fe3GeTe2.

Van der Waals (vdW) crystals with covalently bonded building blocks assembled together through vdW interactions have attracted tremendous attention recently because of their interesting properties and promising applications. Compared to the explosive research on two-dimensional (2D) vdW materials, quasi-one-dimensional (quasi-1D) vdW crystals have received considerably less attention, while they also present rich physics and engineering implications. Here we report on the thermal conductivity of exfoliated quasi-1D Ta2Pd3Se8 vdW nanowires. Interestingly, even though the interatomic interactions along each molecular chain are much stronger than the interchain vdW interactions, the measured thermal conductivity still demonstrates a clear dependence on the cross-sectional size up to >110 nm. The results also reveal that partial ballistic phonon transport can persist over 13 μm at room temperature along the molecular chain direction, the longest experimentally observed ballistic transport distance with observable effects on thermal conductivity so far. First-principles calculations suggest that the ultralong ballistic phonon transport arises from the highly focused longitudinal phonons propagating along the molecular chains. These data help to understand phonon transport through quasi-1D vdW crystals, facilitating various applications of this class of materials.

van der Waals (vdW) crystals are promising candidates for integrated phase retardation applications due to their large optical birefringence. Among the two major types of vdW materials, the hyperbolic vdW crystals are inherently inadequate for optical retardation applications since the supported polaritonic modes are exclusively transverse-magnetic (TM) polarized and relatively lossy. Elliptic vdW crystals, on the other hand, represent a superior choice. For example, molybdenum disulfide (MoS2 ) is a natural uniaxial vdW crystal with extreme elliptic anisotropy in the frequency range of optical communication. Both transverse-electric (TE) polarized ordinary and TM polarized extraordinary waveguide modes can be supported in MoS2 microcrystals with suitable thicknesses. In this work, low-loss transmission of these guided modes is demonstrated with nano-optical imaging at the near-infrared (NIR) wavelength (1530 nm). More importantly, by combining theoretical calculations and NIR nanoimaging, the modal birefringence between the orthogonally polarized TE and TM modes is shown to be tunable in both sign and magnitude via varying the thickness of the MoS2 microcrystal. This tunability represents a unique new opportunity to control the polarization behavior of photons with vdW materials.

The discoveries of intrinsic ferromagnetism in atomically thin van der Waals crystals have opened a new research field enabling fundamental studies on magnetism at two-dimensional (2D) limit as well as development of magnetic van der Waals heterostructures. Currently, a variety of 2D ferromagnetism has been explored mainly by mechanically exfoliating "originally ferromagnetic (FM)" van der Waals crystals, while a bottom-up approach by thin-film growth technique has demonstrated emergent 2D ferromagnetism in a variety of "originally non-FM" van der Waals materials. Here we demonstrate that V5Se8 epitaxial thin films grown by molecular-beam epitaxy exhibit emergent 2D ferromagnetism with intrinsic spin polarization of the V 3d electrons despite that the bulk counterpart is "originally antiferromagnetic". Moreover, thickness-dependence measurements reveal that this newly developed 2D ferromagnet could be classified as an itinerant 2D Heisenberg ferromagnet with weak magnetic anisotropy, broadening a lineup of 2D magnets to those potentially beneficial for future spintronics applications.

Strongly Correlated Molecular Magnet with Curie Temperature above 60 K

Photoacoustic (PA) and modulated reflectance (MR) spectroscopy have been applied to study the indirect and direct band gap for van der Waals (vdW) crystals: dichalcogenides (MoS2, MoSe2, MoTe2, HfS2, HfSe2, WS2, WSe2, ReS2, ReSe2, SnS2 and SnSe2) and monochalcogenides (GaS, GaSe, InSe, GeS, and GeSe). It is shown that the indirect band gap can be determined by PA technique while the direct band gap can be probed by MR spectroscopy which is not sensitive to indirect optical transitions. By measuring PA and MR spectra for a given compound and comparing them with each other it is easy to conclude about the band gap character in the investigated compound and the energy difference between indirect and direct band gap. In this work such measurements, comparisons, and analyses have been performed and chemical trends in variation of indirect and direct band gap with the change in atom sizes have been discussed for proper sets of vdW crystals. It is shown that both indirect and direct band gap in vdW crystals follow the well-known chemical trends in semiconductor compounds.

Recent advancements in nanophotonic devices rely on materials with high refractive index and large optical anisotropy. Among them, van der Waals (vdW) crystals have garnered considerable interest due to their record-value optical properties originating from their complex layered structure. Moreover, the number of vdW crystals increases rapidly every year, but their traditional optical characterization is time-consuming and cannot keep up with vdW crystals’ appearance. Here, we introduce an express method for the determination of vdW optical properties to resolve this issue by taking into account their anisotropy. Our approach relies on polarized micro-transmittance, which allows us to demonstrate the superior optical response of vdW crystals on the example of hBN and GeS2. Hence, our developed technique offers a universal tool for the characterization of vdW materials’ optical properties for current and next-generation vdW-based photonic devices.

Integrating van der Waals materials on paper substrates for electrical and optical applications

The recent advent of van der Waals (vdW) crystals are considered as a new class of material for optoelectronics or photonics applications, as they have a wide range of optical band gap energies and electrical transport properties. Furthermore, due to the nature of vdW interactions, these vdW materials can be transferred onto different substrates, making them a promising candidate for integrated photonics applications. Here, we will exploit these unique properties and describe how to realize ultrathin and integrable light sources, based on photonic crystal cavities integrated van der Waals light emitters. Our demonstrated device can be operated at room temperature with fast modulation speed and enhanced emission intensity. Additionally, we will show ultrathin (~0.14 λ) van der Waals metalenses, which not only can exhibit near diffraction-limited focusing and imaging, but also can be transferred onto flexible substrates to show strain- induced tunable focusing.

In recent years, there has been an explosive increase in the research on van der Waals (vdW) crystals because of their great potential applications in many optoelectronic devices. It is necessary to determine their temperature-dependent lattice vibration characteristics because their thermal and electrical transport are closely related to the anharmonic phonon effect, which will affect the performance of the devices. We review the temperature-dependent Raman spectroscopy of vdW crystals, systematically introduce the thermal behavior of optical phonons, and summarize their shift with temperature. Upon analyzing the theoretical models and summarizing the reported experimental data, it is found that the phonon shifts of vdW crystals have a "quasi-linear" relationship with temperature, which is widely described with first-order temperature (FOT) coefficients obtained through a linear fit. Thus, subsequently, the phonon shifts of monolayer materials, different-thickness crystals, suspended and supported samples, in-plane and out-of-plane modes in the same vdW materials, as well as heterostructures and alloys are discussed through comparative analysis of FOT coefficients.

Origins of heat transport anisotropy in MoTe2 and other bulk van der Waals materials

The discoveries of ferromagnetism down to the atomically thin limit in van der Waals (vdW) crystals by mechanical exfoliation have enriched the family of magnetic thin films [C. Gong et al., Nature 546, 265-269 (2017) and B. Huang et al., Nature 546, 270-273 (2017)]. However, compared to the study of traditional magnetic thin films by physical deposition methods, the toolbox of the vdW crystals based on mechanical exfoliation and transfer suffers from low yield and ambient corrosion problem and now is facing new challenges to study magnetism. For example, the formation of magnetic superlattice is difficult in vdW crystals, which limits the study of the interlayer interaction in vdW crystals [M. Gibertini, M. Koperski, A. F. Morpurgo, K. S. Novoselov, Nat. Nanotechnol. 14, 408-419 (2019)]. Here, we report a strategy of interlayer engineering of the magnetic vdW crystal Fe3GeTe2 (FGT) by intercalating quaternary ammonium cations into the vdW spacing. Both three-dimensional (3D) vdW superlattice and two-dimensional (2D) vdW monolayer can be formed by using this method based on the amount of intercalant. On the one hand, the FGT superlattice shows a strong 3D critical behavior with a decreased coercivity and increased domain wall size, attributed to the co-engineering of the anisotropy, exchange interaction, and electron doping by intercalation. On the other hand, the 2D vdW few layers obtained by over-intercalation are capped with organic molecules from the bulk crystal, which not only enhances the ferromagnetic transition temperature (TC), but also substantially protects the thin samples from degradation, thus allowing the preparation of large-scale FGT ink in ambient environment.

Low-dimensional van der Waals (vdW) materials can harness tightly confined polaritonic waves to deliver unique advantages for nanophotonic biosensing. The reduced dimensionality of vdW materials, as in the case of two-dimensional graphene, can greatly enhance plasmonic field confinement, boosting sensitivity and efficiency compared to conventional nanophotonic devices that rely on surface plasmon resonance in metallic films. Furthermore, the reduction of dielectric screening in vdW materials enables electrostatic tunability of different polariton modes, including plasmons, excitons, and phonons. One-dimensional vdW materials, particularly single-walled carbon nanotubes, possess unique form factors with confined excitons to enable single-molecule detection as well as in vivo biosensing. We discuss basic sensing principles based on vdW materials, followed by technological challenges such as surface chemistry, integration, and toxicity. Finally, we highlight progress in harnessing vdW materials to demonstrate new sensing functionalities that are difficult to perform with conventional metal/dielectric sensors.

Van der Waals electride: Toward intrinsic two-dimensional ferromagnetism of spin-polarized anionic electrons

Electromagnetic field confinement is crucial for nanophotonic technologies, since it allows for enhancing light-matter interactions, thus enabling light manipulation in deep sub-wavelength scales. In the terahertz (THz) spectral range, radiation confinement is conventionally achieved with specially designed metallic structures-such as antennas or nanoslits-with large footprints due to the rather long wavelengths of THz radiation. In this context, phonon polaritons-light coupled to lattice vibrations-in van der Waals (vdW) crystals have emerged as a promising solution for controlling light beyond the diffraction limit, as they feature extreme field confinements and low optical losses. However, experimental demonstration of nanoscale-confined phonon polaritons at THz frequencies has so far remained elusive. Here, it is provided by employing scattering-type scanning near-field optical microscopy combined with a free-electron laser to reveal a range of low-loss polaritonic excitations at frequencies from 8 to 12 THz in the vdW semiconductor α-MoO3 . In this study, THz polaritons are visualized with: i) in-plane hyperbolic dispersion, ii) extreme nanoscale field confinement (below λo ⁄75), and iii) long polariton lifetimes, with a lower limit of >2ps.

The interlayer stacking shift in van der Waals (vdW) crystals represents an important degree of freedom to control various material properties, including magnetism, ferroelectricity, and electrical properties. On the other hand, the structural phase transitions driven by interlayer sliding in vdW crystals often exhibit thickness-dependent, sample-specific behaviors with significant hysteresis, complicating a clear understanding of their intrinsic nature. Here, the stacking configuration of the recently identified vdW crystal, γ-GeSe, is investigated, and the disordering manipulation of stacking sequence is demonstrated. It is observed that the well-ordered AB' stacking configuration in as-synthesized samples undergoes irreversible disordering upon Joule heating via electrical biasing or thermal treatment, as confirmed by atomic resolution scanning transmission electron microscopy (STEM). Statistical analysis of STEM data reveal the emergence of stacking disorder, with samples subjected to high electrical bias reaching the maximum levels of disorder. The energies of various stacking configurations and energy barriers for interlayer sliding are examined using first-principles calculation and a parameterized model to elucidate the key structural parameters related to stacking shift. The susceptibility of interlayer stacking to disorder through electrical or thermal treatments should be carefully considered to fully comprehend the structural and electrical properties of vdW crystals.