2D SnTe films with a thickness of as little as 2 atomic layers (ALs) have recently been shown to be ferroelectric with in‐plane polarization. Remarkably, they exhibit transition temperatures (Tc ) much higher than that of bulk SnTe. Here, combining molecular beam epitaxy, variable temperature scanning tunneling microscopy, and ab initio calculations, the underlying mechanism of the Tc enhancement is unveiled, which relies on the formation of γ‐SnTe, a van der Waals orthorhombic phase with antipolar inter‐layer coupling in few‐AL thick SnTe films. In this phase, 4n − 2 AL (n = 1, 2, 3…) thick films are found to possess finite in‐plane polarization (space group Pmn21), while 4n AL thick films have zero total polarization (space group Pnma). Above 8 AL, the γ‐SnTe phase becomes metastable, and can convert irreversibly to the bulk rock salt phase as the temperature is increased. This finding unambiguously bridges experiments on ultrathin SnTe films with predictions of robust ferroelectricity in GeS‐type monochalcogenide monolayers. The observed high transition temperature, together with the strong spin‐orbit coupling and van der Waals structure, underlines the potential of atomically thin γ‐SnTe films for the development of novel spontaneous polarization‐based devices.

There is considerable interest in van der Waals (vdW) materials as potential hosts for chiral skyrmionic spin textures. Of particular interest is the ferromagnetic, metallic compound Fe3GeTe2 (FGT), which has a comparatively high Curie temperature (150–220 K). Several recent studies have reported the observation of chiral Néel skyrmions in this compound, which is inconsistent with its presumed centrosymmetric structure. Here the observation of Néel type skyrmions in single crystals of FGT via Lorentz transmission electron microscopy (LTEM) is reported. It is shown from detailed X‐ray diffraction structure analysis that FGT lacks an inversion symmetry as a result of an asymmetric distribution of Fe vacancies. This vacancy‐induced breaking of the inversion symmetry of this compound is a surprising and novel observation and is a prerequisite for a Dzyaloshinskii–Moriya vector exchange interaction which accounts for the chiral Néel skyrmion phase. This phenomenon is likely to be common to many 2D vdW materials and suggests a path to the preparation of many such acentric compounds. Furthermore, it is found that the skyrmion size in FGT is strongly dependent on its thickness: the skyrmion size increases from ≈100 to ≈750 nm as the thickness of the lamella is increased from ≈90 nm to ≈2 µm. This extreme size tunability is a feature common to many low symmetry ferro‐ and ferri‐magnetic compounds.

Weyl Semimetals (WSMs), a recently discovered topological state of matter, exhibit an electronic structure governed by linear band dispersions and degeneracy (Weyl) points leading to rich physical phenomena, which are yet to be exploited in thin film devices. While WSMs were established in the monopnictide compound family several years ago, the growth of thin films has remained a challenge. Here, we report the growth of epitaxial thin films of NbP and TaP by means of molecular beam epitaxy. Single crystalline films are grown on MgO (001) substrates using thin Nb (Ta) buffer layers, and are found to be tensile strained (1%) and with slightly P-rich stoichiometry with respect to the bulk crystals. The resulting electronic structure exhibits topological surface states characteristic of a P-terminated surface, linear dispersion bands in agreement with the calculated band structure, and a Fermi-level shift of -0.2 eV with respect to the Weyl points. Consequently, the electronic transport is dominated by both holes and electrons with carrier mobilities close to 10 3 cm 2 /Vs at room-temperature. The growth of epitaxial thin films opens up the use of strain and controlled doping to access and tune the electronic structure of Weyl Semimetals on demand, paving the way for the rational design and fabrication of electronic devices ruled by topology.

Transition‐metal phosphides (TMP) prepared by atomic layer deposition (ALD) are reported for the first time. Ultrathin Co‐P films were deposited by using PH3 plasma as the phosphorus source and an extra H2 plasma step to remove excess P in the growing films. The optimized ALD process proceeded by self‐limited layer‐by‐layer growth, and the deposited Co‐P films were highly pure and smooth. The Co‐P films deposited via ALD exhibited better electrochemical and photoelectrochemical hydrogen evolution reaction (HER) activities than similar Co‐P films prepared by the traditional post‐phosphorization method. Moreover, the deposition of ultrathin Co‐P films on periodic trenches was demonstrated, which highlights the broad and promising potential application of this ALD process for a conformal coating of TMP films on complex three‐dimensional (3D) architectures.

Cr(1+δ)Te2 are pseudo-layered compounds consisting of CrTe2 transition metal dichalcogenide (TMD) layers with additional (δ) self-intercalated Cr atoms. The recent search for ferromagnetic 2D materials revived the interest into chromium tellurides. Here, Cr(1+δ)Te2 nanolayers are epitaxially grown on MoS2 (0001), forming prototypical van der Waals heterostructures. Under optimized growth conditions, ultrathin films of only two TMD layers with a single intercalated Cr-layer are achieved, forming a 2D sheet with van der Waals surfaces. Detailed compositional and structural characterization by scanning tunneling microscopy, grazing incidence x-ray diffraction, and high-resolution Rutherford backscattering indicate the layer-by-layer growth and that the δ can be tuned by post-growth annealing in a range between ∼0.5 and 1. X-ray magnetic circular dichroism and magnetometry measurements demonstrate that all self-intercalated Cr(1+δ)Te2 nanolayers exhibit strong ferromagnetism with magnetic moments larger than 3μB per Cr-atom. The magnetic properties are maintained in the ultrathin limit of a material with a single intercalation layer. Interestingly, the magnetic anisotropy can be tuned from close to isotropic (δ = 1) to a desirable perpendicular anisotropy for low δ values. Thus, the bottom-up growth of these 2D Cr(1+δ)Te2 sheets is a promising approach for designing magnetic van der Waals heterostructures.