While the discovery of two-dimensional (2D) magnets opens the door for fundamental physics and next-generation spintronics, it is technically challenging to achieve the room-temperature ferromagnetic (FM) order in a way compatible with potential device applications. Here, we report the growth and properties of single- and few-layer CrTe2, a van der Waals (vdW) material, on bilayer graphene by molecular beam epitaxy (MBE). Intrinsic ferromagnetism with a Curie temperature (TC) up to 300 K, an atomic magnetic moment of ~0.21 $${\mu }_{{\rm{B}}}$$ μ B /Cr and perpendicular magnetic anisotropy (PMA) constant (Ku) of 4.89 × 105 erg/cm3 at room temperature in these few-monolayer films have been unambiguously evidenced by superconducting quantum interference device and X-ray magnetic circular dichroism. This intrinsic ferromagnetism has also been identified by the splitting of majority and minority band dispersions with ~0.2 eV at Г point using angle-resolved photoemission spectroscopy. The FM order is preserved with the film thickness down to a monolayer (TC ~ 200 K), benefiting from the strong PMA and weak interlayer coupling. The successful MBE growth of 2D FM CrTe2 films with room-temperature ferromagnetism opens a new avenue for developing large-scale 2D magnet-based spintronics devices.

Conjugated polymers such as polyethylenedioxythiophene (pEDOT), polypyrrole (pPy), and polyaniline (pAni) exhibit high electrochemical capacities, making them appealing as electrode materials for energy storage, electrochemical desalination, and chemical sensing. Recent work has established the growth of thin films of pEDOT using alternating gas-phase exposures of the EDOT monomer and a metal chloride (e.g., MoCl 5 ) oxidant in a process termed oxidative molecular layer deposition (oMLD). Here, we describe the first demonstration of oMLD of amine-containing conjugated polymers. We find that pyrrole (Py) and MoCl 5 undergo self-limiting surface reactions during oMLD exposures to form conformal pPy thin films, but oMLD using aniline (Ani) and p-phenylenediamine (PDA) monomers yields unexpected azo functionality. The formation of azo groups is attributed to an MoCl 5 -amine surface adduct that spatially constrains polymerization reactions near the amine group and produces azo groups when coupling two primary amines. pPy grown by oMLD exhibits a record-breaking 282 mAh/g capacity in an aqueous electrolyte, and PDA/MoCl 5 oMLD yields azo polymers of interest as anode materials for alkali-ion batteries. Alternating between Py and PDA monomers during oMLD produces molecularly assembled copolymers with qualitatively different electrochemical responses from the isolated monomer structures. This work lays the foundation for the growth of conformal thin films of conjugated amine polymers with molecular-level control of composition and thickness.

No abstract

One of the most promising avenues in 2D materials research is the synthesis of antiferromagnets employing 2D van der Waals (vdW) magnets. However, it has proven challenging, due in part to the complicated fabrication process and undesired adsorbates as well as the significantly deteriorated ferromagnetism at atomic layers. Here, the engineering of the antiferromagnetic (AFM) interlayer exchange coupling between atomically thin yet ferromagnetic CrTe 2 layers in an ultra-high vacuum-free 2D magnetic crystal, Cr 5 Te 8 is reported. By self-introducing interstitial Cr atoms in the vdW gaps, the emergent AFM ordering and the resultant giant magnetoresistance effect are induced. A large negative magnetoresistance (10%) with a plateau-like feature is revealed, which is consistent with the AFM interlayer coupling between the adjacent CrTe 2 main layers in a temperature window of 30 K below the Néel temperature. Notably, the AFM state has a relatively weak interlayer exchange coupling, allowing a switching between the interlayer AFM and ferromagnetic states at moderate magnetic fields. This work represents a new route to engineering low-power devices that underpin the emerging spintronic technologies, and an ideal laboratory to study 2D magnetism.

Tuning interactions between Dirac states in graphene has attracted enormous interest because it can modify the electronic spectrum of the 2D material, enhance electron correlations, and give rise to novel condensed‐matter phases such as superconductors, Mott insulators, Wigner crystals, and quantum anomalous Hall insulators. Previous works predominantly focus on the flat band dispersion of coupled Dirac states from different twisted graphene layers. In this work, a new route to realizing flat band physics in monolayer graphene under a periodic modulation from substrates is proposed. Graphene/SiC heterostructure is taken as a prototypical example and it is demonstrated experimentally that the substrate modulation leads to Dirac fermion cloning and, consequently, the proximity of the two Dirac cones of monolayer graphene in momentum space. Theoretical modeling captures the cloning mechanism of the Dirac states and indicates that moiré flat bands can emerge at certain magic lattice constants of the substrate, specifically when the period of modulation becomes nearly commensurate with the false(3 × 3false)R30o\[(\sqrt 3 \; \times \;\sqrt 3 )R{30^o}\] supercell of graphene. The results show that epitaxial single monolayer graphene on suitable substrates is a promising platform for exploring exotic many‐body quantum phases arising from interactions between Dirac electrons.