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Layered van der Waals materials have risen as powerful platforms to artificially engineer correlated states of matter. Here we show the emergence of a multiferroic order in a twisted dichalcogenide bilayer superlattice at quarter-filling. We show that the competition between Coulomb interactions leads to the simultaneous emergence of ferrimagnetic and ferroelectric orders. We derive the magnetoelectric coupling for this system, which leads to a direct strong coupling between the charge and spin orders. We show that, due to intrinsic spin-orbit coupling effects, the electronic structure shows a non-zero Chern number, thus displaying a topological multiferroic order. We show that this topological state gives rise to interface modes at the different magnetic and ferroelectric domains of the multiferroic. We demonstrate that these topological modes can be tuned with external electric fields as well as triggered by supermoire effects generated by a substrate. Our results put forward twisted van der Waals materials as a potential platform to explore multiferroic symmetry breaking orders and, ultimately, controllable topological excitations in magnetoelectric domains., Submission to SciPost, 6 figures

Layered van der Waals materials have risen as a powerful platform to engineer artificial competing states of matter. Here we show the emergence of multiferroic order in twisted chromium trihalide bilayers, an order fully driven by the moiré pattern and absent in aligned multilayers. Using a combination of spin models and ab initio calculations, we show that a spin texture is generated in the moiré supercell of the twisted system as a consequence of the competition between stacking-dependent interlayer magnetic exchange and magnetic anisotropy. An electric polarization arises associated with such a non-collinear magnetic state due to the spin-orbit coupling, leading to the emergence of a local ferroelectric order following the moiré. Among the stochiometric trihalides, our results show that twisted CrBr$_3$ bilayers give rise to the strongest multiferroic order. We further show the emergence of a strong magnetoelectric coupling, which allows the electric generation and control of magnetic skyrmions. Our results put forward twisted chromium trihalide bilayers, and in particular CrBr$_3$ bilayers, as a powerful platform to engineer artificial multiferroic materials and electrically tunable topological magnetic textures., 5+3 pages, 4 figures, supplemental material

Low dimensional magnetism has been powerfully boosted as a promising candidate for numerous applications. The stability of the long-range magnetic order is directly dependent on the electronic structure and the relative strength of the competing magnetic exchange constants. Here, we report a comparative pressure-dependent theoretical and experimental study of the electronic structure and exchange interactions of two-dimensional ferromagnets CrBr3 and Cr2Ge2Te6 . While CrBr3 is found to be a Mott-Hubbard-like insulator, Cr2Ge2Te6 shows a charge-transfer character due to the broader character of the Te 5p bands at the Fermi level. This different electronic behaviour is responsible of the robust insulating state of CrBr3 , in which the magnetic exchange constants evolve monotonically with pressure, and the proximity to a metal-insulator transition predicted for Cr2Ge2Te6 , which causes a non-monotonic evolution of its magnetic ordering temperature. We provide a microscopic understanding for the pressure evolution of the magnetic properties of the two systems.

In this study we present a detailed ab initio analysis of the magnetic properties of VSe2 . Ab initio calculations in the so-called 1T structure yield a ferromagnetic phase as most stable, with a magnetic moment of about 0.6 {\mu} B /V. According to our calculations this ferromagnetic state is on the verge of instability. We have modeled ab initio the charge density wave state reported in the literature. This introduces a periodic lattice distortion leading to a supercell with periodicity 4a x 4a x 3c (4a x 4a for the monolayer) in which we have fully relaxed the atomic positions. We demonstrate that this structural rearrangement causes a strong reduction in the density of states at the Fermi level and the ground state of the system becomes non-magnetic for the bulk. In the monolayer limit the rearrangement induces a Peierls distortion causing an energy gap opening at the Fermi level and the quenching of ferromagnetism.

This paper shows that the oxygen vacancies observed experimentally in thin films of LaCoO3 subject to tensile strain are thermodynamically stable according to ab initio calculations. By using DFT calculations, we show that oxygen vacancies on the order of 6 % forming chains perpendicular to the (001) direction are more stable than the stoichiometric solution. These lead to magnetic Co2+ ions surrounding the vacancies that couple ferromagnetically. The remaining Co3+ cations in an octahedral environment are non magnetic. The gap leading to a ferromagnetic insulating phase occurs naturally and we provide a simple ionic picture to explain the resulting electronic structure., Comment: 7 pages, 7 figures