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Topological crystalline insulators (TCIs) host topological phases of matter protected by crystal symmetries. Topological surface states in three-dimensional TCIs have been predicted and observed in IV-VI SnTe-class semiconductors. Despite the prediction of a two-dimensional (2D) TCI characterized by two pairs of edge states inside the bulk gap, materials challenges have thus far prevented its experimental realization. Here we report the growth and characterization of bilayer SnTe on the 2$H$-NbSe$_2$ substrate by molecular beam epitaxy and scanning tunneling microscopy. We experimentally observe two anticorrelated, periodically modulated pairs of conducting edge states along the perimeters of the sample with a large band gap exceeding $0.2$ eV. We identify these states with a 2D TCI through first principles calculations. Finally, we probe the coupling of adjacent topological edge states and demonstrate the resulting energy shift driven by a combination of electrostatic interactions and tunneling coupling. Our work opens the door to investigations of tunable topological states in 2D TCIs, of potential impact for spintronics and nanoelectronics applications at room temperature.

Super-moire materials represent a novel playground to engineer states of matter beyond the possibilities of conventional moire materials. However, from the computational point of view, understanding correlated matter in these systems requires solving models with several millions of atoms, a formidable task for state-of-the-art methods. Conventional wavefunction methods for correlated matter scale with a cubic power with the number of sites, a major challenge for super-moire materials. Here, we introduce a methodology capable of solving correlated states in super-moire materials by combining a kernel polynomial method with a quantics tensor cross matrix product state algorithm. This strategy leverages a mapping of the super-moire structure to a many-body Hilbert space efficiently sampled with a tensor cross matrix product state method, where individual evaluations are performed with a Chebyshev kernel polynomial algorithm. We demonstrate this approach with interacting super-moire systems with up to several millions of atoms, showing its ability to capture correlated states in moire-of-moire systems and domain walls between different moire systems. Our manuscript puts forward a widely applicable methodology to study correlated matter in ultra-long length scales, enabling rationalizing correlated super-moire phenomena., Comment: 11 pages, 5 figures

Van der Waals monolayers featuring magnetic states provide a fundamental building block for artificial quantum matter. Here, we establish the emergence of a multicomponent ground state featuring magneto-orbital excitations of the 3d2-transition metal trihalide VCl3 monolayer. We show that monolayer VCl3 realizes a ground state with simultaneous magnetic and orbital ordering using density functional theory. Using first-principles methods we derive an effective Hamiltonian with intertwined spin and orbital degree of freedom, which we demonstrate can be tuned by strain. We show that magneto-orbitons appear as the collective modes of this complex order, and arise from coupled orbiton magnon excitations due to the magneto-orbital coupling in the system. Our results establish VCl3 as a promising 2D material to observe emergent magneto-orbital excitations and provide a platform for multicomponent symmetry breaking., Comment: 7 pages, 3 figures

Twisted magnetic van der Waals materials provide a flexible platform to engineer new forms of unconventional magnetism. Here we demonstrate the emergence of electrically tunable topological moir\'e magnetism in twisted bilayers of the spin-spiral multiferroic NiI$_2$. We establish a rich phase diagram featuring uniform spiral phases, a variety of $k\pi$-skyrmion lattices, and nematic spin textures ordered at the moir\'e scale. The emergence of these phases is driven by the local stacking and the resulting modulated frustration in the spin spiral stemming from the moir\'e pattern. Notably, when the spin-spiral wavelength is commensurate with the moir\'e length scale by an integer $k$, multi-walled skyrmions become pinned to the moir\'e pattern. We show that the strong magnetoelectric coupling displayed by the moir\'e multiferroic allows the electric control of the $k\pi$-skyrmion lattices by an out-of-plane electric field, which couples to the moir\'e-induced electric polarization. While adiabatic changes in the electric field preserve the topology of the spin configurations, abrupt variations can trigger transitions between different skyrmion lattice ground states. Our results establish a highly tunable platform for skyrmionics based on twisted van der Waals multiferroics, potentially enabling a new generation of ultrathin topologically-protected spintronic devices., Comment: 8 pages, 4 figures

Layered van der Waals two-dimensional (2D) magnets are a cornerstone of ultrathin spintronic and magnonic devices. The recent discovery of a 2D multiferroic with strong magnetoelectric coupling in NiI$_2$ offers a promising platform for the electrical control of spin-wave transport. In this work, using ab initio calculations, we investigate how the magnonic properties of monolayer NiI$_2$ can be controlled using an external electric field. We show that the emergence of a ferroelectric polarization leads to an energy splitting in the magnon spectrum, thus establishing a way to detect the electric polarization experimentally. We also show the modulation of the magnon splitting and the energy position of the singularities in magnon DOS by an electric field due to the strong magnetoelectric coupling. Our results highlight the interplay between ferroelectricity and magnons in van der Waals multiferroics and pave the way to design electrically tunable magnetic devices at the 2D limit.

Carbon-based nanostructures possessing {\pi}-electron magnetism have attracted tremendous interest due to their great potential for nano spintronics. In particular, quantum chains with magnetic molecular units synthesized by on-surface reactions provide an ideal playground for investigating magnetic exchange interactions between localized spin components. Here, we present an extensive study of antiferromagnetic nanographene chains with the diazahexabenzocoronene molecule as the repeating unit. A combination of bond-resolved scanning tunneling microscopy, density functional theory and quantum spin models revealed their detailed structures and electronic and magnetic properties. We found that the antiferromagnetic chains host a collective state featuring gapped excitations for an even number of repeating units and one featuring a Kondo excitation for an odd number. Comparing with exact many-body quantum spin models, our molecular chains provide the realization of an entangled quantum Heisenberg model. Coupled with the tunability of the molecular building blocks, these systems can act as an ideal platform for the experimental realization of topological spin lattices.

The emergence of correlated phenomena arising from the combination of 1$\mathrm{T}$ and 1$\mathrm{H}$ van der Waals layers is the focus of intense research. Here, we synthesize a novel self-stacked 6$\mathrm{R}$ phase in NbSeTe, showing a perfect alternating 1T and 1H layers that grow coherently along the c-direction, as revealed by scanning transmission electron microscopy. Angle resolved photoemission spectroscopy shows a mixed contribution of the trigonal and octahedral Nb bands to the Fermi level. Diffuse scattering reveals temperature-independent short-range charge fluctuations with propagation vector $\mathrm{q_{CO}}$=(0.25,0), derived from the condensation of a longitudinal mode in the 1T layer. We observe that ligand disorder quenches the formation of a charge density wave. Magnetization measurements suggest the presence of an inhomogeneous, short-range magnetic order, further supported by the absence of a clear phase transition in the specific heat. These experimental analyses in combination with \textit{ab initio} calculations indicate that the ground state of 6$\mathrm{R}$-NbSeTe is described by a statistical distribution of short-range charge-modulated and spin-correlated regions driven by ligand disorder. Our results devise a route to synthesize 1$\mathrm{T}$-1$\mathrm{H}$ self-stacked bulk heterostructures to study emergent phases of matter., Comment: 12 pages, including Supplementary Information. 4 figures + 6 supplementary figures

CeSiI has been recently isolated in the ultrathin limit, establishing CeSiI as the first intrinsic two-dimensional van der Waals heavy-fermion material up to 85 K. We show that, due to the strong Ce spin-orbit coupling, the local moments develop a multipolar real-space magnetic texture, leading to local pseudospins with a nearly vanishing net moment. To elucidate its Kondo-screened regime, we extract from first principles the parameters of the Kondo lattice model describing this material. We develop a fractional pseudofermion methodology in combination with ab initio calculations to reveal the nature of the Kondo-screened heavy fermion state in CeSiI. Using this formalism, we analyze the competing magnetic interactions leading to a heavy-fermion order as a function of the magnetic exchange between the localized f-electrons and the strength of the Kondo coupling. Our results show that the magnetic exchange interactions promote an unconventional momentum-dependent heavy-fermion Kondo screened phase, establishing the nature of the heavy-fermion behavior of ultrathin CeSiI observed experimentally., Comment: 8 pages, 4 figures

Progress in layered van der Waals materials has resulted in the discovery of ferromagnetic and ferroelectric materials down to the monolayer limit. Recently, evidence of the first purely two-dimensional multiferroic material was reported in monolayer NiI$_2$. However, probing multiferroicity with scattering-based and optical bulk techniques is challenging on 2D materials, and experiments on the atomic scale are needed to fully characterize the multiferroic order at the monolayer limit. Here, we use scanning tunneling microscopy (STM) supported by theoretical calculations based on density functional theory (DFT) to probe and characterize the multiferroic order in monolayer NiI$_2$. We demonstrate that the type-II multiferroic order displayed by NiI$_2$, arising from the combination of a magnetic spin spiral order and a strong spin-orbit coupling, allows probing the multiferroic order in the STM experiments. Moreover, we directly probe the magnetoelectric coupling of NiI$_2$ by external electric field manipulation of the multiferroic domains. Our findings establish a novel point of view to analyse magnetoelectric effects at the microscopic level, paving the way towards engineering new multiferroic orders in van der Waals materials and their heterostructures.

In order to characterize in detail the charge density wave (CDW) transition of 1$T$-VSe$_2$, its electronic structure and lattice dynamics are comprehensively studied by means of x-ray diffraction, angle resolved photoemission (ARPES), diffuse and inelastic x-ray scattering (IXS), and state-of-the-art first principles density functional theory calculations. Resonant elastic x-ray scattering (REXS) does not show any resonant enhancement at either V or Se K-edges, indicating that the CDW peak describes a purely structural modulation of the electronic ordering. ARPES identifies (i) a pseudogap at T$>$T$_{CDW}$, which leads to a depletion of the density of states in the $ML-M'L'$ plane at T$<$T$_{CDW}$, and (ii) anomalies in the electronic dispersion reflecting a sizable impact of phonons on it. A diffuse scattering precursor, characteristic of soft phonons, is observed at room temperature (RT) and leads to the full collapse of the low-energy phonon ($\omega_1$) with propagation vector (0.25 0 -0.3) r.l.u. We show that the frequency and linewidth of this mode are anisotropic in momentum space, reflecting the momentum dependence of the electron-phonon interaction (EPI), hence demonstrating that the origin of the CDW is, to a much larger extent, due to the momentum dependence EPI with a small contribution from nesting. The pressure dependence of the $\omega_1$ soft mode remains nearly constant up to 13 GPa at RT, with only a modest softening before the transition to the high-pressure monoclinic $C2/m$ phase. The wide set of experimental data are well captured by our state-of-the art first-principles anharmonic calculations with the inclusion of van der Waals (vdW) corrections in the exchange-correlation functional. The description of the electronics and dynamics of VSe$_2$ reported here adds important pieces of information to the understanding of the electronic modulations of TMDs.

The emergence of symmetry-breaking orders such as ferromagnetism and the weak interlayer bonding in van der Waals materials, offers a unique platform to engineer novel heterostructures and tune transport properties like thermal conductivity. Here, we report the experimental and theoretical study of the cross-plane thermal conductivity, $\kappa_\perp$, of the van der Waals 2D ferromagnet Fe$_3$GeTe$_2$. We observe a non-monotonic increase of $\kappa_\perp$ with the thickness and a large suppression in artificially-stacked layers, indicating a diffusive transport regime with ballistic contributions. These results are supported by the theoretical analyses of the accumulated thermal conductivity, which show an important contribution of phonons with mean free paths between 10 and 200 nm. Moreover, our experiments show a reduction of the $\kappa_\perp$ in the low-temperature ferromagnetic phase occurring at the magnetic transition. The calculations show that this reduction in $\kappa_\perp$ is associated with a decrease in the group velocities of the acoustic phonons and an increase in the phonon-phonon scattering of the Raman modes that couple to the magnetic phase. These results demonstrate the potential of van der Waals ferromagnets for thermal transport engineering.

Two-dimensional van der Waals materials have become an established platform to engineer flat bands which can lead to strongly-correlated emergent phenomena. In particular, the family of Ta dichalcogenides in the 1\textit{T} phase presents a star-of-David charge density wave that creates a flat band at the Fermi level. For TaS$_2$ and TaSe$_2$ this flat band is at half filling leading to a magnetic insulating phase. In this work, we theoretically demonstrate that ligand substitution in the TaSe$_{2-x}$Te$_x$ system produces a transition from the magnetic insulator to a non-magnetic metal in which the flat band gets doped away from half-filling. For $x\in[{0.846},{1.231}]$ the spin-polarized flat band is self-doped and the system becomes a magnetic metal. In this regime, we show that attractive interactions promote three different spin-triplet superconducting phases as a function of $x$, corresponding to a nodal f-wave and two topologically-different chiral p-wave superconducting phases. Our results establish monolayer TaSe$_{2-x}$Te$_{x}$ as a promising platform for correlated flat band physics leading to unconventional superconducting states., Comment: 6 pages, 4 figures and suplemental material

Mixed halide chemistry has recently been utilized to tune the intrinsic magnetic properties of transition-metal halides $-$ one of the largest families of magnetic van der Waals materials. Prior studies have shown that the strength of exchange interactions, hence the critical temperature, can be tuned smoothly with halide composition for a given ground-state. Here we show that the ground-state itself can be altered by a small change of halide composition leading to a quantum phase transition in FeCl$_{3-x}$Br$_x$. Specifically, we find a three-fold jump in the N\'{e}el temperature and a sign change in the Weiss temperature at $x= 0.08$ corresponding to only $3\%$ bromine doping. Using neutron scattering, we reveal a change of the ground-state from spiral order in FeCl$_3$ to A-type antiferromagnetic order in FeBr$_3$. Using first-principles calculations, we show that a delicate balance between nearest and next-nearest neighbor interactions is responsible for such a transition. These results support the proximity of FeCl$_3$ to a spiral spin liquid state, in which competing interactions and nearly degenerate magnetic $k$-vectors may cause large changes in response to small perturbations., Comment: 6 pages, 4 figures

Quantum-disordered models provide a versatile platform to explore the emergence of quantum excitations in many-body systems. The engineering of spin models at the atomic scale with scanning tunneling microscopy and the local imaging of excitations with electrically driven spin resonance has risen as a powerful strategy to image spin excitations in finite quantum spin systems. Here, focusing on $S=1/2$ lattices as realized by Ti in MgO, we show that dynamical spin excitations provide a robust strategy to infer the nature of the underlying Hamiltonian. We show that finite-size interference of the dynamical many-body spin excitations of a generalized long-range Heisenberg model allows the underlying spin couplings to be inferred. We show that the spatial distribution of local spin excitations in Ti islands and ladders directly correlates with the underlying ground state in the thermodynamic limit. Using a supervised learning algorithm, we demonstrate that the different parameters of the Hamiltonian can be extracted by providing the spatially and frequency-dependent local excitations that can be directly measured by electrically driven spin resonance with scanning tunneling microscopy. Our results put forward local dynamical excitations in confined quantum spin models as versatile witnesses of the underlying ground state, providing an experimentally robust strategy for Hamiltonian inference in complex real spin models., Comment: 11 pages, 10 figures

We investigate the electronic structure of Cs$_2$CuCl$_4$, a material discussed in the framework of a frustrated quantum antiferromagnet, by means of resonant inelastic x-ray scattering (RIXS) and Density Functional Theory (DFT). From the non-dispersive highly localized dd excitations, we resolve the crystal field splitting of the Cu$^{2+}$ ions in a strongly distorted tetrahedral coordination. This allows us to model the RIXS spectrum within the Crystal Field Theory (CFT), assign the dd orbital excitations and retrieve experimentally the values of the crystal field splitting parameters D$_q$, D$_s$ and D$_{\tau}$. The electronic structure obtained ab-initio agrees with the RIXS spectrum and modelled by CFT, highlighting the potential of combined spectroscopic, cluster and DFT calculations to determine the electronic ground state of complex materials., Comment: 7 pages, 4 figures

VSe$_2$ is a layered compound that has attracted great attention due to its proximity to a ferromagnetic state that is quenched by the presence of a charge density wave (CDW) phase. In the monolayer limit, unrelated experiments have reported different CDW orders with transition temperatures in the range of 130 to 220 K, making this monolayer very controversial. Here we perform first-principles non-perturbative anharmonic phonon calculations in monolayer VSe$_2$ in order to estimate the CDW order and the corresponding transition temperature. Our analysis solves previous experimental contradictions as we reveal that monolayer VSe$_2$ develops two independent charge density wave orders associated to $\sqrt{3} \times \sqrt{7}$ and $4 \times 4$ modulations that compete as a function of strain. In fact, tiny variations of only 1.5% in the lattice parameter are enough to stabilize one order or the other, which underlines that the CDW order becomes substrate-dependent. The predicted CDW temperature is strain-dependent and has a value of around 220 K, in good agreement with experiments. Moreover, we analyze the impact of external Lennard-Jones interactions on the CDW. We show that these can act together with the anharmonicity to suppress the CDW orders. In the particular case of monolayer VSe$_2$, this may give rise to the emergence of a ferromagnetic order., Comment: 8 pages, 4 figures, and supplemental material

Ferroelectric van der Waals heterostructures provide a natural platform to design a variety of electrically controllable devices. In this work, we demonstrate that AB bilayer graphene encapsulated in MoTe$_2$ acts as a valley valve that displays a switchable built-in topological gap, leading to ferroelectrically driven topological channels. Using a combination of ab initio calculations and low energy models, we show that the ferroelectric order of MoTe$_2$ allows the control of the gap opening in bilayer graphene and leads to topological channels between different ferroelectric domains. Moreover, we analyze the effect that the moir\'e modulation between MoTe$_2$ and graphene layers has in the topological modes, demonstrating that the edge states are robust against moir\'e modulations of the ferroelectrically-induced electric potential. Our results put forward ferroelectric/graphene heterostructures as versatile platforms to engineer switchable built-in topological channels without requiring an external electric bias., Comment: 8 pages, 4 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 moir\'e 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 moir\'e 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 moir\'e. 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., Comment: 5+3 pages, 4 figures, supplemental material

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., Comment: Submission to SciPost, 6 figures

The discovery of multiferroic behavior in monolayer NiI$_2$ provides a new symmetry-broken state in van der Waals monolayers, featuring the simultaneous emergence of helimagnetic order and ferroelectric order at a critical temperature of $T=21$ K. However, the microscopic origin of multiferroic order in NiI$_2$ monolayer has not been established, and in particular, the role of non-colinear magnetism and spin-orbit coupling in this compound remains an open problem. Here we reveal the origin of the two-dimensional multiferroicity in NiI$_2$ using first-principles electronic structure methods. We show that the helimagnetic state appears as a consequence of the long-range magnetic exchange interactions, featuring sizable magnetic moments in the iodine atoms. We demonstrate that the electronic density reconstruction accounting for the ferroelectric order emerges from the interplay of non-collinear magnetism and spin-orbit coupling. We demonstrate that the ferroelectric order is controlled by the iodine spin-orbit coupling, and leads to an associated electronically-driven distortion in the lattice. Our results establish the microscopic origin of the multiferroic behavior in monolayer NiI$_2$, putting forward the coexistence of helical magnetic order and ligand spin-orbit coupling as driving forces for multiferroic behavior in two-dimensional materials., Comment: 7 pages, 4 figures

The recent discovery of high-T$_{c}$ superconductivity (HTS) in Sr-doped NdNiO$_2$ has sparked a renewed interest in investigating nickelates as cuprate counterparts. Parent cuprates [Cu$^{2+}$: d$^9$] are antiferromagnetic charge-transfer insulators with the involvement of a single d$_{x^2-y^2}$ band around the Fermi level and strong $p-d$ hybridization. In contrast, isoelectronic NdNiO$_2$ [Ni$^+$: d$^9$] is metallic with a d$_{x^2-y^2}$ band self-doped by Nd-d states. Using first-principles calculations, we study the effect of Sr-doping in the electronic and magnetic properties of infinite-layer nickelates as well as the nature of the holes. We find that hole doping tends to make the material more cuprate-like as it minimizes the self-doping effect, it enhances the $p-d$ hybridization, and it produces low-spin (S=0, non-magnetic) Ni$^{2+}$ dopants in analogy with the S=0 Zhang-Rice singlets that appear in cuprates., Comment: 7 pages, 7 figures

The application of pressure has been demonstrated to induce intriguing phase transitions in topological nodal-line semimetals. In this work we analyze how uniaxial pressure affects the topological character of BaSn2 , a Dirac nodal-line semimetal in the absence of spin-orbit coupling. Using calculations based on the density functional theory and a model tight-binding Hamiltonian, we find the emergence of a second nodal line for pressures higher than 4 GPa. We examine the topological features of both phases demonstrating that a nontrivial character is present in both of them. Thus, providing evidence of a topological-to-topological phase transition in which the number of topological nodal lines increases. The orbital overlap increase between Ba dxz and dyz orbitals and Sn pz orbitals and the preservation of crystal symmetries are found to be responsible for the advent of this transition. Furthermore, we pave the way to experimentally test this kind of transition by obtaining a topological relation between the zero-energy modes that arise in each phase when a magnetic field is applied.

Transition metal dichalcogenides are promising candidates to show long-range ferromagnetic order in the single-layer limit. Based on ab initio calculations, we report the emergence of a charge density wave (CDW) phase in monolayer 1T-CrTe$_2$. We demonstrate that this phase is the ground state in the single-layer limit at any strain value. We obtain an optical phonon mode of $1.96$ THz that connects CDW phase with the undistorted 1T phase. Localization of the $a_{1g}$ orbital of CrTe$_2$ produces an out-of-plane orientation of the magnetic moments, circumventing the restrictions of the Mermin-Wagner theorem and producing ferromagnetic long-range order in the two-dimensional limit. This orbital-localization is enhanced by the CDW phase. Tensile strain also increases the localization of this orbital driving the system to become ordered. CrTe$_2$ becomes an example of a material where the CDW phase produces the stabilization of the long-range ferromagnetic order. Our results show that both strain and phase switching are mechanisms to control the 2D ferromagnetic order of CrTe$_2$.

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.

We present a detailed analysis of the structure dependence of the lattice thermal conductivity of SrTiO3. We have used both ab initio Molecular Dynamic simulations and Density Functional Theory calculations to decouple the effect of different structural distortions on the thermal conductivity. We have identified two main mechanisms for tuning the thermal conductivity when a distortion is applied. First, the modification of the acoustic-modes energy dispersion when a change in the lattice parameters is imposed and second, the low energy polar modes. In particular and counterintuitively, we have found that an increase in the angle of the oxygen octahedral rotations increases the thermal conductivity due to its coupling to these polar modes.

How magnetism emerges in low-dimensional materials such as transition metal dichalcogenides at the monolayer limit is still an open question. Herein, we present a comprehensive study of the magnetic properties of single crystal and monolayer VSe$_{2}$, both experimentally and \emph{ab initio}. Magnetometry, X-ray magnetic circular dichrosim (XMCD) and \emph{ab initio} calculations demonstrate that the charge density wave in bulk stoichiometric VSe$_{2.0}$ causes a structural distortion with a strong reduction in the density of sates at the Fermi level, prompting the system towards a non-magnetic state but on the verge of a ferromagnetic instability. In the monolayer limit, the structural rearrangement induces a Peierls distortion with the opening of an energy gap at the Fermi level and the absence of magnetic order. Control experiments on defect-induced VSe$_{2-\delta}$ single crystals show a breakdown of magnetism, discarding vacancies as a possible origin of magnetic order in VSe$_{2}$., Comment: polished version, updated acknowledgments

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

In this paper we explore the different mechanisms that affect the thermopower of a band insulating perovskite (in this case, SrTiO$_3$) when subject to strain (both compressive or tensile). We analyze the high temperature, entropy dominated limit and the lower temperature, energy-transport regime. We observe that the effect of strain in the high-temperature Seebeck coefficient is small at the concentration levels of interest for thermoelectric applications. However, the effective mass changes substantially with strain, which produces an opposite effect to that of the degeneracy-breakups produced by strain. In particular, we find that the thermopower can be enhanced by applying tensile strain in the adequate regime. We conclude that the detrimental effect of strain in thermopower due to band splitting is a minor effect that will not hamper the optimization of the thermoelectric properties of oxides with t$_{2g}$-active bands by applying strain., Comment: 10 pages, 7 figures