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Knowledge of the occupation ratio and the energy splitting of a two-level system yields a direct readout of its temperature. Based on this principle, the determination of the temperature of an individual two-level magnetic atom was demonstrated using Electron Spin Resonance (ESR) via Scanning Tunneling Microscopy (ESR-STM). The temperature determination proceeds in two steps. First, energy splitting is determined using ESR-STM. Second, the equilibrium occupation of the two-level atom is determined in a resonance experiment of a second nearby atom, that has now two different resonant peaks, associated to the two states of the magnetic two-level atom. The ratio of the heights of its resonance peaks yields the occupation ratio. Here we present theory work to address three key aspects: first, we find how shot-noise and back-action limit the precision of this thermometry method; second, we study how the geometry of the nearby spins can be used to enhance signal-to-noise ratio. We predict ESR-STM thermometry can achieve a resolution of 10 mK using temperatures in the T= 1K range. Third, we show how ESR-STM thermometry can be used to detect thermal gradients as small as 5 mK/nm.

A generalization of the graphene honeycomb model to the case where each site in the honeycomb lattice contains a $n-$fold degenerate set of eigenstates of the $C_3$ symmetry has been recently proposed to describe several systems, including triangulene crystals and photonic lattices. These generalized honeycomb models are defined by $(n_a,n_b)$, the number $C_3$ eigenstates in the $a$ and $b$ sites of the unit cell, resulting in $n_a+n_b$ bands. Thus, the $(1,1)$ case gives the coventional honeycomb model that describes the two low-energy bands in graphene. Generalizations, such as $(2,1)$, $(2,2)$ and $(3,3)$ display several non-trivial features, such as coexisting graphene-like Dirac cones with flat-bands, both at zero and finite-energy, as well as robust degeneracy points where a flat-band and a parabolic band meet at the $\Gamma$-point. Here, we explore the edge states of this class of crystals, using as reference triangulene crystals, and we find several types of edge states absent in the conventional $(1,1)$ honeycomb case, associated to the non-trivial features of the two-dimensional (2D) bands of the high-fold case. First, we find dispersive edge states associated to the finite-energy flat-bands, that occur both at the armchair and zigzag termination. Second, in the case of non-centrosymmetric triangulene crystals that lead to a $S=1$ Dirac band, we have a bonding-antibonding pair of dispersive edge states, localized in the same edge so that their energy splitting is reduced as their localization increases, opposite to the conventional behavior of pairs of states localized in opposite edges. Third, for the $(3,3)$ case, that hosts a gap separating a pair of flat conduction and valence bands, we find non-dispersive edge states with $E=0$ in all edge terminations., Comment: 15 pages, 7 figures

Altermagnets are a new class of magnetic materials with zero net magnetization (like antiferromagnets) but spin-split electronic bands (like ferromagnets) over a fraction of reciprocal space. As in antiferromagnets, magnons in altermagnets come in two flavours, that either add one or remove one unit of spin to the $S=0$ ground state. However, in altermagnets these two magnon modes are non-degenerate along some directions in reciprocal space. Here we show that the lifetime of altermagnetic magnons has a very strong dependence on both flavour and direction. Strikingly, coupling to Stoner modes leads to a complete suppression of magnon propagation along selected spatial directions. This giant anisotropy will impact electronic, spin, and energy transport properties and may be exploited in spintronic applications., Comment: 9 pages, 11 figures (including the appendices)

The study of open-shell nanographenes has relied on a paradigm where spins are the only low-energy degrees of freedom. Here we show that some nanographenes can host low-energy excitations that include strongly coupled spin and orbital degrees of freedom. The key ingredient is the existence of orbital degeneracy, as a consequence of leaving the benzenoid/half-filling scenario. We analyze the case of nitrogen-doped triangulenes, using both density-functional theory and Hubbard model multiconfigurational and random-phase approximation calculations. We find a rich interplay between orbital and spin degrees of freedom that confirms the need to go beyond the spin-only paradigm, opening a new venue in this field of research., Comment: 6 pages, 4 figures

Motivated by recent experimental breakthroughs, we propose a strategy to design two-dimensional spin lattices with competing interactions that lead to non-trivial emergent quantum states. We consider $S=1/2$ nanographenes with $C_3$ symmetry as building blocks, and we leverage the potential to control both the sign and the strength of exchange with first neighbours to build a family of spin models. Specifically, we consider the case of a Heisenberg model in a triangle-decorated honeycomb lattice with competing ferromagnetic and antiferromagnetic interactions whose ratio can be varied in a wide range. Based on exact diagonalization of both fermionic and spin models we predict a quantum phase transition between a valence bond crystal of spin singlets with triplon excitations living in a Kagom\'e lattice and a N\'eel phase of effective $S=3/2$ in the limit of dominant ferromagnetic interactions., Comment: 6 pages, 4 figures

Phenalenyl is a radical nanographene with triangular shape that hosts an unpaired electron with spin S = 1/2. The open-shell nature of phenalenyl is expected to be retained in covalently bonded networks. Here, we study a first step in that direction and report the synthesis of the phenalenyl dimer by combining in-solution synthesis and on-surface activation and its characterization both on Au(111) and on a monolayer of NaCl on top of Au(111) by means of inelastic electron tunneling spectroscopy (IETS). IETS shows inelastic steps that, together with a thorough theoretical analysis, are identified as the singlet-triplet excitation arising from interphenalenyl exchange. Two prominent features of our data permit to shed light on the nature of spin interactions in this system. First, the excitation energies with and without the NaCl decoupling layer are 48 and 41 meV, respectively, indicating a significant renormalization of the spin excitation energies due to exchange with the Au(111) electrons. Second, a position-dependent bias-asymmetry of the height of the inelastic steps is accounted for by an interphenalenyl hybridization of the singly occupied phenalenyl orbitals that is only possible via third neighbor hopping. This hybridization is also essential to activate kinetic interphenalenyl exchange. Our results set the stage for future work on the bottom-up synthesis of spin S = 1/2 spin lattices with large exchange interaction., Comment: 16 pages main manuscript, 4 main figures; supplementary information containing additional data is included

Nanographene triangulenes with a S = 1 ground state have been used as building blocks of antiferromagnetic Haldane spin chains realizing a symmetry protected topological phase. By means of inelastic electron spectroscopy, it was found that the intermolecular exchange contains both linear and non-linear interactions, realizing the bilinear-biquadratic Hamiltonian. Starting from a Hubbard model, and mapping it to an interacting Creutz ladder, we analytically derive these effective spin-interactions using perturbation theory, up to fourth order. We find that for chains with more than two units other interactions arise, with same order-of-magnitude strength, that entail second neighbor linear, and three-site non-linear exchange. Our analytical expressions compare well with experimental and numerical results. We discuss the extension to general S = 1 molecules, and give numerical results for the strength of the non-linear exchange for several nanographenes. Our results pave the way towards rational design of spin Hamiltonians for nanographene based spin chains., Comment: 21 pages, 8 figures

We provide a comprehensive theory of magnetic phases in two-dimensional triangulene crystals, using both Hubbard model and density functional theory (DFT) calculations. We consider centrosymmetric and non-centrosymmetric triangulene crystals. In all cases, DFT and mean-field Hubbard model predict the emergence of broken-symmetry antiferromagnetic (ferrimagnetic) phases for the centrosymmetric (non-centrosymmetric) crystals. This includes the special case of the [4,4]triangulene crystal, whose non-interacting energy bands feature a gap with flat valence and conduction bands. We show how the lack of contrast between the local density of states of these bands, recently measured via scanning tunneling spectroscopy, is a natural consequence of a broken-symmetry N\'eel state that blocks intermolecular hybridization. Using random phase approximation, we also compute the spin wave spectrum of these crystals, including the recently synthesized [4,4]triangulene crystal. The results are in excellent agreement with the predictions of a Heisenberg spin model derived from multi-configuration calculations for the unit cell. We conclude that experimental results are compatible with an antiferromagnetically ordered phase where each triangulene retains the spin predicted for the isolated species.

The scalar spin chirality is a three-body physical observable that plays an outstanding role both in classical magnetism, characterizing non-coplanar spin textures, and in quantum magnetism, as an order parameter for chiral spin liquids. In quantum information, the scalar spin chirality is a witness of genuine tripartite entanglement. Here we propose an indirect measurement scheme, based on the Hadamard test, to estimate the scalar spin chirality for general quantum states. We apply our method to study chirality in two types of quantum states: generic one-magnon states of a ferromagnet, and the ground state of a model with competing symmetric and antisymmetric exchange. We show a single-shot determination of the scalar chirality is possible for chirality eigenstates, via quantum phase estimation with a single auxiliary qutrit. Our approach provides a unified theory of chirality in classical and quantum magnetism., Comment: 5 pages, 3 figures

We propose a new class of magnetic proximity effects based on the spin dependent hybridization between the electronic states at the Fermi energy in a non-magnetic conductor and the narrow spin split bands of a ferromagnetic insulator. Unlike conventional exchange proximity, we show this hybridization proximity effect has a very strong influence on the non-magnetic layer and can be further modulated by application of an electric field. We use DFT calculations to illustrate this effect in graphene placed next to a monolayer of CrI$_3$, a ferromagnetic insulator. We find strong hybridization of the graphene bands with the narrow conduction band of CrI$_3$ in one spin channel only. We show that our results are robust with respect to lattice mismatch and twist angle variations. Furthermore, we show that an out-of-plane electric field can be used to modulate the hybridization strength, paving the way for applications., Comment: 6 pages, 4 figures

We study indirect exchange interactions between localized spins of magnetic impurities in spin-valley coupled systems described with the Kane-Mele model. Our model captures the main ingredients of the energy bands of 1H transition metal dichalcogenides (TMDs) monolayers, such as 1H-MoS$_2$ and 1H-NbSe$_2$. To obtain the effective interactions, we use the exact diagonalization of the Hamiltonian, avoiding momentum cut-offs. We start by comparing the standard perturbation expansion in terms of the Kondo exchange with the exact calculation of the interaction, treating the local spins classically. We find that perturbation theory works well even beyond the regime where the relevant figure of merit, the ratio between the exchange $J$ and the hopping $t$, is small. We verify that the effective indirect exchange Hamiltonian derived from perturbation theory also works in the non-perturbative regime. Additionally, we analyse the interplay between the symmetry of the different terms of the interaction (Heisenberg, Ising, and Dzyaloshinskii$-$Moriya (DM)), the Fermi-surface topology, and the crystallographic direction in which the impurities are placed. We show that the indirect exchange along the armchair direction is actually Heisenberg-like, due to the reflection symmetry of the crystal structure around this direction. Finally, we explore the exploitation of indirect exchange, combined with atomic manipulation, to engineer the Majumdar-Ghosh Model. Our results show that TMDs provide an extremely versatile platform to engineer indirect exchange interactions., Comment: 13 pages, 7 figures

We propose a protocol to certify the presence of entanglement in artificial on-surface atomic and molecular spin arrays using electron spin resonance carried by scanning tunnel microscopes (ESR-STM). We first generalize the theorem that relates global spin susceptibility as an entanglement witness to the case of anisotropic Zeeman interactions, relevant for surfaces. We then propose a method to measure the spin susceptibilities of surface-spin arrays combining ESR-STM with atomic manipulation. Our calculations show that entanglement can be certified in antiferromagnetically coupled spin dimers and trimers with state of the art ESR-STM magnetometry.

Magnons and plasmons are two very different types of collective modes, acting on the spin and charge degrees of freedom, respectively. At first sight, the formation of hybrid plasmon-magnon polaritons in heterostructures of plasmonic and magnetic systems would face two challenges, the small mutual interaction, via Zeeman coupling of the electromagnetic field of the plasmon with the spins, and the energy mismatch, as in most systems plasmons have energies in the eV range, orders of magnitude larger than magnons. Here we show that graphene plasmons form polaritons with the magnons of two-dimensional ferrromagnetic insulators, placed up to to half a micron apart, with Rabi couplings in the range of 100 GHz (dramatically larger than cavity QED magnonics). This strong coupling is facilitated both by the small energy of graphene plasmons and the cooperative super-radiant nature of the plasmon-magnon coupling afforded by phase matching. We show that the Rabi coupling can be modulated both electrically and mechanically and we propose a attenuated total internal reflection experiment to implement ferromagnetic resonance experiments on 2D ferromagnets driven by plasmon excitation., Comment: 7 pages, 3 figures, appendix

The spin and lattice dynamics of a ferromagnetic nanoparticle are studied via molecular dynamics and with semi-classical spin dynamics simulations where spin and lattice degrees of freedom are coupled via a dynamic uniaxial anisotropy term. We show that this model conserves total angular momentum, whereas spin and lattice angular momentum are not conserved. We carry out simulations of the the Einstein-de Haas effect for a Fe nanocluster with more than 500 atoms that is free to rotate, using a modified version of the open-source spinlattice dynamics code (SPILADY). We show that the rate of angular momentum transfer between spin and lattice is proportional to the strength of the magnetic anisotropy interaction. The addition of the anisotropy allows full spin-lattice relaxation to be achieved on previously reported timescales of \sim 100 ps and for tight-binding magnetic anisotropy energies comparable to those of small Fe nanoclusters., Comment: 23 pages, 3 figures

Systems that can be described with the same mathematical models that account for the properties of electrons in graphene are known as graphene-like systems. These include magnons, photons, polaritons, acoustic waves, and electrons in honeycomb lattices, either natural or artificial. All of them feature an outstanding property, the existence of states localized at the edges. We distinguish two classes of edge states depending on whether or not a topological band gap is present in the two-dimensional energy bands. We introduce the theory of edge states in terms of tight-binding models and discuss their properties, with an emphasis on the interplay between their one-way character and the topological nature of the bulk phase., Comment: Invited review chapter for Encyclopedia of Condensed Matter Physics, 2nd edition (Elsevier), 9 pages, 6 figures

Detection is most often the main impediment to reduce the number of spins in paramagnetic resonance experiments. Here we propose a new route to carry out electrically-detected spin resonance of an individual spin, placed at the edge of a quantum spin Hall insulator (QSHI). The edges of a QSHI host a one dimensional electron gas with perfect spin-momentum locking. Therefore, the spin relaxation induced by emission of an electron-hole pair at the edge state of the QSHI can generate current. Here we demonstrate that driving the system with an $AC$ signal, a nonequilibrium occupation can be induced in the absence of applied bias voltage, resulting in a $DC$ measurable current. We compute the $DC$ current as a function of the Rabi frequency $\Omega$, the spin relaxation and decoherence times, $T_1$ and we discuss the feasibility of this experiment with state-of-the-art instrumentation., Comment: 5 pages, 1 figure

A scanning tunneling microscope (STM) can probe the inelastic spin excitations of single magnetic atoms in a surface via spin-flip assisted tunneling. A particular and intriguing case is the Mn dimer case. We show here that the existing theories for inelastic transport spectroscopy do not explain the observed spin transitions when both atoms are equally coupled to the STM tip and the substrate. The hyperfine coupling to the nuclear spins is shown to lead to a finite excitation amplitude, but the physical mechanism leading to the large inelastic signal observed is still unknown. We discuss some other alternatives that break the symmetry of the system and allows for larger excitation probabilities., Comment: 4 pages, 2 figures

Quantum state preparation is a key step in all digital quantum simulation algorithms. Here we propose methods to initialize on a gate-based quantum computer a general class of quantum spin wave functions, the so-called Valence-Bond-Solid (VBS) states, that are important for two reasons. First, VBS states are the exact ground states of a class of interacting quantum spin models introduced by Affleck, Kennedy, Lieb and Tasaki (AKLT). Second, the two-dimensional VBS states are universal resource states for measurement-based quantum computing. We find that schemes to prepare VBS states based on their tensor-network representations yield quantum circuits that are too deep to be within reach of noisy intermediate-scale quantum (NISQ) computers. We then apply the general non-deterministic method herein proposed to the preparation of the spin-1 and spin-3/2 VBS states, the ground states of the AKLT models defined in one dimension and in the honeycomb lattice, respectively. Shallow quantum circuits of depth independent of the lattice size are explicitly derived for both cases, making use of optimization schemes that outperform standard basis gate decomposition methods. Given the probabilistic nature of the proposed routine, two strategies that achieve a quadratic reduction of the repetition overhead for any VBS state defined on a bipartite lattice are devised. Our approach should permit to use NISQ processors to explore the AKLT model and variants thereof, outperforming conventional numerical methods in the near future., Comment: Main text: 17 pages, 7 figures. Appendices: 10 pages, 5 figures. QASM files to be added in next version of preprint

Equilateral triangle-shaped graphene nanoislands with a lateral dimension of $n$ benzene rings are known as $[n]$triangulenes. Individual $[n]$triangulenes are open-shell molecules, with single-particle electronic spectra that host $n-1$ half-filled zero modes and a many-body ground state with spin $S=(n-1)/2$. The on-surface synthesis of triangulenes has been demonstrated for $n=3,4,5,7$ and the observation of a Haldane symmetry-protected topological phase has been reported in chains of $[3]$triangulenes. Here, we provide a unified theory for the electronic properties of a family of two-dimensional honeycomb lattices whose unit cell contains a pair of triangulenes with dimensions $n_a,n_b$. Combining density functional theory and tight-binding calculations, we find a wealth of half-filled narrow bands, including a graphene-like spectrum (for $n_a=n_b=2$), spin-1 Dirac electrons (for $n_a=2,n_b=3$), $p_{x,y}$-orbital physics (for $n_a=n_b=3$), as well as a gapped system with flat valence and conduction bands (for $n_a=n_b=4$). All these results are rationalized with a class of effective Hamiltonians acting on the subspace of the zero-energy states that generalize the graphene honeycomb model to the case of fermions with an internal pseudospin degree of freedom with $C_3$ symmetry., Comment: 12 pages, 7 figures

A theorem that establishes a one-to-one relation between zero-temperature static spin-spin correlators and coupling constants for a general class of quantum spin Hamiltonians bilinear in the spin operators has been recently established by J. Quintanilla, using an argument in the spirit of the Hohenberg-Kohn theorem in density functional theory. Quintanilla's theorem gives a firm theoretical foundation to quantum spin Hamiltonian learning using spin structure factors as input data. Here we extend the validity of the theorem in two directions. First, following the same approach as Mermin, the proof is extended to the case of finite-temperature spin structure factors, thus ensuring that the application of this theorem to experimental data is sound. Second, we note that this theorem applies to all types of Hamiltonians expressed as sums of bilinear operators, so that it can also relate the density-density correlators to the Coulomb matrix elements for interacting electrons in the lowest Landau level., Comment: 4 pages

Paramagnons are the collective modes that govern the spin response of nearly magnetic conductors. In some cases they mediate electron pairing leading to superconductivity. This scenario may occur in 2H-NbSe$_2$ monolayers, that feature spin-valley coupling on account of spin-orbit interactions and their lack of inversion symmetry. Here we explore spin anisotropy of paramagnons both for non-centrosymmetric Kane-Mele-Hubbard models for 2H-NbSe$_2$ monolayers described with a DFT-derived tight-binding model. In the infinite wavelength limit we find spatially uniform paramagnons with energies around $1$~meV that feature a colossal off-plane uniaxial magnetic anisotropy, with quenched transversal spin response. At finite wave vectors, longitudinal and transverse channels reverse roles: XY fluctuations dominate within a significant portion of the Brillouin zone. Our results show that 2H-NbSe$_2$ is close to a Coulomb-driven in-plane (XY) spin density wave instability., Comment: 10 pages (6 main text, 4 supplementary material), 10 figures (4 in the main text, 6 in the SM)

The Haldane phase for antiferromagnetic spin-1 chains is a celebrated topological state of matter, featuring gapped excitations and fractional spin-1/2 edge states. Here, we provide numerical evidence that this phase can be realized with a Hubbard model at half filling, where each $s=1$ spin is stored in a four-site fermionic structure. We find that the noninteracting limit of our proposed model describes a one-dimensional topological insulator, and we conjecture it to be adiabatically connected to the Haldane phase. Our work suggests a route to build spin-1 networks using Hubbard model quantum simulators., Comment: Revised version, including Supplemental Material

We study the emergence of magnetism and its interplay with structural properties in a two dimensional molecular crystal of cyclacenes, using density functional theory (DFT). Isolated cyclacenes with an even number of fused benzenes host two unpaired electrons in two topological protected zero modes, at the top and bottom carbon rings that form the molecule. We show that, in the gas phase, electron repulsion promotes an open-shell singlet with strong intramolecular antiferromagnetic exchange. We consider a closed packing triangular lattice crystal phase and we find a strong dependence of the band structure and magnetic interactions on the rotation angle of the cyclacenes with respect to the crystal lattice vectors. The orientational ground state maximizes the intermolecular hybridization, yet local moments survive. Intermolecular exchange is computed to be antiferromagnetic, and DFT predicts a broken symmetry $120^\circ$ spin phase reflecting the frustration of the intermolecular spin coupling. Thus, the cyclacene crystal realizes a bilayer of two antiferromagnetically coupled S = 1/2 triangular lattices. Our results provide a bottom-up route towards carbon based strongly correlated platforms in two dimensions.

We propose quantum circuits to test interferometric complementarity using symmetric two-way interferometers coupled to a which-path detector. First, we consider the two-qubit setup in which the controlled transfer of path information to the detector subsystem depletes interference on the probed subspace, testing the visibility-distinguishability trade-off via minimum-error state discrimination measurements. Next, we consider the quantum eraser setup, in which reading out path information in the right basis recovers an interference pattern. These experiments are then carried out in an IBM superconducting transmon processor. A detailed analysis of the results is provided. Despite finding good agreement with theory at a coarse level, we also identify small but persistent systematic deviations preventing the observation of full particle-like and wave-like statistics. We understand them by carefully modeling two-qubit gates, showing that even small coherent errors in their implementation preclude the observation of Bohr's strong formulation of complementarity., Comment: 18 pages, 8 figures

We study the electronic properties of the heterobilayer of vanadium and iron oxychlorides, VOCl and FeOCl, two layered air stable van der Waals insulating oxides with different types of antiferromagnetic order in bulk: VOCl monolayers are ferromagnetic (FM) whereas the FeOCl monolayers are antiferromagnetic (AF). We use density functional theory (DFT) calculations, with Hubbard correction that is found to be needed to describe correctly the insulating nature of these compounds. We compute the magnetic anisotropy and propose a spin model Hamiltonian. Our calculations show that interlayer coupling in weak and ferromagnetic so that magnetic order of the monolayers is preserved in the heterobilayers providing thereby a van der Waals heterostructure that combines two monolayers with different magnetic order. Interlayer exchange should lead both to exchange bias and to the emergence of hybrid collective modes that that combine FM and AF magnons. The energy band of the heterobilayer show a type II band alignment, and feature spin-splitting of the states of the AF layer due to the breaking of the inversion symmetry., Comment: 6 pages, 3 figures

When magnetic atoms are inserted inside a superconductor, the superconducting order is locally depleted as a result of the antagonistic nature of magnetism and superconductivity1. Thereby, distinctive spectral features, known as Yu-Shiba-Rusinov states, appear inside the superconducting gap2-4. The search for Yu-Shiba-Rusinov states in different materials is intense, as they can be used as building blocks to promote Majorana modes5 suitable for topological quantum computing6. Here we report the first realization of Yu-Shiba-Rusinov states in graphene, a non-superconducting 2D material, and without the participation of magnetic atoms. We induce superconductivity in graphene by proximity effect7-9 brought by adsorbing nanometer scale superconducting Pb islands. Using scanning tunneling microscopy and spectroscopy we measure the superconducting proximity gap in graphene and we visualize Yu-Shiba-Rusinov states in graphene grain boundaries. Our results reveal the very special nature of those Yu-Shiba-Rusinov states, which extends more than 20 nm away from the grain boundaries. These observations provide the long sought experimental confirmation that graphene grain boundaries host local magnetic moments10-14 and constitute the first observation of Yu-Shiba-Rusinov states in a chemically pure system.

The discovery of ferromagnetic order in monolayer 2D crystals has opened a new venue in the field of two dimensional (2D) materials. 2D magnets are not only interesting on their own, but their integration in van der Waals heterostructures allows for the observation of new and exotic effects in the ultrathin limit. The family of Chromium trihalides, CrI$_3$, CrBr$_3$ and CrCl$_3$, is, so far, the most studied among magnetic 2D crystals. In this mini-review, we provide a perspective of the state of the art of the theoretical understanding of magnetic 2D trihalides, most of which will also be relevant for other 2D magnets, such as vanadium trihalides. We discuss both the well-established facts, such as the origin of the magnetic moment and magnetic anisotropy and address as well open issues such as the nature of the anisotropic spin couplings and the magnitude of the magnon gap. Recent theoretical predictions on Moir\' e magnets and magnetic skyrmions are also discussed. Finally, we give some prospects about the future interest of these materials and possible device applications., Comment: This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in Nano Letters, copyright \c{opyright} American Chemical Society after peer review

Quantum confinement of graphene Dirac-like electrons in artificially crafted nanometer structures is a long sought goal that would provide a strategy to selectively tune the electronic properties of graphene, including bandgap opening or quantization of energy levels However, creating confining structures with nanometer precision in shape, size and location, remains as an experimental challenge, both for top-down and bottom-up approaches. Moreover, Klein tunneling, offering an escape route to graphene electrons, limits the efficiency of electrostatic confinement. Here, a scanning tunneling microscope (STM) is used to create graphene nanopatterns, with sub-nanometer precision, by the collective manipulation of a large number of H atoms. Individual graphene nanostructures are built at selected locations, with predetermined orientations and shapes, and with dimensions going all the way from 2 nanometers up to 1 micron. The method permits to erase and rebuild the patterns at will, and it can be implemented on different graphene substrates. STM experiments demonstrate that such graphene nanostructures confine very efficiently graphene Dirac quasiparticles, both in zero and one dimensional structures. In graphene quantum dots, perfectly defined energy band gaps up to 0.8 eV are found, that scale as the inverse of the dots linear dimension, as expected for massless Dirac fermions, Comment: Main Manuscript and Supporting Information

Non reciprocal spin waves have a chiral asymmetry so that their energy is different for two opposite wave vectors. They are found in atomically thin ferromagnetic overlayers with in plane magnetization and are linked to the anti-symmetric Dzyaloshinskii-Moriya surface exchange. We use an itinerant fermion theory based on first principles calculations to predict that non-reciprocal magnons can occur in Fe$_3$GeTe$_2$, the first stand alone metallic two dimensional crystal with off-plane magnetization. We find that both the energy and lifetime of magnons are non-reciprocal and we predict that acoustic magnons can have lifetimes up to hundreds of picoseconds, orders of magnitude larger than in other conducting magnets., Comment: 5 pages, 4 figure; supplemental material: 5 pages, 5 figures

Semiconducting ferromagnet-nonmagnet interfaces in van der Waals heterostructures present a unique opportunity to investigate magnetic proximity interactions dependent upon a multitude of phenomena including valley and layer pseudospins, moir\'e periodicity, or exceptionally strong Coulomb binding. Here, we report a charge-state dependency of the magnetic proximity effects between MoSe$_2$ and CrBr$_3$ in photoluminescence, whereby the valley polarization of the MoSe$_2$ trion state conforms closely to the local CrBr$_3$ magnetization, while the neutral exciton state remains insensitive to the ferromagnet. We attribute this to spin-dependent interlayer charge transfer occurring on timescales between the exciton and trion radiative lifetimes. Going further, we uncover by both the magneto-optical Kerr effect and photoluminescence a domain-like spatial topography of contrasting valley polarization, which we infer to be labyrinthine or otherwise highly intricate, with features smaller than 400 nm corresponding to our optical resolution. Our findings offer a unique insight into the interplay between short-lived valley excitons and spin-dependent interlayer tunnelling, while also highlighting MoSe$_2$ as a promising candidate to optically interface with exotic spin textures in van der Waals structures.

Magnons dominate the magnetic response of the recently discovered insulating ferromagnetic two dimensional crystals such as CrI$_3$. Because of the arrangement of the Cr spins in a honeycomb lattice, magnons in CrI$_3$ bear a strong resemblance with electronic quasiparticles in graphene. Neutron scattering experiments carried out in bulk CrI$_3$ show the existence of a gap at the Dirac points, that has been conjectured to have a topological nature. Here we propose a theory for magnons in ferromagnetic CrI$_3$ monolayers based on an itinerant fermion picture, with a Hamiltonian derived from first principles. We obtain the magnon dispersion for 2D CrI$_3$ with a gap at the Dirac points with the same Berry curvature in both valleys. For CrI$_3$ ribbons, we find chiral in-gap edge states. Analysis of the magnon wave functions in momentum space further confirms their topological nature. Importantly, our approach does not require to define a spin Hamiltonian, and can be applied to both insulating and conducting 2D materials with any type of magnetic order., Comment: Includes supplementary material

In this paper we develop the excitonic theory of Kerr rotation angle in a two-dimensional (2D) transition metal dichalcogenide at zero magnetic field. The finite Kerr angle is induced by the interplay between spin-orbit splitting and proximity exchange coupling due to the presence of a ferromagnet. We compare the excitonic effect with the single particle theory approach. We show that the excitonic properties of the 2D material lead to a dramatic change in the frequency dependence of the optical response function. We also find that the excitonic corrections enhance the optical response by a factor of two in the case of MoS2 in proximity to a Cobalt thin film., Comment: Accepted for publication in Physical Review B

Chromium trihalides (CrI$_3$, CrBr$_3$ and CrCl$_3$) form a prominent family of isostructural insulating layered materials in which ferromagnetic order has been observed down to the monolayer. Here we provide a comprehensive computational study of magneto-optical properties that are used as probes for the monolayer ferromagnetic order: magnetic circular dichroism and magneto-optic Kerr effect. Using a combination of density functional and Bethe-Salpeter theories, we calculate both the optical absorption and the magneto-optical Kerr angle spectra, including both excitonic effects and spinorial wave functions. We compare the magneto-optical response of the chromium trihalides series and we find that its strength is governed by the spin-orbit coupling of the ligand atoms (I, Br, Cl).

Two-dimensional (2D) massive Dirac electrons possess a finite Berry curvature, with Chern number $\pm 1/2$, that entails both a quantized dc Hall response and a subgap full-quarter Kerr rotation. The observation of these effects in 2D massive Dirac materials such as gapped graphene, hexagonal boron nitride or transition metal dichalcogenides (TMDs) is obscured by the fact that Dirac cones come in pairs with opposite sign Berry curvatures, leading to a vanishing Chern number. Here, we show that the presence of spin-orbit interactions, combined with an exchange spin splitting induced either by diluted magnetic impurities or by proximity to a ferromagnetic insulator, gives origin to a net magneto-optical Kerr effect in such systems. We focus on the case of TMD monolayers and study the dependence of Kerr rotation on frequency and exchange spin splitting. The role of the substrate is included in the theory and found to critically affect the results. Our calculations indicate that state-of-the-art magneto-optical Kerr spectroscopy can detect a single magnetic impurity in diluted magnetic TMDs., Comment: 8 pages, 3 figures

We revisit quantum phase estimation algorithms for the purpose of obtaining the energy levels of many-body Hamiltonians and pay particular attention to the statistical analysis of their outputs. We introduce the mean phase direction of the parent distribution associated with eigenstate inputs as a new post-processing tool. By connecting it with the unknown phase, we find that if used as its direct estimator, it exceeds the accuracy of the standard majority rule using one less bit of resolution, making evident that it can also be inverted to provide unbiased estimation. Moreover, we show how to directly use this quantity to accurately find the energy levels when the initialized state is an eigenstate of the simulated propagator during the whole time evolution, which allows for shallower algorithms. We then use IBM Q hardware to carry out the digital quantum simulation of three toy models: a two-level system, a two-spin Ising model and a two-site Hubbard model at half-filling. Methodologies are provided to implement Trotterization and reduce the variability of results in noisy intermediate scale quantum computers., Comment: 16 pages, 15 figures

Gate-based quantum computers can in principle simulate the adiabatic dynamics of a large class of Hamiltonians. Here we consider the cyclic adiabatic evolution of a parameter in the Hamiltonian. We propose a quantum algorithm to estimate the Berry phase and use it to classify the topological order of both single-particle and interacting models, highlighting the differences between the two. This algorithm is immediately extensible to any interacting topological system. Our results evidence the potential of near-term quantum hardware for the topological classification of quantum matter., Comment: Main text: 4 pages, 3 figures; Supplemental material: 9 pages, 9 figures

In this book chapter, we introduce different schemes to create quantum states of matter in engineered graphene nanoribbons. We will focus on the emergence of controllable magnetic interactions, topological quantum magnets, and the interplay of magnetism and superconductivity. We comment on the experimental signatures of those states stemming from their electronic and spin excitations, that can be observed with atomic resolution using scanning probe techniques., Comment: 14 pages, 9 figures. Submitted book chapter for "Graphene Nanoribbons", Edited by A. Tejeda, P. Seneor, L. Brey

We propose a method to realize a broad class of tunable fermionic Hamiltonians in graphene bilayer. For that matter, we consider graphene bilayer functionalized with sp$^3$ defects that induce zero energy resonances hosting an individual electron each. The application of an off-plane electric field opens up a gap, so that the zero energy resonance becomes an in-gap bound state whose confinement scales inversely with the gap. Controlling both the distance among the defects and the applied electric field, we can define fermionic models, even lattices, whose hoppings and Coulomb interactions can be tuned. We consider in detail the case of triangular and honeycomb artificial lattices and we show how, for a given arrangement of the sp$^3$ centers, these lattices can undergo an electrically controlled transition between the weak and strong coupling regimes.

We consider a hybrid structure formed by graphene and an insulating antiferromagnet, separated by a dielectric of thickness up to $d\simeq 500 \,nm$. When uncoupled, both graphene and the antiferromagnetic surface host their own polariton modes coupling the electromagnetic field with plasmons in the case of graphene, and with magnons in the case of the antiferromagnet. We show that the hybrid structure can host two new types of hybrid polariton modes. First, a surface magnon-plasmon polariton whose dispersion is radically changed by the carrier density of the graphene layer, including a change of sign in the group velocity. Second, a surface plasmon-magnon polariton formed as a linear superposition of graphene surface plasmon and the antiferromagnetic bare magnon. This polariton has a dispersion with two branches, formed by the anticrossing between the dispersive surface plasmon and the magnon. We discuss the potential these new modes have for combining photons, magnons, and plasmons to reach new functionalities., Comment: 12 pages, 4 figures

We study the optical properties of semiconducting transition metal dichalcogenide monolayers under the influence of strong out-of-plane magnetic fields, using the effective massive Dirac model. We pay attention to the role of spin-orbit coupling effects, doping level and electron-electron interactions, treated at the Hartree-Fock level. We find that optically-induced valley and spin imbalance, commonly attained with circularly polarized light, can also be obtained with linearly polarized light in the doped regime. Additionally, we explore an exchange-driven mechanism to enhance the spin-orbit splitting of the conduction band, in n-doped systems, controlling both the carrier density and the intensity of the applied magnetic field., Comment: 20 pages, 7 figures

We consider spin relaxation of finite-size spin chains exchanged coupled with a one dimensional (1D) electron gas at the edge of a Quantum Spin Hall (QSH) insulator. Spin lifetimes can be enhanced due to two independent mechanisms. First, the suppression of spin-flip forward scattering inherent in the spin momentum locking of the QSH edges. Second, the reduction of spin-flip backward scattering due to destructive interference of the quasiparticle exchange, modulated by $k_F d$, where $d$ is the inter-spin distance and $k_F$ is the Fermi wavenumber of the electron gas. We show that the spin lifetime of the $S=1/2$ ground state of odd-numbered chains of antiferromagnetically (AFM) coupled $S=1/2$ spins can be increased more than 4 orders of magnitude by properly tuning the product $k_Fd$ and the spin size $N$, in strong contrast with the 1D case. Possible physical realizations together with some potential issues are also discussed., Comment: 11 pages, 3 figures

We systematically investigate the relationships between structural and electronic effects of finite size zigzag or armchair carbon nanotubes of various diameters and lengths, starting from a molecular template of varying shape and diameter, i.e. cyclic oligoacene or oligophenacene molecules, and disclosing how adding layers and/or end-caps (i.e. hemi-fullerenes) can modify their (poly)radicaloid nature. We mostly used tight-binding and finite-temperature density-based methods, the former providing a simple but intuitive picture about their electronic structure, and the latter dealing effectively with strong correlation effects by relying on a fractional occupation number weighted electron density (\rho FOD ), with additional RAS-SF calculations backing up the latter results. We also explore how minor structural modifications of nanotube end-caps might influence the results, showing that topology, together with the chemical nature of the systems, is pivotal for the understanding of the electronic properties of these and other related systems.

A scanning tunneling microscope is used to explore the evolution of electron and Cooper pair transport across single Mn-phthalocyanine molecules adsorbed on Pb(111) from tunneling to contact ranges. Normal-metal as well as superconducting tips give rise to a gradual transition of the Bardeen-Cooper-Schrieffer energy gap in the tunneling range into a zero-energy resonance close to and at contact. Supporting transport calculations show that in the normal-metal - superconductor junctions this resonance reflects the merging of in-gap Yu-Shiba-Rusinov states as well as the onset of Andreev reflection. For the superconductor - superconductor contacts the zero-energy resonance is rationalized in terms of a finite Josephson current that is carried by phase-dependent Andreev and Yu-Shiba-Rusinov levels.

We address the interplay between stacking and interlayer exchange for ferromagnetically ordered CrI$_3$, both for bilayers and bulk. Whereas bulk CrI$_3$ is ferromagnetic, both magneto-optical and transport experiments show that interlayer exchange for CrI$_3$ bilayers is antiferromagnetic. Bulk CrI$_3$ is known to assume two crystal structures, rhombohedral and monoclinic, that differ mostly in the stacking between monolayers. Below 210-220 Kelvin, bulk CrI$_3$ orders in a rhombohedral phase. Our density functional theory calculations show a very strong dependence of interlayer exchange and stacking. Specifically, the ground states of both bulk and free-standing CrI$_3$ bilayers are ferromagnetic for the rhombohedral phase. In contrast, the energy difference between both configurations is more than one order of magnitude smaller for the monoclinic phase, and eventually becomes antiferromagnetic when either positive strain or on-site Hubbard interactions ($U \geq 3$) are considered. We also explore the interplay between interlayer hybrydization and stacking, using a Wannier basis, and between interlayer hybrydization and relative magnetic alignment for CrI$_3$ bilayers, that helps to account for the very large tunnel magnetoresistance obvserved in recent experiments., Comment: 5 pages, 3 figures. New version of the manuscript

We propose spin valves where a 2D non-magnetic conductor is intercalated between two ferromagnetic insulating layers. In this setup, the relative orientation of the magnetizations of the insulating layers can have a strong impact on the in-plane conductivity of the 2D conductor. We first show this for a graphene bilayer, described with a tight-binding model, placed between two ferromagnetic insulators. In the anti-parallel configuration, a band gap opens at the Dirac point, whereas in the parallel configuration, the graphene bilayer remains conducting. We then compute the electronic structure of graphene bilayer placed between two monolayers of the ferromagnetic insulator CrI$_3$, using density functional theory. Consistent with the model, we find that a gap opens at the Dirac point only in the antiparallel configuration., Comment: 5 pages, 4 figures

Topological invariants allow to characterize Hamiltonians, predicting the existence of topologically protected in-gap modes. Those invariants can be computed by tracing the evolution of the occupied wavefunctions under twisted boundary conditions. However, those procedures do not allow to calculate a topological invariant by evaluating the system locally, and thus require information about the wavefunctions in the whole system. Here we show that artificial neural networks can be trained to identify the topological order by evaluating a local projection of the density matrix. We demonstrate this for two different models, a 1-D topological superconductor and a 2-D quantum anomalous Hall state, both with spatially modulated parameters. Our neural network correctly identifies the different topological domains in real space, predicting the location of in-gap states. By combining a neural network with a calculation of the electronic states that uses the Kernel Polynomial Method, we show that the local evaluation of the invariant can be carried out by evaluating a local quantity, in particular for systems without translational symmetry consisting of tens of thousands of atoms. Our results show that supervised learning is an efficient methodology to characterize the local topology of a system., Comment: 9 pages, 6 figures

We propose a mechanism to drive singlet-triplet spin transitions electrically, in a wide class of graphene nanostructures that present pairs of in-gap zero modes, localized at opposite sublattices. Examples are rectangular nanographenes with short zigzag edges, armchair ribbon heterojunctions with topological in-gap states and graphene islands with sp$^3$ functionalization. The interplay between the hybridization of zero modes and Coulomb repulsion leads to symmetric exchange interaction that favors a singlet ground state. Application of an off-plane electric field to the graphene nanostructure generates an additional Rashba spin-orbit coupling, which results in antisymmetric exchange interaction that mixes $S=0$ and $S=1$ manifolds. We show that modulation in time of either the off-plane electric field or the applied magnetic field permits to perform electrically driven spin resonance in a system with very long spin relaxation times.

The observation of ferromagnetic order in a monolayer of CrI$_3$ has been recently reported, with a Curie temperature of 45 Kelvin and off-plane easy axis. Here we study the origin of magnetic anisotropy, a necessary ingredient to have magnetic order in two dimensions, combining two levels of modeling, density functional calculations and spin model Hamiltonians. We find two different contributions to the magnetic anisotropy of the material, both favoring off-plane magnetization and contributing to open a gap in the spin wave spectrum. First, ferromagnetic super-exchange across the $\simeq $ 90 degree Cr-I-Cr bonds, are anisotropic, due to the spin orbit interaction of the ligand I atoms. Second, a much smaller contribution that comes from the single ion anisotropy of the $S=3/2$ Cr atom. Our results permit to establish the XXZ Hamiltonian, with a very small single ion anisotropy, as the adequate spin model for this system. Using spin wave theory we estimate the Curie temperature and we highlight the essential role played by the gap that magnetic anisotropy induces on the magnon spectrum., Comment: 8 pages, 5 figures