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We use the topological heavy fermion (THF) model and its Kondo Lattice (KL) formulation to study the symmetric Kondo state in twisted bilayer graphene. Via a large-N approximation, we find a symmetric Kondo (SK) state in KL mode at fillings $\nu=0,\pm 1,\pm 2$. In the SK state, all symmetries are preserved and the local moments are Kondo screened by the conduction electrons. At the mean-field level of the THF model at $\nu=0,\pm 1, \pm 2, \pm 3$, we also find a similar symmetric state. We study the stability of the symmetric state by comparing its energy with the ordered states and find the ordered states to have lower energy. However, moving away from integer fillings by doping holes to the light bands, we find the energy difference is reduced, which suggests the loss of ordering and a tendency towards Kondo screening. In order to include many-body effects beyond the mean-field approximation, we perform dynamical mean-field theory (DMFT) calculations on the THF model. We find the spin susceptibility follows a Curie behavior at $\nu=0, \pm 1,\pm 2$ down to $\sim 2\text{K}$ where the onset of screening of the local moment becomes visible. This hints to very low Kondo temperatures at these fillings, in agreement with the outcome of our mean-field calculations. At non-integer filling $\nu=\pm 0.5,\pm 0.8,\pm 1.2$ DMFT shows deviations from a $1/T$-susceptibility at much higher temperatures, suggesting a more effective screening of local moments with doping. Finally, we study the effect of a $C_{3z}$-rotational-symmetry-breaking strain via mean-field approaches and find that a symmetric phase (that only breaks $C_{3z}$ symmetry) can be stabilized at sufficiently large strain at $\nu=0,\pm 1, \pm 2$. Our results suggest that a symmetric Kondo phase is strongly suppressed at integer fillings, but could be stabilized either at non-integer fillings or by applying strain., Comment: 40 pages, 15 figures

Exotic ordered ground states driven by electronic correlations are expected to be induced in monolayer graphene when doped to the Van Hove singularity. Such doping levels are reached by intercalating Gd in graphene on SiC(0001), resulting in a strong homogeneity and stability. The electronic spectrum now exhibits severe renormalizations. Flat bands develop which is driven by electronic correlations according to our theoretical studies. Due to strong electron-phonon coupling in this regime, polaron replica bands develop. Thus, interesting ordered ground states should be made accessible.

Magic-angle twisted bilayer graphene (MA-tBLG) has appeared as a tunable testing ground to investigate the conspiracy of electronic interactions, band structure, and lattice degrees of freedom to yield exotic quantum many-body ground states in a two-dimensional Dirac material framework. While the impact of external parameters such as doping or magnetic field can be conveniently modified and analyzed, the all-surface nature of the quasi-2D electron gas combined with its intricate internal properties pose a challenging task to characterize the quintessential nature of the different insulating and superconducting states found in experiments. We analyze the interplay of internal screening and dielectric environment on the intrinsic electronic interaction profile of MA-tBLG. We find that interlayer coupling generically enhances the internal screening. The influence of the dielectric environment on the effective interaction strength depends decisively on the electronic state of MA-tBLG. Thus, we propose the experimental tailoring of the dielectric environment, e.g. by varying the capping layer composition and thickness, as a promising pursuit to provide further evidence for resolving the hidden nature of the quantum many-body states in MA-tBLG., Comment: 9 pages, 3 figures, supplemental material included (8 figures)

In contrast to the Hubbard model, the extended Hubbard model, which additionally accounts for non-local interactions, lacks systemic studies of thermodynamic properties especially across the metal-insulator transition. Using a variational principle, we perform such a systematic study and describe how non-local interactions screen local correlations differently in the Fermi-liquid and in the insulator. The thermodynamics reveal that non-local interactions are at least in parts responsible for first-order metal-insulator transitions in real materials., Comment: 19 pages, 9 figures. Resubmission to SciPost

Monolayers of transition metal dichalcogenides (TMDCs) exhibit an exceptionally strong Coulomb interaction between charge carriers due to the two-dimensional carrier confinement in connection with weak dielectric screening. High densities of excited charge carriers in the various band-structure valleys cause strong many-body renormalizations that influence both the electronic properties and the optical response of the material. We investigate electronic and optical properties of the typical monolayer TMDCs MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$ in the presence of excited carriers by solving semiconductor Bloch equations on the full Brillouin zone. With increasing carrier density, we systematically find a reduction of the exciton binding energies due to Coulomb screening and Pauli blocking. Together with excitation-induced band-gap shrinkage this leads to redshifts of excitonic resonances up to the dissociation of excitons. As a central result, we predict for all investigated monolayer TMDCs that the $\Sigma$-valley shifts stronger than the K-valley. Two of the materials undergo a transition from direct to indirect band gaps under carrier excitation similar to well-known strain-induced effects. Our findings have strong implications for the filling of conduction-band valleys with excited carriers and are relevant to transport and optical applications as well as the emergence of phonon-driven superconductivity.

Using ab-initio calculations we reveal the nature of the insulating phase recently found experimentally in monolayer 1T-NbSe$_2$. We find soft phonon modes in a large parts of the Brillouin zone indicating the strong-coupling nature of a charge-density-wave instability. Structural relaxation of a $\sqrt{13}\times\sqrt{13}$ supercell reveals a Star-of-David reconstruction with an energy gain of 60 meV per primitive unit cell. The band structure of the distorted phase exhibits a half-filled flat band which is associated with orbitals that are delocalized over several atoms in each Star of David. By including many-body corrections through a combined GW, hybrid-functional, and DMFT treatment, we find the flat band to split into narrow Hubbard bands. The lowest energy excitation across the gap turns out to be between itinerant Se-$p$ states and the upper Hubbard band, determining the system to be a charge-transfer insulator. Combined hybrid-functional and GW calculations show that long-range interactions shift the Se-$p$ states to lower energies. Thus, a delicate interplay of local and long-range correlations determines the gap nature and its size in this distorted phase of the monolayer 1T-NbSe$_2$., Comment: 10 pages, 11 figures

Atomically thin layers of transition metal dichalcogenides (TMDCs) exhibit exceptionally strong Coulomb interaction between charge carriers due to the two-dimensional carrier confinement in connection with weak dielectric screening. The van der Waals nature of interlayer coupling makes it easy to integrate TMDC layers into heterostructures with different dielectric or metallic substrates. This allows to tailor electronic and optical properties of these materials, as Coulomb interaction inside atomically thin layers is very susceptible to screening by the environment. Here we theoretically investigate dynamical screening effects in TMDCs due to bulk substrates doped with carriers over a large density range, thereby offering three-dimensional plasmons as tunable degree of freedom. We report a wide compensation of renormalization effects leading to a spectrally more stable exciton than predicted for static substrate screening, even if plasmons and excitons are in resonance. We also find a nontrivial dependence of the single-particle band gap on substrate doping density due to dynamical screening. Our investigation provides microscopic insight into the mechanisms that allow for manipulations of TMDC excitons by means of arbitrary plasmonic environments on the nanoscale.

Plasmonic excitations behave fundamentally different in layered materials in comparison to bulk systems. They form gapless modes, which in turn couple at low energies to the electrons. Thereby they can strongly influence superconducting instabilities. Here, we show how these excitations can be controlled from the outside via changes in the dielectric environment or in the doping level, which allows for external tuning of the superconducting transition temperature. By solving the gap equation for an effective system, we find that the plasmonic influence can both strongly enhance or reduce the transition temperature, depending on the details of the plasmon-phonon interplay. We formulate simple experimental guidelines to find plasmon- induced elevated transition temperatures in layered materials., Comment: 13 pages, 10 figures

The electronic and optical properties of monolayer transition-metal dichalcogenides (TMDs) and van der Waals heterostructures are strongly subject to their dielectric environment. In each layer the field lines of the Coulomb interaction are screened by the adjacent material, which reduces the single-particle band gap as well as exciton and trion binding energies. By combining an electrostatic model for a dielectric hetero-multi-layered environment with semiconductor many-particle methods, we demonstrate that the electronic and optical properties are sensitive to the interlayer distances on the atomic scale. Spectroscopical measurements in combination with a direct solution of a three-particle Schr\"odinger equation reveal trion binding energies that correctly predict recently measured interlayer distances.

Nanostructures with open shell transition metal or molecular constituents host often strong electronic correlations and are highly sensitive to atomistic material details. This tutorial review discusses method developments and applications of theoretical approaches for the realistic description of the electronic and magnetic properties of nanostructures with correlated electrons. First, the implementation of a flexible interface between density functional theory and a variant of dynamical mean field theory (DMFT) highly suitable for the simulation of complex correlated structures is explained and illustrated. On the DMFT side, this interface is largely based on recent developments of quantum Monte Carlo and exact diagonalization techniques allowing for efficient descriptions of general four fermion Coulomb interactions, reduced symmetries and spin-orbit coupling, which are explained here. With the examples of the Cr (001) surfaces, magnetic adatoms, and molecular systems it is shown how the interplay of Hubbard U and Hund's J determines charge and spin fluctuations and how these interactions drive different sorts of correlation effects in nanosystems. Non-local interactions and correlations present a particular challenge for the theory of low dimensional systems. We present our method developments addressing these two challenges, i.e., advancements of the dynamical vertex approximation and a combination of the constrained random phase approximation with continuum medium theories. We demonstrate how non-local interaction and correlation phenomena are controlled not only by dimensionality but also by coupling to the environment which is typically important for determining the physics of nanosystems., Comment: tutorial review submitted to EPJ-ST (scientific report of research unit FOR 1346); 14 figures, 26 pages

The interplay of Coulomb and electron-phonon interactions with thermal and quantum fluctuations facilitates rich phase diagrams in two-dimensional electron systems. Layered transition metal dichalcogenides hosting charge, excitonic, spin and superconducting order form an epitomic material class in this respect. Theoretical studies of materials like NbS$_2$ have focused on the electron-phonon coupling whereas the Coulomb interaction, particularly strong in the monolayer limit, remained essentially untouched. Here, we analyze the interplay of short- and long-range Coulomb as well as electron-phonon interactions in NbS$_2$ monolayers. The combination of these interactions causes electronic correlations that are fundamentally different to what would be expected from the interaction terms separately. The fully interacting electronic spectral function resembles the non-interacting band structure but with appreciable broadening. An unexpected coexistence of strong charge and spin fluctuations puts NbS$_2$ close to spin and charge order, suggesting monolayer NbS$_2$ as a platform for atomic scale engineering of electronic quantum phases.

While the Hubbard model is the standard model to study Mott metal-insulator transitions, it is still unclear to which extent it can describe metal-insulator transitions in real solids, where non-local Coulomb interactions are always present. By using a variational principle, we clarify this issue for short- and long-ranged non-local Coulomb interactions for half-filled systems on bipartite lattices. We find that repulsive non-local interactions generally stabilize the Fermi-liquid regime. The metal-insulator phase boundary is shifted to larger interaction strengths to leading order linearly with non-local interactions. Importantly, non-local interactions can raise the order of the metal-insulator transition. We present a detailed analysis of how the dimension and geometry of the lattice as well as the temperature determine the critical non-local interaction leading to a first-order transition: for systems in more than two dimensions with non-zero density of states at the Fermi energy the critical non-local interaction is arbitrarily small; otherwise it is finite., Comment: 10 pages, 11 figures

The role of defects in van der Waals heterostructures made of graphene and hexagonal boron nitride (h-BN) is studied by a combination of ab initio and model calculations. Despite the weak van der Waals interaction between layers, defects residing in h-BN, such as carbon impurities and antisite defects, reveal a hybridization with graphene p$_{\rm z}$ states, leading to midgap state formation. The induced midgap states modify the transport properties of graphene and can be reproduced by means of a simple effective tight-binding model. In contrast to carbon defects, it is found that oxygen defects do not strongly hybridize with graphene's low-energy states. Instead, oxygen drastically modifies the band gap of graphene, which emerges in a commensurate stacking on h-BN lattices., Comment: 5 pages, 4 figures

We demonstrate how weak hybridization can lead to apparent heavy doping of 2d materials even in case of physisorptive binding. Combining ab-intio calculations and a generic model we show that strong reshaping of Fermi surfaces and changes in Fermi volumes on the order of several 10$\%$ can arise without actual charge transfer. This pseudodoping mechanism is very generically effective in metallic 2d materials either weakly absored to metallic substrates or embedded in vertical heterostructures. It can explain strong apparent doping of TaS2 on Au (111) observed in recent experiments. Consequences of pseudodoping for many-body instabilities are discussed., Comment: 5 pages, 2 figures

We investigate the Peierls-Feynman-Bogoliubov variational principle to map Hubbard models with nonlocal interactions to effective models with only local interactions. We study the renormalization of the local interaction induced by nearest-neighbor interaction and assess the quality of the effective Hubbard models in reproducing observables of the corresponding extended Hubbard models. We compare the renormalization of the local interactions as obtained from numerically exact determinant Quantum Monte Carlo to approximate but more generally applicable calculations using dual boson, dynamical mean field theory, and the random phase approximation. These more approximate approaches are crucial for any application with real materials in mind. Furthermore, we use the dual boson method to calculate observables of the extended Hubbard models directly and benchmark these against determinant Quantum Monte Carlo simulations of the effective Hubbard model., Comment: 12 pages, 10 figures

A quantitative description of Coulomb interactions is developed for two-dimensional superconducting materials, enabling us to compare intrinsic with external screening effects, such as those due to substrates. Using the example of a doped monolayer of MoS2 embedded in a tunable dielectric environment, we demonstrate that the influence of external screening is limited to a length scale, bounded from below by the effective thickness of the quasi-two-dimensional material and from above by its intrinsic screening length. As a consequence, it is found that unconventional Coulomb-driven superconductivity cannot be induced in MoS2 by tuning the substrate properties alone. Our calculations of the retarded Morel-Anderson Coulomb potential {\mu *} reveal that the Coulomb interactions, renormalized by the reduced layer thickness and the substrate properties, can shift the onset of the electron-phonon driven superconducting phase in monolayer MoS2 but do not significantly affect the critical temperature at optimal doping., Comment: 8 pages, 5 figures

The recently proposed theoretical concept of a Hund's metal is regarded as a key to explain the exotic magnetic and electronic behavior occuring in the strongly correlated electron systems of multiorbital metallic materials. However, a tuning of the abundance of parameters, that determine these systems, is experimentally challenging. Here, we investigate the smallest possible realization of a Hund's metal, a Hund's impurity, realized by a single magnetic impurity strongly hybridized to a metallic substrate. We experimentally control all relevant parameters including magnetic anisotropy and hybridization by hydrogenation with the tip of a scanning tunneling microscope and thereby tune it through a regime from emergent magnetic moments into a multi-orbital Kondo state. Our comparison of the measured temperature and magnetic field dependent spectral functions to advanced many-body theories will give relevant input for their application to non-Fermi liquid transport, complex magnetic order, or unconventional superconductivity.

We report on the quenching of single Ni adatom moments on Te-terminated Bi2Te2Se and Bi2Te3 topological insulator surfaces. The effect becomes manifested as a missing X-ray magnetic circular dichroism for resonant L3,2 transitions into partially filled Ni 3d states of occupancy n_d = 9.2. On the basis of a comparative study of Ni and Fe using scanning tunneling microscopy and ab initio calculations we are able to relate the element specific moment formation to a local Stoner criterion. While Fe adatoms form large spin moments of m_s = 2.54 mu_B with out-of-plane anisotropy due to a sufficiently large density of states at the Fermi energy, Ni remains well below an effective Stoner threshold for local moment formation. With the Fermi level remaining in the bulk band gap after adatom deposition, non-magnetic Ni and preferentially out-of-plane oriented magnetic Fe with similar structural properties on Bi2Te2Se surfaces constitute a perfect platform to study off-on effects of time-reversal symmetry breaking on topological surface states.

The rich phenomenology of plasmonic excitations in the dichalcogenides is analyzed as a function of doping. The many-body polarization, the dielectric response function and electron energy loss spectra are calculated using an ab initio based model involving material-realistic Coulomb interactions, band structure and spin-orbit coupling. Focusing on the representative case of MoS$_2$, a plethora of plasmon bands are observed, originating from scattering processes within and between the conduction or valence band valleys. We discuss the resulting square-root and linear collective modes, arising from long-range versus short-range screening of the Coulomb potential. We show that the multi-orbital nature of the bands and spin-orbit coupling strongly affects inter-valley scattering processes by gapping certain two-particle modes at large momentum transfer.

The electronic structure of the Cr(001) surface with its sharp resonance at the Fermi level is a subject of controversial debate of many experimental and theoretical works. To date, it is unclear whether the origin of this resonance is an orbital Kondo or an electron-phonon coupling effect. We have combined ab initio density functional calculations with dynamical mean-field simulations to calculate the orbitally resolved spectral function of the Cr(001) surface. The calculated orbital character and shape of the spectrum is in agreement with data from (inverse) photoemission experiments. We find that dynamic electron correlations crucially influence the surface electronic structure and lead to a low energy resonance in the $d_{z^2}$ and $d_{xz/yz}$ orbitals. Our results help to reconvene controversial experimental results from (I)PES and STM measurements., Comment: 8 pages, 5 figures

We introduce an approach to derive realistic Coulomb interaction terms in free standing layered materials and vertical heterostructures from ab-initio modelling of the corresponding bulk materials. To this end, we establish a combination of calculations within the framework of the constrained random phase approximation, Wannier function representation of Coulomb matrix elements within some low energy Hilbert space and continuum medium electrostatics, which we call Wannier function continuum electrostatics (WFCE). For monolayer and bilayer graphene we reproduce full ab-initio calculations of the Coulomb matrix elements within an accuracy of $0.2$eV or better. We show that realistic Coulomb interactions in bilayer graphene can be manipulated on the eV scale by different dielectric and metallic environments. A comparison to electronic phase diagrams derived in [M. M. Scherer et al., Phys. Rev. B 85, 235408 (2012)] suggests that the electronic ground state of bilayer graphene is a layered antiferromagnet and remains surprisingly unaffected by these strong changes in the Coulomb interaction., Comment: 12 pages, 8 figures

We describe a variational approach to solving Anderson impurity models by means of exact diagonalization. Optimized parameters of a discretized auxiliary model are obtained on the basis of the Peierls-Feynman-Bogoliubov principle. Thereby, the variational approach resolves ambiguities related with the bath discretization, which is generally necessary to make Anderson impurity models tractable by exact diagonalization. The choice of variational degrees of freedom made here allows systematic improvements of total energies over mean field decouplings like Hartree-Fock. Furthermore, our approach allows us to embed arbitrary bath discretization schemes in total energy calculations and to systematically optimize and improve on traditional routes to the discretization problem such as fitting of hybridization functions on Matsubara frequencies. Benchmarks in terms of a single orbital Anderson model demonstrate that the variational exact diagonalization method accurately reproduces free energies as well as several single- and two-particle observables obtained from an exact solution. Finally, we demonstrate the applicability of the variational exact diagonalization approach to realistic five orbital problems with the example system of Co impurities in bulk Cu and compare to continuous-time Monte Carlo calculations. The accuracy of established bath discretization schemes is assessed in the framework of the variational approach introduced here., Comment: 10 pages, 4 figures, accepted in PRB, v2: Added section on spectral information

Ultrafast magnetization dynamics in metallic heterostructures consists of a combination of local demagnetization in the ferromagnetic constituent and spin-dependent transport contributions within and in between the constituents. Separation of these local and non-local contributions is essential to obtain microscopic understanding and for potential applications of the underlying microscopic processes. By comparing the ultrafast changes of the polarization rotation and ellipticity in the magneto-optical Kerr effect (MOKE) we observe a time-dependent magnetization profile M(z,t) in Co/Cu(001) films by exploiting the effective depth sensitivity of the method. By analyzing the spatio-temporal correlation of these profiles we find that on time scales before hot electron thermalization (<100 fs) the transient magnetization of Co films is governed by spin-dependent transport effects, while after hot electron thermalization (>200 fs) local spin-flip processes dominate., Comment: 9 pages, 6 figures; revised version (title/abstract changed, text/figures from former ancillary file now included in main text, one additional figure, slightly expanded discussion); conclusions remain the same as in previous version

Valley polarization in graphene breaks inversion symmetry and therefore leads to second-harmonic generation. We present a complete theory of this effect within a single-particle approximation. It is shown that this may be a sensitive tool to measure the valley polarization created, e.g., by polarized light and, thus, can be used for a development of ultrafast valleytronics in graphene., Comment: 5 pages, 3 figures

A wide range of materials, like d-wave superconductors, graphene, and topological insulators, share a fundamental similarity: their low-energy fermionic excitations behave as massless Dirac particles rather than fermions obeying the usual Schrodinger Hamiltonian. This emergent behavior of Dirac fermions in condensed matter systems defines the unifying framework for a class of materials we call "Dirac materials''. In order to establish this class of materials, we illustrate how Dirac fermions emerge in multiple entirely different condensed matter systems and we discuss how Dirac fermions have been identified experimentally using electron spectroscopy techniques (angle-resolved photoemission spectroscopy and scanning tunneling spectroscopy). As a consequence of their common low-energy excitations, this diverse set of materials shares a significant number of universal properties in the low-energy (infrared) limit. We review these common properties including nodal points in the excitation spectrum, density of states, specific heat, transport, thermodynamic properties, impurity resonances, and magnetic field responses, as well as discuss many-body interaction effects. We further review how the emergence of Dirac excitations is controlled by specific symmetries of the material, such as time-reversal, gauge, and spin-orbit symmetries, and how by breaking these symmetries a finite Dirac mass is generated. We give examples of how the interaction of Dirac fermions with their distinct real material background leads to rich novel physics with common fingerprints such as the suppression of back scattering and impurity-induced resonant states., Comment: Review article accepted in Adv. Phys. 77 pages

Using first principle calculations, we examine the sequence of phases in electron doped dichalcogenides, such as recently realized in field-gated MoS$_2$. Upon increasing the electron doping level, we observe a succession of semiconducting, metallic, superconducting and charge density wave regimes, i.e. in different order compared to the phase diagram of (semi-)metallic dichalcogenides such as TiSe$_2$. Both instabilities trace back to a softening of phonons which couple the electron populated conduction band minima. The superconducting dome, calculated using Eliashberg theory, is found to fit the experimentally observed phase diagram, obtained from resistivity measurements. The charge density wave phase at higher electron doping concentrations as predicted from instabilities in the phonon modes is further corroborated by detecting the accompanying lattice deformation in density functional based supercell relaxations. Upon charge density wave formation, doped MoS$_2$ remains metallic but undergoes a Lifschitz transition, where the number of Fermi pockets is reduced., Comment: 5 pages, 4 figures

The successful isolation of graphene ten years ago has evoked a rapidly growing scientific interest in the nature of two-dimensional (2D) crystals. A number of different 2D crystals has been produced since then, with properties ranging from superconductivity to insulating behavior. Here, we predict the possibility for realizing ferromagnetic 2D crystals by exfoliating atomically thin films of K2CuF4. From a first-principles theoretical analysis, we find that single layers of K2CuF4 form exactly 2D Kosterlitz-Thouless systems. The 2D crystal can form a free-standing membrane, and exhibits an experimentally accessible transition temperature and robust magnetic moments of 1 Bohr magneton per formula unit. 2D K2CuF4 unites ferromagnetic and insulating properties and is a demonstration of principles for nanoelectronics such as novel 2D-based heterostructures., Comment: 8 pages, 6 figures (supplementary information included)

We investigate the electronic and magnetic properties of single Fe, Co, and Ni atoms and clusters on monolayer graphene (MLG) on SiC(0001) by means of scanning tunneling microscopy (STM), x-ray absorption spectroscopy, x-ray magnetic circular dichroism (XMCD), and ab initio calculations. STM reveals different adsorption sites for Ni and Co adatoms. XMCD proves Fe and Co adatoms to be paramagnetic and to exhibit an out-of-plane easy axis in agreement with theory. In contrast, we experimentally find a nonmagnetic ground state for Ni monomers while an increasing cluster size leads to sizeable magnetic moments. These observations are well reproduced by our calculations and reveal the importance of hybridization effects and intra-atomic charge transfer for the properties of adatoms and clusters on MLG., Comment: 8 pages (supplementary included), 4 figures, (supplementary included)

We present a joint theoretical and experimental investigation of charge doping and electronic potential landscapes in hybrid structures composed of graphene and semiconducting single layer MoS2. From first-principles simulations we find electron doping of graphene due to the presence of rhenium impurities in MoS2. Furthermore, we show that MoS2 edges give rise to charge reordering and a potential shift in graphene, which can be controlled through external gate voltages. The interplay of edge and impurity effects allows the use of the graphene-MoS2 hybrid as a photodetector. Spatially resolved photocurrent signals can be used to resolve potential gradients and local doping levels in the sample., Comment: 11 pages, 7 figures

To understand how nonlocal Coulomb interactions affect the phase diagram of correlated electron materials, we report on a method to approximate a correlated lattice model with nonlocal interactions by an effective Hubbard model with on-site interactions U* only. The effective model is defined by the Peierls-Feynman-Bogoliubov variational principle. We find that the local part of the interaction U is reduced according to U*=U-V', where V' is a weighted average of nonlocal interactions. For graphene, silicene and benzene we show that the nonlocal Coulomb interaction can decrease the effective local interaction by more than a factor of 2 in a wide doping range., Comment: Accepted for publication in PRL. Supplemental material added in this version

We investigate the effect of spin-orbit coupling on the behavior of magnetic impurity at the edge of a zigzag graphene ribbon by means of quantum Monte Carlo simulations. A peculiar interplay of Kane-Mele type spin-orbit and impurity-host coupling is found to affect local properties such as the impurity magnetic moment and spectral densities. The special helical nature of the topological insulator on the edge is found to affect nonlocal quantities, such as the two-particle and spin-spin correlation functions linking electrons on the impurity with those in the conduction band., Comment: 12 figures. And a shorter version will be published in PRB

We report photoemission experiments revealing the valence electron spectral function of Mn, Fe, Co and Ni atoms on the Ag(100) surface. The series of spectra shows splittings of higher energy features which decrease with the filling of the 3d shell and a highly non-monotonous evolution of spectral weight near the Fermi edge. First principles calculations demonstrate that two manifestations of Hund's exchange $J$ are responsible for this evolution. First, there is a monotonous reduction of the effective exchange splittings with increasing filling of the 3d shell. Second, the amount of charge fluctuations and, thus, the weight of quasiparticle peaks at the Fermi level varies non-monotonously through this 3d series due to a distinct occupancy dependence of effective charging energies $U_{\rm eff}$., Comment: 5 pages, 3 figures

A combined experimental and theoretical study of doping individual Fe atoms into Bi2Se3 is presented. It is shown through a scanning tunneling microscopy study that single Fe atoms initially located at hollow sites on top of the surface (adatoms) can be incorporated into subsurface layers by thermally-activated diffusion. Angle-resolved photoemission spectroscopy in combination with ab-initio calculations suggest that the doping behavior changes from electron donation for the Fe adatom to neutral or electron acceptance for Fe incorporated into substitutional Bi sites. According to first principles calculations within density functional theory, these Fe substitutional impurities retain a large magnetic moment thus presenting an alternative scheme for magnetically doping the topological surface state. For both types of Fe doping, we see no indication of a gap at the Dirac point., Comment: 5 pages, 4 figures

Resonant scatterers such as hydrogen adatoms can strongly enhance the low energy density of states in graphene. Here, we study the impact of these impurities on the electronic screening. We find a two-faced behavior: Kubo formula calculations reveal an increased dielectric function $\varepsilon$ upon creation of midgap states but no metallic divergence of the static $\varepsilon$ at small momentum transfer $q\to 0$. This bad metal behavior manifests also in the dynamic polarization function and can be directly measured by means of electron energy loss spectroscopy. A new length scale $l_c$ beyond which screening is suppressed emerges, which we identify with the Anderson localization length., Comment: 5 pages, 4 figures

The influence of graphene islands on the electronic structure of the Ir(111) surface is investigated. Scanning tunneling spectroscopy (STS) indicates the presence of a two-dimensional electron gas with a binding energy of -160meV and an effective mass of -0.18m_e underneath single-layer graphene on the Ir(111) surface. Density functional calculations reveal that the STS features are predominantly due to a holelike surface resonance of the Ir(111) substrate. Nanometer-sized graphene islands act as local gates, which shift and confine the surface resonance., Comment: Accepted by Physical Review Letters, Feb 17, 2012

The robustness of the gapless topological surface state hosted by a 3D topological insulator against perturbations of magnetic origin has been the focus of recent investigations. We present a comprehensive study of the magnetic properties of Fe impurities on a prototypical 3D topological insulator Bi$_2$Se$_3$ using local low temperature scanning tunneling microscopy and integral x-ray magnetic circular dichroism techniques. Single Fe adatoms on the Bi$_2$Se$_3$ surface, in the coverage range $\approx 1%$ are heavily relaxed into the surface and exhibit a magnetic easy axis within the surface-plane, contrary to what was assumed in recent investigations on the opening of a gap. Using \textit{ab initio} approaches, we demonstrate that an in-plane easy axis arises from the combination of the crystal field and dynamic hybridization effects., Comment: 5 pages, 3 figures, typos corrected

We have investigated the magnetism of the bare and graphene-covered (111) surface of a Ni single crystal employing three different magnetic imaging techniques and ab initio calculations, covering length scales from the nanometer regime up to several millimeters. With low temperature spinpolarized scanning tunneling microscopy (SP-STM) we find domain walls with widths of 60 - 90 nm, which can be moved by small perpendicular magnetic fields. Spin contrast is also achieved on the graphene-covered surface, which means that the electron density in the vacuum above graphene is substantially spin-polarized. In accordance with our ab initio calculations we find an enhanced atomic corrugation with respect to the bare surface, due to the presence of the carbon pz orbitals and as a result of the quenching of Ni surface states. The latter also leads to an inversion of spinpolarization with respect to the pristine surface. Room temperature Kerr microscopy shows a stripe like domain pattern with stripe widths of 3 - 6 {\mu}m. Applying in-plane-fields, domain walls start to move at about 13 mT and a single domain state is achieved at 140 mT. Via scanning electron microscopy with polarization analysis (SEMPA) a second type of modulation within the stripes is found and identified as 330 nm wide V-lines. Qualitatively, the observed surface domain pattern originates from bulk domains and their quasi-domain branching is driven by stray field reduction.

We address the interaction of graphene with 3d transition metal adatoms and the formation of localized magnetic moments by means of first-principles calculations. By comparing calculations within the generalized gradient approximation (GGA) to GGA+U we find that the electronic configuration and the adsorption geometries can be very sensitive to effects of local Coulomb interactions U in the transition metal d-orbitals. We find high-spin configurations being favorable for Cr and Mn adatoms independent of the functional. For Fe, Co and Ni different electronic configurations are realized depending on the value of the local Coulomb interaction strength U. Chemical control over the spin of the adatoms by hydrogenation is demonstrated: NiH and CoH adsorbed to graphene exhibit spin S=1/2 and S=1, respectively.

Linear CoCu_nCo clusters on Cu(111) are fabricated by means of atomic manipulation. They represent a two-site Kondo system with tunable interaction. Scanning tunneling spectroscopy reveals oscillations of the Kondo temperature T_K with the number n of Cu atoms for n>=3. Density functional calculations show that the Ruderman-Kittel-Kasuya-Yosida interaction mediated by the Cu chains causes the oscillations. Calculations find ferromagnetic and antiferromagnetic interaction for n=1 and 2, respectively. Both interactions lead to a decrease of T_K as experimentally observed., Comment: 5 pages, 3 figures

We investigate the adsorption of graphene sheets on h-BN substrates by means of first-principles calculations in the framework of adiabatic connection fluctuation-dissipation theory in the random phase approximation. We obtain adhesion energies for different crystallographic stacking configurations and show that the interlayer bonding is due to long-range van der Waals forces. The interplay of elastic and adhesion energies is shown to lead to stacking disorder and moir\'e structures. Band structure calculations reveal substrate induced mass terms in graphene which change their sign with the stacking configuration. The dispersion, absolute band gaps and the real space shape of the low energy electronic states in the moir\'e structures are discussed. We find that the absolute band gaps in the moir\'e structures are at least an order of magnitude smaller than the maximum local values of the mass term. Our results are in agreement with recent STM experiments., Comment: 8 pages, 8 figures, revised and extended version, to appear in Phys. Rev. B

We report photoemission experiments revealing the full valence electron spectral function of Ce adatoms on Ag(111), W(110) and Rh(111) surfaces. A transfer of Ce 4f spectral weight from the ionization peak towards the Fermi level is demonstrated upon changing the substrate from Ag(111) to Rh(111). In the intermediate case of Ce on W(110) the ionization peak is found to be split. This evolution of the spectra is explained by means of first-principles theory which clearly demonstrates that a reliable understanding of magnetic adatoms on metal surfaces requires simultaneous low and high energy spectroscopic information., Comment: 4 pages, 3 figures

To obtain an effective many-body model of graphene and related materials from first principles we calculate the partially screened frequency dependent Coulomb interaction. In graphene, the effective on-site (Hubbard) interaction is U_00 = 9.3 eV in close vicinity to the critical value separating conducting graphene from an insulating phase emphasizing the importance of non-local Coulomb terms. The nearest-neighbor Coulomb interaction strength is computed to U_01 = 5.5 eV. In the long wavelength limit, we find the effective background dielectric constant of graphite to be \epsilon = 2.5 in very good agreement with experiment., Comment: 4 pages, 3 figures (revised version)

The realistic description of correlated electron systems has taken an important step forward a few years ago as the combination of density functional methods and the dynamical mean-field theory was conceived. This framework allows access to both high and low energy physics and is capable of the description of the specific physics of strongly correlated materials, like the Mott metal-insulator transition. A very important step in the procedure is the interface between the band structure method and the dynamical mean-field theory and its impurity solver. We present a general interface between a projector augmented wave based density functional code and many-body methods based on Wannier functions obtained from a projection on local orbitals. The implementation is very flexible and allows for various applications. Quantities like the momentum resolved spectral function are accessible. We present applications to SrVO$_3$ and the metal-insulator transition in Ca$_{2-x}$Sr$_{x}$RuO$_4$.

An intrinsic issue of the LDA+DMFT approach is the so called double counting of interaction terms. How to choose the double-counting potential in a manner that is both physically sound and consistent is unknown. We have conducted an extensive study of the charge transfer system NiO in the LDA+DMFT framework using quantum Monte Carlo and exact diagonalization as impurity solvers. By explicitly treating the double-counting correction as an adjustable parameter we systematically investigated the effects of different choices for the double counting on the spectral function. Different methods for fixing the double counting can drive the result from Mott insulating to almost metallic. We propose a reasonable scheme for the determination of double-counting corrections for insulating systems., Comment: 7 pages, 6 figures

We develop a first-principles theory of resonant impurities in graphene and show that a broad range of typical realistic impurities leads to the characteristic sublinear dependence of the conductivity on the carrier concentration. By means of density functional calculations various organic groups as well as ad-atoms like H absorbed to graphene are shown to create midgap states within +-0.03eV around the neutrality point. A low energy tight-binding description is mapped out. Boltzmann transport theory as well as a numerically exact Kubo formula approach yield the conductivity of graphene contaminated with these realistic impurities in accordance with recent experiments., Comment: 4 pages, 4 figures

We study the origin of the temperature-induced Mott transition in Ca2RuO4. As a method we use the local-density approximation+dynamical mean-field theory. We show the following. (i) The Mott transition is driven by the change in structure from long to short c-axis layered perovskite (L-Pbca to S-Pbca); it occurs together with orbital order, which follows, rather than produces, the structural transition. (ii) In the metallic L-Pbca phase the orbital polarization is ~0. (iii) In the insulating S-Pbca phase the lower energy orbital, ~xy, is full. (iv) The spin-flip and pair-hopping Coulomb terms reduce the effective masses in the metallic phase. Our results indicate that a similar scenario applies to Ca_{2-x}Sr_xRuO_4 (x<0.2). In the metallic x< 0.5 structures electrons are progressively transferred to the xz/yz bands with increasing x, however we find no orbital-selective Mott transition down to ~300 K., Comment: 4 pages, 3 figures; published version

Based on ab-initio calculations we identify possible scenarios for the Kondo effect due to Co ad-atoms on graphene. General symmetry arguments show that for magnetic atoms in high-symmetry positions, the Kondo effect in graphene is controlled not only by the spin but also by the orbital degree of freedom. For a Co atom absorbed on top of a carbon atom, the Kondo effect is quenched by spin-orbit coupling below an energy scale of $\sim 15$\,K. For Co with spin $S=1/2$ located in the center of a hexagon, an SU(4) Kondo model describes the entanglement of orbital moment and spin at higher energies, while below \sim 60$\,meV spin-orbit coupling leads to a more conventional SU(2) Kondo effect. The interplay of the orbital Co physics and the peculiar band-structure of graphene is directly accessible in Fourier transform tunneling spectroscopy or in the gate-voltage dependence of the Kondo temperature displaying a very strong, characteristic particle-hole asymmetry., Comment: 6 pages, 4 figures (extended version)

We consider the theory of Kondo effect and Fano factor energy dependence for magnetic impurity (Co) on graphene. We have performed a first principles calculation and find that the two dimensional $E_1$ representation made of $d_{xz},d_{yz}$ orbitals is likely to be responsible for the hybridization and ultimately Kondo screening for cobalt on graphene. There are few high symmetry sites where magnetic impurity atom can be adsorbed. For the case of Co atom in the middle of hexagon of carbon lattice we find anomalously large Fano $q$-factor, $q\approx 80$ and strongly suppressed coupling to conduction band. This anomaly is a striking example of quantum mechanical interference related to the Berry phase inherent to graphene band structure., Comment: 5 pages, 5 eps figure files

The electronic structure of a prototype Kondo system, a cobalt impurity in a copper host is calculated with accurate taking into account of correlation effects on the Co atom. Using the recently developed continuous-time QMC technique, it is possible to describe the Kondo resonance with a complete four-index Coulomb interaction matrix. This opens a way for completely first-principle calculations of the Kondo temperature. We have demonstrated that a standard practice of using a truncated Hubbard Hamiltonian to consider the Kondo physics can be quantitatively inadequate., Comment: 6 pages, 4 figures

Monovalent impurities on graphene can be divided into ionically and covalently bond impurities. The covalent impurities cause universal midgap states as the carbon atom next to the impurity is effectively decoupled from the graphene pi-bands. The electronic structure of graphene suppresses migration of these impurities and making the universal midgap very stable. This effect is strongest for neutral covalently bond impurities. The ionically bond impurities have migration barriers of typically less than 0.1eV. An asymmetry between anions and cations regarding their adsorption sites and topology of their potential energy landscape is predicted., Comment: 4 pages, 3 figures, 2 tables