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A. I. Lichtenstein

Publications and source records attributed to A. I. Lichtenstein.

At least 55 records · Page 3Linked to original sources

Standard model of the rare-earths, analyzed from the Hubbard I approximation

In this work we examine critically the electronic structure of the rare-earth elements by use of the so-called Hubbard I approximation. From the theoretical side all measured features of both occupied and unoccupied states are reproduced, without significant deviations between observations and theory. We also examine cohesive properties like the equilibrium volume and bulk modulus, where we find, in general, a good agreement between theory and measurements. In addition we have reproduced the spin and orbital moments of these elements, as they are reflected from measurements of the saturation moment. We have also employed the Hubbard I approximation to extract the interatomic exchange parameters of an effective spin Hamiltonian for the heavy rare earths. We show that the Hubbard I approximation gives results which are consistent with calculations where $4f$ electrons are treated as core states for Gd. The latter approach was also used to address the series of the heavy/late rare-earths. Via Monte Carlo simulations we obtained ordering temperatures which reproduce measurements within about $20\%$. We have further illustrated the accuracy of these exchange parameters by comparing measured and calculated magnetic configurations for the heavy rare earths and the magnon dispersion for Gd. The Hubbard I approximation is compared to other theories of the electronic structure, and we argue that it is superior. We discuss the relevance of our results in general, and how this makes it possible to treat the electronic structure of materials containing rare-earth elements, such as permanent magnets, magnetostrictive compounds, photovoltaics, optical fibers, topological insulators, and molecular magnets.

cond-mat.str-el↗

Many-body effects on Cr(001) surfaces: An LDA+DMFT study

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.

cond-mat.str-el↗

Tuning emergent magnetism in a Hund's impurity

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.

cond-mat.str-el↗

Plaquette Valence Bond Theory of High-Temperature Superconductivity

We present a strong-coupling approach to the theory of high-temperature superconductivity based on the observation of a quantum critical point in the plaquette within the t,t' Hubbard model. The crossing of ground state energies in the N=2,3,4 sectors occurs for parameters close to the optimal doping. The theory predicts the maximum of the d(x2-y2)-wave order parameter at the border between localized and itinerant electron behavior and gives a natural explanation for the pseudo-gap formation via soft-fermion mode related to local singlet states of the plaquette in the environment. Our approach follows the general line of resonating valence bond theory stressing a crucial role of singlets in the physics of high-Tc superconductors, but focuses on the formation of local singlets, similar to phenomena observed in frustrated one-dimensional quantum spin models.

cond-mat.str-el↗

Self-consistent Dual Boson approach to single-particle and collective excitations in correlated systems

We propose an efficient dual boson scheme, which extends the DMFT paradigm to collective excitations in correlated systems. The theory is fully self-consistent both on the one- and on the two-particle level, thus describing the formation of collective modes as well as the renormalization of electronic and bosonic spectra on equal footing. The method employs an effective impurity model comprising both fermionic and bosonic hybridization functions. Only single- and two-electron Green's functions of the reference problem enter the theory, due to the optimal choice of the self-consistency condition for the effective bosonic bath. We show that the theory is naturally described by a dual Luttinger-Ward functional and obeys the relevant conservation laws.

cond-mat.str-el↗

Comparing XMCD and DFT with STM spin excitation spectroscopy for Fe and Co adatoms on Cu$_{2}$N/Cu(100)

We report on the magnetic properties of Fe and Co adatoms on a Cu$_{2}$N/Cu(100)-$c(2 \times 2)$ surface investigated by x-ray magnetic dichroism measurements and density functional theory (DFT) calculations including the local coulomb interaction. We compare these results with properties formerly deduced from STM spin excitation spectroscopy (SES) performed on the individual adatoms. In particular we focus on the values of the local magnetic moments determined by XMCD compared to the expectation values derived from the description of the SES data.The angular dependence of the projected magnetic moments along the magnetic field, as measured by XMCD, can be understood on the basis of the SES Hamiltonian. In agreement with DFT, the XMCD measurements show large orbital contributions to the total magnetic moment for both magnetic adatoms.

cond-mat.mes-hall↗

Racah materials: role of atomic multiplets in intermediate valence systems

We address the long-standing mystery of the nonmagnetic insulating state of the intermediate valence compound SmB$_6$. Within a combination of the local density approximation (LDA) and an exact diagonalization (ED) of an effective discrete Anderson impurity model, the intermediate valence ground state with the $f$-shell occupation $\langle n_{4f} \rangle=5.6$ is found for the Sm atom in SmB$_6$. This ground state is a singlet, and the first excited triplet state $\sim 3$ meV higher in the energy. SmB$_6$ is a narrow band insulator already in LDA, with the direct band gap of $\sim 10$ meV. The electron correlations increase the band gap which now becomes indirect. Thus, the many-body effects are relevant to form the indirect band gap, crucial for the idea of ``topological Kondo insulator" in SmB$_6$. Also, an actinide analog PuB$_6$ is considered, and the intermediate valence singlet ground state is found for the Pu atom. We propose that [Sm,Pu]B$_6$ belong to a new class of the intermediate valence materials with the multi-orbital ``Kondo-like" singlet ground-state. Crucial role of complex spin-orbital $f^n$-$f^{n+1}$ multiplet structure differently hybridized with ligand states in such Racah materials is discussed.

cond-mat.str-el↗

Layer-resolved magnetic exchange interactions of surfaces of late 3d elements: effects of electronic correlations

We present the results of an ab initio study of magnetic properties of Fe, Co and Ni surfaces. In particular, we discuss their electronic structure and magnetic exchange interactions (Jij), as obtained by means of a combination of density functional theory and dynamical mean-field theory. All studied systems have a pronounced tendency to ferromagnetism both for bulk and surface atoms. The presence of narrow-band surface states is shown to enhance the magnetic moment as well as the exchange couplings. The most interesting results were obtained for the Fe surface where the atoms have a tendency to couple antiferromagnetically with each other. This interaction is relatively small, when compared to interlayer ferromagnetic interaction, and strongly depends on the lattice parameter. Local correlation effects are shown to lead to strong changes of the overall shape of the spectral functions. However, they seem to not play a decisive role on the overall picture of the magnetic couplings studied here. We have also investigated the influence of correlations on the spin and orbital moments of the bulk-like and surface atoms. We found that dynamical correlations in general lead to enhanced values of the orbital moment.

physics.comp-ph↗

Microscopic origin of Heisenberg and non-Heisenberg exchange interactions in ferromagnetic bcc Fe

By means of first principles calculations we investigate the nature of exchange coupling in ferromagnetic bcc Fe on a microscopic level. Analyzing the basic electronic structure reveals a drastic difference between the $3d$ orbitals of $E_g$ and $T_{2g}$ symmetries. The latter ones define the shape of the Fermi surface, while the former ones form weakly-interacting impurity levels. We demonstrate that, as a result of this, in Fe the $T_{2g}$ orbitals participate in exchange interactions, which are only weakly dependent on the configuration of the spin moments and thus can be classified as Heisenberg-like. These couplings are shown to be driven by Fermi surface nesting. In contrast, for the $E_g$ states the Heisenberg picture breaks down, since the corresponding contribution to the exchange interactions is shown to strongly depend on the reference state they are extracted from. Our analysis of the nearest-neighbour coupling indicates that the interactions among $E_g$ states are mainly proportional to the corresponding hopping integral and thus can be attributed to be of double-exchange origin.

cond-mat.mtrl-sci↗

Exchange parameters of strongly correlated materials: extraction from spin-polarised density functional theory plus dynamical mean field theory

In this paper we present an accurate numerical scheme for extracting inter-atomic exchange parameters ($J_{ij}$) of strongly correlated systems, based on first-principles full-potential electronic structure theory. The electronic structure is modelled with the help of a full-potential linear muffin-tin orbital method. The effects of strong electron correlations are considered within the charge self-consistent density functional theory plus dynamical mean-field theory (DFT+DMFT). The exchange parameters are then extracted using the magnetic force theorem, hence all the calculations are performed within a single computational framework. The method allows to investigate how the $J_{ij}$-parameters are affected by dynamical electron correlations. In addition to describing the formalism and details of the implementation, we also present magnetic properties of a few commonly discussed systems, characterised by different degrees of electron localisation. In bcc Fe we found a minor renormalisation of the $J_{ij}$ interactions once the dynamical correlations are introduced. However, generally, if the magnetic coupling has several competing contributions from different orbitals, the redistribution of the spectral weight and changes in the exchange splitting of these states can lead to a dramatic modification of the total interaction parameter. In NiO we found that both static and dynamical mean-field results provide an adequate description of the exchange interactions, which is somewhat surprising given the fact that these two methods result in quite different electronic structures. By employing Hubbard-I approximation for the treatment of the $4f$ states in hcp Gd we reproduce the experimentally observed multiplet structure. The calculated exchange parameters result to be rather close to the ones obtained by treating the $4f$ electrons as non-interacting core states.

cond-mat.str-el↗

Correlation-driven charge and spin fluctuations in LaCoO$_3$

The spin transition in LaCoO$_3$ has been investigated within the density-functional theory + dynamical mean-field theory formalism using continuous time quantum Monte Carlo. Calculations on the experimental rhombohedral atomic structure with two Co sites per unit cell show that an independent treatment of the Co atoms results in a ground state with strong charge fluctuations induced by electronic correlations. Each atom shows a contribution from either a $d^5$ or a $d^7$ state in addition to the main $d^6$ state. These states play a relevant role in the spin transition which can be understood as a low spin-high spin (LS-HS) transition with significant contributions ($\sim$ $10$ %) to the LS and HS states of $d^5$ and $d^7$ states respectively. A thermodynamic analysis reveals a significant kinetic energy gain through introduction of charge fluctuations, which in addition to the potential energy reduction lowers the total energy of the system.

cond-mat.str-el↗

Plasmons in strongly correlated systems: spectral weight transfer and renormalized dispersion

We study the charge-density dynamics within the two-dimensional extended Hubbard model in the presence of long-range Coulomb interaction across the metal-insulator transition point. To take into account strong correlations we start from self-consistent extended dynamical mean-field theory and include non-local dynamical vertex corrections through a ladder approximation to the polarization operator. This is necessary to fulfill charge conservation and to describe plasmons in the correlated state. The calculated plasmon spectra are qualitatively different from those in the random-phase approximation: they exhibit a spectral density transfer and a renormalized dispersion with enhanced deviation from the canonical $\sqrt{q}$-behavior. Both features are reminiscent of interaction induced changes found in single-electron spectra of strongly correlated systems.

cond-mat.str-el↗

Probing of valley polarization in graphene via optical second-harmonic generation

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.

cond-mat.mes-hall↗

First-principles modelling of magnetic excitations in Mn12

We have developed a fully microscopic theory of magnetic properties of the prototype molecular magnet Mn12. First, the intra-molecular magnetic properties have been studied by means of first-principles density functional-based methods, with local correlation effects being taken into account within the local density approximation plus U (LDA+U) approach. Using the magnetic force theorem, we have calculated the interatomic isotropic and anisotropic exchange interactions and full tensors of single-ion anisotropy for each Mn ion. Dzyaloshinskii-Moriya (DM) interaction parameters turned out to be unusually large, reflecting a low symmetry of magnetic pairs in molecules, in comparison with bulk crystals. Based on these results we predict a distortion of ferrimagnetic ordering due to DM interactions. Further, we use an exact diagonalization approach allowing to work with as large Hilbert space dimension as 10^8 without any particular symmetry (the case of the constructed magnetic model). Based on the computational results for the excitation spectrum, we propose a distinct interpretation of the experimental inelastic neutron scattering spectra.

cond-mat.str-el↗

Twisted magnetic patterns: Exploring the Dzyaloshinskii--Moriya vector

Magnetism - the spontaneous alignment of atomic moments in a material - is driven by quantum-mechanical `exchange' interactions which operate over atomic distances as a result of the fundamental symmetry of electrons. Currently, one of the most active fields of condensed matter physics involves the study of magnetic interactions that cause, or are caused by a twisting of nearby atoms. This can lead to the magnetoelectric effect that couples electric and magnetic properties, and is predicted to play a prominent role in future technology. Here, we discuss the complex relativistic interplay between magnetism and atomic crystal structure in a class of materials called `weak ferromagnets'. The sign of the underpinning Dzyaloshinskii--Moriya interaction has been determined for the first time, by using synchrotron radiation to study iron borate (FeBO3). We present a novel experimental technique based on interference between two x-ray scattering processes (one acts as a reference wave) which we combine with a second unusual approach of turning the atomic antiferromagnetic motif with a small magnetic field. We show that the experimental results provide a clear validation of state-of-the-art theoretical calculations. These experimental and theoretical approaches open up new possibilities for exploring, modelling and exploiting novel magnetic and magnetoelectric materials.

cond-mat.str-el↗

Electronic correlations determine the phase stability of iron up to the melting temperature

We present theoretical results on the high-temperature phase stability and phonon spectra of paramagnetic bcc iron which explicitly take into account many-body effects. Several peculiarities, including a pronounced softening of the [110] transverse (T$_1$) mode and a dynamical instability of the bcc lattice in harmonic approximation are identified. We relate these features to the $α$-to-$γ$ and $γ$-to-$δ$ phase transformations in iron. The high-temperature bcc phase is found to be highly anharmonic and appears to be stabilized by the lattice entropy.

cond-mat.str-el↗

Doping Mechanisms in Graphene-MoS2 Hybrids

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.

cond-mat.mes-hall↗

Ferromagnetic two-dimensional crystals: Single layers of K2CuF4

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.

cond-mat.mes-hall↗