arXiv subjects

V. Eyert

Publications and source records attributed to V. Eyert.

At least 37 records · Page 2Linked to original sources

arXiv2005

The electronic structure of the antiferromagnetic semiconductor MnSb_2S_4

The electronic band structures of orthorhombic (oP28) and monoclinic (mC28) MnSb_2S_4 were investigated with ab initio calculations in the local spin density approximation (LSDA) to the density functional theory (DFT). An analysis of the electronic properties and of the chemical bonding is provided using the augmented spherical wave (ASW) method considering nonmagnetic, ferromagnetic, ferrimagnetic and antiferromagnetic model orderings. In agreement with experimental results both modifications of MnSb_2S_4 are predicted to be antiferromagnetic. While the experimental band gap is missed for the monoclinic polymorph, the calculated band gap for orthorhombic MnSb_2S_4 is close to the experimental one.

cond-mat.mtrl-sci↗

arXiv2005

Covalent bonding and hybridization effects in the corundum-type transition-metal oxides V2O3 and Ti2O3

The electronic structure of the corundum-type transition-metal oxides V2O3 and Ti2O3 is studied by means of the augmented spherical wave method, based on density-functional theory and the local density approximation. Comparing the results for the vanadate and the titanate allows us to understand the peculiar shape of the metal 3d a_{1g} density of states, which is present in both compounds. The a_{1g} states are subject to pronounced bonding-antibonding splitting due to metal-metal overlap along the c-axis of the corundum structure. However, the corresponding partial density of states is strongly asymmetric with considerably more weight on the high energy branch. We argue that this asymmetry is due to an unexpected broadening of the bonding a_{1g} states, which is caused by hybridization with the e_g^{pi} bands. In contrast, the antibonding a_{1g} states display no such hybridization and form a sharp peak. Our results shed new light on the role of the a_{1g} orbitals for the metal-insulator transitions of V2O3. In particular, due to a_{1g} - e_g^{pi} hybridization, an interpretation in terms of molecular orbital singlet states on the metal-metal pairs along the c-axis is not an adequate description.

cond-mat.str-el↗

arXiv2004

Two Aspects of the Mott-Hubbard Transition in Cr-doped V_2O_3

The combination of bandstructure theory in the local density approximation with dynamical mean field theory was recently successfully applied to V$_2$O$_3$ -- a material which undergoes the f amous Mott-Hubbard metal-insulator transition upon Cr doping. The aim of this sh ort paper is to emphasize two aspects of our recent results: (i) the filling of the Mott-Hubbard gap with increasing temperature, and (ii) the peculiarities of the Mott-Hubbard transition in this system which is not characterized by a diver gence of the effective mass for the $a_{1g}$-orbital.

cond-mat.str-el↗

arXiv2004

Ferromagnetism and temperature-dependent Electronic Structure of hcp Gadolinium

We use a combination of a many-body model analysis with an ab initio band structure calculation to derive the temperature dependent electronic quasiparticle structure of the rare-earth metal Gadolinium. As a local-moment system Gd is properly represented by the ferromagnetic (multiband) Kondo-lattice model (s-f (d-f) model). The single-particle part of the model-Hamiltonian is taken from an augmented spherical wave (ASW) band calculation. The proposed method avoids the double counting of relevant interactions by exploiting an exact limiting case of the model and takes into account the correct symmetry of atomic orbitals. The a priori only weakly correlated 5d conduction bands get via interband exchange coupling to the localized 4f levels a distinct temperature dependence which explains by a Rudermann-Kittel-Kasuya-Yosida (RKKY) -type mechanism the ferromagnetism of Gd. We get a self-consistently derived Curie temperature of 294.1 K and a T=0-moment of 7.71 $μ_{\rm B}$, surprisingly close to the experimental values. The striking induced temperature-dependence of the 5d conduction bands explains respective photoemission data. The only parameter of the theory (interband exchange coupling J) is uniquely fixed by the band calculation.

cond-mat.str-el↗

arXiv2004

Charge order, orbital order, and electron localization in the Magneli phase Ti4O7

The metal-insulator transition of the Magneli phase Ti4O7 is studied by means of augmented spherical wave (ASW) electronic structure calculations as based on density functional theory and the local density approximation. The results show that the metal-insulator transition arises from a complex interplay of charge order, orbital order, and singlet formation of those Ti 3d states which mediate metal-metal bonding inside the four-atom chains characteristic of the material. Ti4O7 thus combines important aspects of Fe3O4 and VO2. While the charge ordering closely resembles that observed at the Verwey transition, the orbital order and singlet formation appear to be identical to the mechanisms driving the metal-insulator transition of vanadium dioxide.

cond-mat.str-el↗

arXiv2004

Electronic Structure of Paramagnetic V_2O_3: Strongly Correlated Metallic and Mott Insulating Phase

LDA+DMFT, the computation scheme merging the local density approximation and the dynamical mean-field theory, is employed to calculate spectra both below and above the Fermi energy and spin and orbital occupations in the correlated paramagnetic metallic and Mott insulating phase of V_2O_3. The self-consistent DMFT equations are solved by quantum Monte Carlo simulations. Room temperature calculations provide direct comparison with experiment. They show a significant increase of the quasiparticle height in comparison with the results at 1160 K. We also obtain new insights into the nature of the Mott-Hubbard transition in V_2O_3. Namely, it is found to be strikingly different from that in the one-band Hubbard model due to the orbital degrees of freedom. Furthermore we resolve the puzzle of the unexpectedly small Mott gap in Cr-doped V_2O_3.

cond-mat.str-el↗

arXiv2004

Extended moment formation and magnetic ordering in the trigonal chain compound Ca3Co2O6

The results of electronic structure calculations for the one-dimensional magnetic chain compound Ca3Co2O6 are presented. The calculations are based on density functional theory and the local density approximation and used the augmented spherical wave (ASW) method. Our results allow for deeper understanding of recent experimental findings. In particular, alternation of Co 3d low- and high-spin states along the characteristic chains is related to differences in the oxygen coordination at the inequivalent cobalt sites. Strong hybridization of the d states with the O 2p states lays ground for polarization of the latter and the formation of extended localized magnetic moments centered at the high-spin sites. In contrast, strong metal-metal overlap along the chains gives rise to intrachain ferromagnetic exchange coupling of the extended moments via the d_{3z^2-r^2} orbitals of the low-spin cobalt atoms.

cond-mat.str-el↗

arXiv2003

Microscopic Derivation of Magnetic Coupling in Ca3Co2O6

For cobalt atoms placed along chain structures in Ca3Co2O6, we investigate the spin exchange coupling between atoms in high spin states. Consistent with experimental findings, the coupling is weakly ferromagnetic.

cond-mat.str-el↗

arXiv2003

The Metal-Insulator Transition of the Magneli phase V_4O_7: Implications for V_2O_3

The metal-insulator transition (MIT) of the Magneli phase V_4O_7 is studied by means of electronic structure calculations using the augmented spherical wave method. The calculations are based on density functional theory and the local density approximation. Changes of the electronic structure at the MIT are discussed in relation to the structural transformations occuring simultaneously. The analysis is based on a unified point of view of the crystal structures of all Magneli phase compounds V_nO_2n-1 (3 =< n =< 9) as well as of VO_2 and V_2O_3. This allows to group the electronic bands into states behaving similar to the dioxide or the sesquioxide. In addition, the relationship between the structural and electronic properties near the MIT of these oxides can be studied on an equal footing. For V_4O_7, a strong influence of metal-metal bonding across octahedral faces is found for states both parallel and perpendicular to the hexagonal c_hex axis of V_2O_3. Furthermore, the structural changes at the MIT cause localization of those states, which mediate in-plane metal-metal bonding via octahedral edges. This band narrowing opens the way to an increased influence of electronic correlations, which are regarded as playing a key role for the MIT of V_2O_3.

cond-mat↗

arXiv2003

Prominent quasi-particle peak in the photoemission spectrum of the metallic phase of V_2O_3

We present the first observation of a prominent quasi-particle peak in the photoemission spectrum of the metallic phase of V_2O_3 and report new spectral calculations that combine the local density approximation with the dynamical mean-field theory (using quantum Monte Carlo simulations) to show the development of such a distinct peak with decreasing temperature. The experimental peak width and weight are significantly larger than in the theory.

cond-mat.str-el↗

arXiv2003

Structure and electronic properties of new model dinitride systems: A density-functional study of CN2, SiN2, and GeN2

The dinitrides CN2, SiN2, and GeN2 in assumed pyrite-type structures are studied by means of density functional theory using both ultrasoft pseudopotentials and the augmented spherical wave (ASW) method. The former two materials constitute the large-x limit of the broader class of CNx and SiNx compounds, which are well known for their interesting mechanical and electronic properties. For CN2 a large bulk modulus B_0 of 405 GPa was determined . While SiN2 is found to be a wide band gap compound, the calculated gaps of CN2 and GeN2 are considerably smaller. The trends in structural and electronic properties as e.g. bond lengths, band gaps and covalency are well understood in terms of the interplay of different types of bonding.

cond-mat.mtrl-sci↗

arXiv2003

Octahedral Tilting in ACu3Ru4O12 (A=Na,Ca,Sr,La,Nd)

The perovskite-like compounds ACu3Ru4O12 (A=Na,Ca,Sr,La,Nd) are studied by means of density functional theory based electronic structure calculations using the augmented spherical wave (ASW) method. The electronic properties are strongly influenced by covalent type bonding between transition metal d and oxygen p states. The characteristic tilting of the RuO6 octahedra arises mainly from the Cu--O bonding, allowing for optimal bond lengths between these two atoms. Our results provide a deeper understanding of octahedral tilting as a universal mechanism, applicable to a large variety of multinary compounds.

cond-mat.mtrl-sci↗

arXiv2002

From VO2 to V2O3: The Metal-Insulator Transition of the Magneli Phase V6O11

The metal-insulator transition (MIT) of V6O11 is studied by means of electronic structure calculations using the augmented spherical wave method. The calculations are based on density functional theory and the local density approximation. Changes of the electronic structure at the MIT are discussed in relation to the structural transformations occuring simultaneously. The analysis is based on a unified point of view of the crystal structures of V6O11, VO2, and V2O3. This allows to group the electronic bands into states behaving similar to the dioxide or the sesquioxide. While the sesquioxide-like V 3d_yz states show rather weak changes on entering the low-temperature structure, some of the dioxide-like V 3d_x^2-y^2 states display splittings and shifts similar to those known from VO2. The MIT of V6O11 arises as a combination of changes appearing in both of these compounds. Our results shed new light onto the role of particular electronic states for the MIT of V2O3.

cond-mat.str-el↗

arXiv2001

The LDA+DMFT Approach to Materials with Strong Electronic Correlations

LDA+DMFT is a novel computational technique for ab initio investigations of real materials with strongly correlated electrons, such as transition metals and their oxides. It combines the strength of conventional band structure theory in the local density approximation (LDA) with a modern many-body approach, the dynamical mean-field theory (DMFT). In the last few years LDA+DMFT has proved to be a powerful tool for the realistic modeling of strongly correlated electronic systems. In this paper the basic ideas and the set-up of the LDA+DMFT(X) approach, where X is the method used to solve the DMFT equations, are discussed. Results obtained with X=QMC (quantum Monte Carlo) and X=NCA (non-crossing approximation) are presented and compared. By means of the model system La$_{1-x}$Sr$_{x}$TiO$_{3}$ we show that the method X matters qualitatively and quantitatively. Furthermore, we discuss recent results on the Mott-Hubbard metal-insulator transition in the transition metal oxide V$_2$O$_3$ and the $α$-$γ$ transition in the 4f-electron system Ce.

cond-mat.str-el↗

arXiv2001

Evidence for short range orbital order in paramagnetic insulating (Al,V)_2O_3

The local structure of (Al_0.06V_0.94)_2O_3 in the paramagnetic insulating (PI) and antiferromagnetically ordered insulating (AFI) phase has been investigated using hard and soft x-ray absorption techniques. It is shown that: 1) on a local scale, the symmetry of the vanadium sites in both the PI and the AFI phase is the same; and 2) the vanadium 3d - oxygen 2p hybridization, as gauged by the oxygen 1s absorption edge, is the same for both phases, but distinctly different from the paramagnetic metallic phase of pure V_2O_3. These findings can be understood in the context of a recently proposed model which relates the long range monoclinic distortion of the antiferromagnetically ordered state to orbital ordering, if orbital short range order in the PI phase is assumed. The measured anisotropy of the x-ray absorption spectra is discussed in relation to spin-polarized density functional calculations.

cond-mat.str-el↗

arXiv2001

The Metal-Insulator Transition of NbO2: an Embedded Peierls Instability

Results of first principles augmented spherical wave electronic structure calculations for niobium dioxide are presented. Both metallic rutile and insulating low-temperature NbO2, which crystallizes in a distorted rutile structure, are correctly described within density functional theory and the local density approximation. Metallic conductivity is carried to equal amounts by metal t_{2g} orbitals, which fall into the one-dimensional d_parallel band and the isotropically dispersing e_{g}^{pi} bands. Hybridization of both types of bands is almost negligible outside narrow rods along the line X--R. In the low-temperature phase splitting of the d_parallel band due to metal-metal dimerization as well as upshift of the e_{g}^{pi} bands due to increased p-d overlap remove the Fermi surface and open an optical band gap of about 0.1 eV. The metal-insulator transition arises as a Peierls instability of the d_parallel band in an embedding background of e_{g}^{pi} electrons. This basic mechanism should also apply to VO2, where, however, electronic correlations are expected to play a greater role due to stronger localization of the 3d electrons.

cond-mat.str-el↗

arXiv2000

Mott-Hubbard Metal-Insulator Transition in Paramagnetic V_2O_3: a LDA+DMFT(QMC) Study

The electronic properties of paramagnetic V_2O_3 are investigated by the ab-initio computational scheme LDA+DMFT(QMC). This approach merges the local density approximation (LDA) with dynamical mean-field theory (DMFT) and uses numerically exact quantum Monte Carlo simulations (QMC) to solve the effective Anderson impurity model of DMFT. Starting with the crystal structure of metallic V_2O_3 and insulating (V_{0.962}Cr_{0.038})_2O_3 we find a Mott-Hubbard metal-insulator-like transition at a Coulomb interaction U\approx 5eV. The calculated spectrum is in very good agreement with experiment. Furthermore, the occupation of the (a_{1g},e_{g1}^π,e_{g2}^π) orbitals and the spin state S=1 determined by us agree with recent polarization dependent X-ray-absorption experiments.

cond-mat.str-el↗

arXiv1999

Electronic structure and magnetic interactions in LiV2O4

We present results of all-electron electronic structure calculations for the recently discovered d electron heavy fermion compound LiV_2O_4. The augmented spherical wave calculations are based on density functional theory within the local density approximation. The electronic properties near the Fermi energy originate almost exclusively from V 3d t_{2g} states, which fall into two equally occupied subbands: While sigma-type metal-metal bonding leads to rather broad bands, small pi-type p-d overlap causes a narrow peak at E_F. Without the geometric frustration inherent in the crystal structure, spin-polarized calculations reveal an antiferromagnetic ground state and ferromagnetic order at slightly higher energy. Since direct d-d exchange interaction plays only a minor role, ordering of the localized vanadium moments can be attributed exclusively to a rather weak superexchange interaction. With the magnetic order suppressed by the geometric frustration, the remaining spin fluctuations suggest an explanation of the low temperature behaviour of the specific heat.

cond-mat.str-el↗