arXiv subjects

E. Müller-Hartmann

Publications and source records attributed to E. Müller-Hartmann.

At least 19 recordsLinked to original sources

arXiv2008

Mott-Hubbard exciton in the optical conductivity of YTiO3 and SmTiO3

In the Mott-Hubbard insulators YTiO3 and SmTiO3 we study optical excitations from the lower to the upper Hubbard band, d^1d^1 -> d^0d^2. The multi-peak structure observed in the optical conductivity reflects the multiplet structure of the upper Hubbard band in a multi-orbital system. Absorption bands at 2.55 and 4.15 eV in the ferromagnet YTiO3 correspond to final states with a triplet d^2 configuration, whereas a peak at 3.7 eV in the antiferromagnet SmTiO3 is attributed to a singlet d^2 final state. A strongly temperature-dependent peak at 1.95 eV in YTiO3 and 1.8 eV in SmTiO3 is interpreted in terms of a Hubbard exciton, i.e., a charge-neutral (quasi-)bound state of a hole in the lower Hubbard band and a double occupancy in the upper one. The binding to such a Hubbard exciton may arise both due to Coulomb attraction between nearest-neighbor sites and due to a lowering of the kinetic energy in a system with magnetic and/or orbital correlations. Furthermore, we observe anomalies of the spectral weight in the vicinity of the magnetic ordering transitions, both in YTiO3 and SmTiO3. In the G-type antiferromagnet SmTiO3, the sign of the change of the spectral weight at T_N depends on the polarization. This demonstrates that the temperature dependence of the spectral weight is not dominated by the spin-spin correlations, but rather reflects small changes of the orbital occupation.

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arXiv2007

Electronic phase transitions in the half-filled ionic Hubbard model

A detailed study of electronic phase transitions in the ionic Hubbard model at half filling is presented. Within the dynamical mean field approximation a series of transitions from the band insulator via a metallic state to a Mott-Hubbard insulating phase is found at intermediate values of the one-body potential $Δ$ with increasing the Coulomb interaction $U$. We obtain a critical region in which the metallic phase disappears and a {\it novel} coexistence phase between the band and the Mott insulating state sets in. Our results are consistent with those obtained at low dimensions, thus they provide a concrete description for the charge degrees of freedom of the ionic Hubbard model.

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arXiv2006

Band-Insulator-Metal-Mott-Insulator transition in the half--filled $t-t^{\prime}$ ionic-Hubbard chain

We investigate the ground state phase diagram of the half-filled $t-t^{\prime}$ repulsive Hubbard model in the presence of a staggered ionic potential $Δ$, using the continuum-limit bosonization approach. We find, that with increasing on-site-repulsion $U$, depending on the value of the next-nearest-hopping amplitude $t^{\prime}$, the model shows three different versions of the ground state phase diagram. For $t^{\prime} < t^{\prime}_{\ast}$, the ground state phase diagram consists of the following three insulating phases: Band-Insulator at $U U_{c}$. For $t^{\prime} > t^{\prime}_{c}$ there is only one transition from a spin gapped metallic phase at $U U_{c}$. Finally, for intermediate values of the next-nearest-hopping amplitude $t^{\prime}_{\ast} < t^{\prime} < t^{\prime}_{c}$ we find that with increasing on-site repulsion, at $U_{c1}$ the model undergoes a second-order commensurate-incommensurate type transition from a band insulator into a metallic state and at larger $U_{c2}$ there is a Kosterlitz-Thouless type transition from a metal into a ferroelectric insulator.

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arXiv2005

Re-examining the Verwey transition in Fe3O4

Motivated by recent structural data questioning the adequacy of the charge order (CO)/disorder picture for the Verwey transition (at T=T_V) in magnetite, we re-investigate this issue within a new theoretical picture. Using the state-of-the-art LDA+DMFT method, we show that the non-trivial interplay between the B-site octahedral distortions and strong, multi-orbital electronic correlations in the half-metallic state is a necessary ingredient for a proper quantitative understanding of the physical responses across T_V. While weak CO is found to have very small effects on the low-T spectral function, the low-T charge gap and the resistivity jump across T_V are quantitatively reproduced only upon inclusion of CO in LSDA+DMFT scheme. Our results strongly suggest that the Verwey transition is dominantly driven by multi-orbital electronic correlations with associated JT distortions on the B-sublattice, and constitutes a non-trivial advance in attempts to understand the physics of Fe3O4.

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arXiv2005

Mott-Hubbard quantum criticality in paramagnetic CMR pyrochlores

We present a correlated {\it ab initio} description of the paramagnetic phase of Tl$_2$Mn$_2$O$_7$, employing a combined local density approximation (LDA) with multiorbital dynamical mean field theory (DMFT) treatment. We show that the insulating state observed in this colossal magnetoresistance (CMR) pyrochlore is determined by strong Mn intra- and inter-orbital local electron-electron interactions. Hybridization effects are reinforced by the correlation-induced spectral weight transfer. Our result coincides with optical conductivity measurements, whose low energy features are remarkably accounted for by our theory. Based on this agreement, we study the disorder-driven insulator-metal transition of doped compounds, showing the proximity of Tl$_2$Mn$_2$O$_7$ to quantum phase transitions, in agreement with recent measurements.

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arXiv2005

Insulator-Metal Transition in the Rutile-based VO2

The metal-insulator transition (MIT) in paramagnetic VO2 is studied within LDA+DMFT(IPT), which merges the local density approximation (LDA) with dynamical mean field theory (DMFT). With a fixed value of the Coulomb U=5.0eV, we show how the MIT is understood in a new picture: spectral weight transfer accompanying the increase in the displacement of V ion ($\perp c$) within the strong correlation scenario. Within this new scenario, we find good quantitative agreement with (i) switch of the orbital occupation of (xy,yz+zx,yz-zx), (ii) thermodynamics, and (iii) the one-electron spectral function in the metallic phase of VO2. We also compare our results for the total spectral density with other approaches which use QMC to solve the impurity problem of DMFT.

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arXiv2005

Orbital selective insulator-metal transition in V2O3 under external pressure

We present a detailed account of the physics of Vanadium sesquioxide (${\rm V_2O_3}$), a benchmark system for studying correlation induced metal-insulator transition(s). Based on a detailed perusal of a wide range of experimental data, we stress the importance of multi-orbital Coulomb interactions in concert with first-principles LDA bandstructure for a consistent understanding of the PI-PM MIT under pressure. Using LDA+DMFT, we show how the MIT is of the orbital selective type, driven by large changes in dynamical spectral weight in response to small changes in trigonal field splitting under pressure. Very good quantitative agreement with ($i$) the switch of orbital occupation and ($ii$) S=1 at each $V^{3+}$ site across the MIT, and ($iii$) carrier effective mass in the PM phase, is obtained. Finally, using the LDA+DMFT solution, we have estimated screening induced renormalisation of the local, multi-orbital Coulomb interactions. Computation of the one-particle spectral function using these screened values is shown to be in excellent quantitative agreement with very recent experimental (PES and XAS) results. These findings provide strong support for an orbital-selective Mott transition in paramagnetic ${\rm V_2O_3}$.

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arXiv2004

Metallizing the Mott insulator TiOCl by electron doping: a view from LDA+DMFT

Based on recent experiments, we describe the Mott insulating, but undimerized state of $TiOCl$ using the local-density approximation combined with multi-orbital dynamical mean field theory (LDA+DMFT) for this $3d^{1}$ system.Good agreement with the high estimated value of the superexchange is obtained. The possibility of an electron-doped insulator-metal transition in $TiOCl$ is investigated in this scheme and a Mott-Hubbard transition with a jump in carrier density {\it inside} the metallic state is found. Clear, co-incident, discontinuous changes in orbital occupations are observed, showing that such a transition would involve strong, multi-orbital correlations. These results call for studies on suitably intercalated $TiOCl$ that may induce metallization and, possibly, unconventional superconductivity.

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arXiv2004

VO2: a two-fluid incoherent metal?

We present {\it ab initio} LDA+DMFT results for the many-particle density of states of $VO_{2}$ on the metallic side of the strongly first-order ($T$-driven) insulator-metal transition. In strong contrast to LDA predictions, there is {\it no} remnant of even correlated Fermi liquid behavior in the correlated metal. Excellent quantitative agreement with published photoemission and X-ray absorption experiments is found in the metallic phase. We argue that the absence of FL-quasiparticles provides a natural explanation for the bad-metallic transport for $T > 340 K$. Based on this agreement, we propose that the I-M transition in $VO_{2}$ is an orbital-selective Mott transition, and point out the relevance of orbital resolved one-electron and optical spectroscopy to resolve this outstanding issue.

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arXiv2003

Insulator-Metal transition in the Doped 3d1 Transition Metal Oxide LaTiO3

The doping induced insulator-metal transition in $La_{1-x}Sr_{x}TiO_{3}$ is studied using the ab-initio LDA+DMFT method. Combining the LDA bandstructure for the actual, distorted structure found recently with multi-orbital DMFT to treat electronic correlations, we find: $(i)$ ferro-orbital order in the Mott insulating state without orbital degeneracy, $(ii)$ a continuous filling induced transition to the paramagnetic metal (PM) with $x$, and $(iii)$ excellent quantitative agreement with published photoemission data for the case of 6% doping. Our results imply that this system can be described as a Mott-Hubbard system without orbital (liquid) degeneracy.

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arXiv2003

Towards a Fully Ab-Initio Description of the Diluted Magnetic Semiconductor $Ga_{1-x}Mn_{x}As$. Ferromagnetism, Electronic Structure, and Optical Response

There are two competing views of itinerant ferromagnetism, the first viewing ferromagnetism as resulting from the indirect coupling between local moments via the itinerant carrier dynamics, the so-called RKKY mechanism, while in the alternative picture, ferromagnetism results from the spin polarization of itinerant carriers by the strong atomic Hund interaction - the so-called double exchange (DE) scenario. Which view describes the ferromagnetism in diluted magnetic semiconductors, materials with promise for spintronic applications, is still unclear. Here, we describe the detailed physical response of the prototype material $Ga_{1-x}Mn_{x}As$ using a combination of first-principles bandstructure with methods based on dynamical mean field theory to incorporate strong, dynamical correlations {\it and} intrinsic as well as extrinsic disorder in one single theoretical picture. We show how ferromagnetism is driven by DE, in agreement with very recent observations, along with a good quantitative description of the details of the electronic structure, as probed by scanning tunnelling microscopy (STM) and optical conductivity. Our results show how ferromagnetism can be driven by DE even in diluted magnetic semiconductors with small carrier concentration.

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arXiv2002

Orbital Switching and the First-Order Insulator-Metal Transition in Paramagnetic V_2O_3

The first-order metal-insulator transition (MIT) in paramagnetic $V_{2}O_{3}$ is studied within the ab-initio scheme LDA+DMFT, which merges the local density approximation (LDA) with dynamical mean field theory (DMFT). With a fixed value of the Coulomb $U=6.0 eV$, we show how the abrupt pressure driven MIT is understood in a new picture: pressure-induced decrease of the trigonal distortion within the strong correlation scenario (which is not obtained within LDA). We find good quantitative agreement with $(i)$ switch of the orbital occupation of $(a_{1g},e_{g1}^π, e_{g2}^π)$ and the spin state S=1 across the MIT, $(ii)$ thermodynamics and $dc$ resistivity, and $(iii)$ the one-electron spectral function, within this new scenario.

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arXiv2002

Orbital Kondo Effect in $CrO_{2}$: A LSDA+DMFT Study

Motivated by a collection of experimental results indicating the strongly correlated nature of the ferromagnetic metallic state of $CrO_{2}$, we present results based on a combination of the actual bandstructure [3] with dynamical mean-field theory (DMFT) for the multi-orbital case. In striking contrast with LSDA(+U) [3] and model many-body approaches [14], much better semiquantitative agreement with (i) recent photoemission results, (ii) domain of applicability of the half-metal concept, and (iii) thermodynamic and dc transport data, is obtained within a single picture. Our approach has broad applications for the detailed first principles investigation of other transition metal oxide-based half-metallic ferromagnets.

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arXiv2002

On the Normal State Electronic properties of Layered Sr_2 RuO_4

Based on a comprehensive perusal of experimental results, we construct a microscopic model describing the normal state of layered 4d oxide Sr_2 RuO_4 incorporating relevant quantum chemical features of the material. The high-T anomalies are explained within a Luttinger liquid (LL) picture. Interlayer one-particle hopping drives a dimensional crossover to a correlated Fermi liquid below a scale E^{*} << t_{perp}. Using recently developed chain-dynamical mean field theory, the low value of E^{*}, as well as various puzzling features of the low-T normal state are explained as manifestations of the crossover from the high-T Luttinger liquid state in a consistent way.

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arXiv2002

Derivation of effective spin models from a three band model for CuO_2-planes

The derivation of effective spin models describing the low energy magnetic properties of undoped CuO_2-planes is reinvestigated. Our study aims at a quantitative determination of the parameters of effective spin models from those of a multi-band model and is supposed to be relevant to the analysis of recent improved experimental data on the spin wave spectrum of La_2CuO_4. Starting from a conventional three-band model we determine the exchange couplings for the nearest and next-nearest neighbor Heisenberg exchange as well as for 4- and 6-spin exchange terms via a direct perturbation expansion up to 12th (14th for the 4-spin term) order with respect to the copper-oxygen hopping t_pd. Our results demonstrate that this perturbation expansion does not converge for hopping parameters of the relevant size. Well behaved extrapolations of the couplings are derived, however, in terms of Pade approximants. In order to check the significance of these results from the direct perturbation expansion we employ the Zhang-Rice reformulation of the three band model in terms of hybridizing oxygen Wannier orbitals centered at copper ion sites. In the Wannier notation the perturbation expansion is reorganized by an exact treatment of the strong site-diagonal hybridization. The perturbation expansion with respect to the weak intersite hybridizations is calculated up to 4th order for the Heisenberg coupling and up to 6th order for the 4-spin coupling. It shows excellent convergence and the results are in agreement with the Pade approximants of the direct expansion. The relevance of the 4-spin coupling as the leading correction to the nearest neighbor Heisenberg model is emphasized.

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arXiv2002

On the heavy-fermion behavior of the pyrochlore transition-metal oxide $LiV_{2}O_{4}$

Motivated by the heavy fermion Fermi liquid (HFFL) features observed at low-$T$ in the pyrochlore $LiV_{2}O_{4}$, we consider a material-specific model that includes aspects of the local quantum chemistry, the geometrically frustrated lattice structure, and strong correlations in a {\it single} approach. In particular, we show how geometrical frustration (GF) gives rise to a crossover scale, $T^{*}<<J$, the intersite (AF) exchange, below which the metallic system shows HFFL features. Our scenario is a specific realization of the importance of GF effects in driving HFFL behavior in $LiV_{2}O_{4}$, and provides a natural understanding of various puzzling features observed experimentally.

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arXiv2001

Dynamical correlations in half-metallic manganites

Motivated by the recent optical and photoemission measurements on half-metallic ferromagnetic three-dimensional manganites, we combine a tight-binding fit of the one-particle bandstructure with the dynamical mean-field theory, which treats the dynamical orbital correlations and the combination of Jahn-Teller and doping-induced disorder on the same footing. We show how all of the above effects are necessary to obtain good semiquantitative agreement with experimental features. As applications, we show how modest external magnetic fields drive drastic changes in the optical spectrum, demonstrating the {\it colossal ac magnetoconductivity}. The photoemission lineshape contribution is evaluated, and good agreement with published experimental work is found.

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arXiv2001

On the Origin of the Non-Fermi Liquid Behavior of SrRuO_{3}

Motivated by the unusual features observed in the transport properties of the ferromagnetic "bad metal" $SrRuO_{3}$, we construct a model incorporating essential features of the realistic structure of this nearly cubic material. In particular, we show how the $t_{2g}$orbital {\it orientation} in the perfectly cubic structure determines the peculiar structure of the hybridization matrix, and demonstrate how the local non-Fermi liquid features arise when interactions are switched on. we discuss the effect of the slight deviation from the cubic structure (at low-$T$) qualitatively. The model provides a consistent explanation of the features observed recently in the optical response of $SrRuO_{3}$.

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