arXiv subjects

V. Eyert

Publications and source records attributed to V. Eyert.

At least 19 recordsLinked to original sources

arXiv2019

Oxygen vacancies and hydrogen doping in LaAlO3/SrTiO3 heterostructures: electronic properties and impact on surface and interface reconstruction

We investigate the effect of oxygen vacancies and hydrogen dopants at the surface and inside slabs of LaAlO3, SrTiO3, and LaAlO3/SrTiO3 heterostructures on the electronic properties by means of electronic structure calculations as based on density functional theory. Depending on the concentration, the presence of these defects in LaAlO3 slab can suppress the surface conductivity. In contrast, in insulating SrTiO3 slabs already very small concentrations of oxygen vacancies or hydrogen dopant atoms induce a finite occupation of the conduction band. Surface defects in insulating LaAlO3/SrTiO3 heterostructure slabs with three LaAlO3 overlayers lead to the emergence of interface conductivity. Calculated defect formation energies reveal strong preference of hydrogen dopant atoms for surface sites for all structures and concentrations considered. Strong decrease of the defect formation energy of hydrogen adatoms with increasing thickness of the LaAlO3 overlayer and crossover from positive to negative values, taken together with the metallic conductivity induced by hydrogen adatoms, seamlessly explains the semiconductor-metal transition observed for these heterostructures as a function of the overlayer thickness. Moreover, we show that the potential drop and concomitant shift of (layer resolved) band edges is suppressed for the metallic configuration. Finally, magnetism with stable local moments, which form atomically thin magnetic layers at the interface, is generated by oxygen vacancies either at the surface or the interface, or by hydrogen atoms buried at the interface. In particular, oxygen vacancies in the TiO2 interface layer cause drastic downshift of the 3d e_g states of the Ti atoms neighboring the vacancies, giving rise to strongly localized magnetic moments, which add to the two-dimensional background magnetization.

cond-mat.str-el↗

arXiv2017

Weakly-correlated nature of ferromagnetism in non symmorphic CrO$_2$ revealed by bulk-sensitive soft X ray ARPES

Chromium dioxide CrO$_2$ belongs to a class of materials called ferromagnetic half-metals, whose peculiar aspect is to act as a metal in one spin orientation and as semiconductor or insulator in the opposite one. Despite numerous experimental and theoretical studies motivated by technologically important applications of this material in spintronics, its fundamental properties such as momentum resolved electron dispersions and Fermi surface have so far remained experimentally inaccessible due to metastability of its surface that instantly reduces to amorphous Cr$_2$O$_3$. In this work, we demonstrate that direct access to the native electronic structure of CrO$_2$ can be achieved with soft-X-ray angle-resolved photoemission spectroscopy whose large probing depth penetrates through the Cr$_2$O$_3$ layer. For the first time the electronic dispersions and Fermi surface of CrO$_2$ are measured, which are fundamental prerequisites to solve the long debate on the nature of electronic correlations in this material. Since density functional theory augmented by a relatively weak local Coulomb repulsion gives an exhaustive description of our spectroscopic data, we rule out strong-coupling theories of CrO$_2$. Crucial for the correct interpretation of our experimental data in terms of the valence band dispersions is the understanding of a non-trivial spectral response of CrO$_2$ caused by interference effects in the photoemission process originating from the non-symmorphic space group of the rutile crystal structure of CrO$_2$.

cond-mat.mtrl-sci↗

arXiv2017

Electronic properties of LaAlO3/SrTiO3 n-type interfaces: A GGA+U study

The role of electronic correlation effects for a realistic description of the electronic properties of LaAlO3/SrTiO3 heterostructures as covered by the on-site Coulomb repulsion within the GGA+U approach is investigated. Performing a systematic variation of the values of the Coulomb parameters applied to the Ti 3d and La 4f orbitals we put previous suggestions to include a large value for the La 4f states into perspective. Furthermore, our calculations provide deeper insight into the band gap landscape in the space spanned by these Coulomb parameters and the resulting complex interference effects. In addition, we identify important correlations between the local Coulomb interaction within the La 4f shell, the band gap, and the atomic displacements at the interface. In particular, these on-site Coulomb interactions influence buckling within the LaO interface layer, which via its strong coupling to the electrostatic potential in the LAO overlayer causes considerable shifts of the electronic states at the surface and eventually controls the band gap.

cond-mat.str-el↗

arXiv2016

Analysis of electronic and structural properties of surfaces and interfaces based on LaAlO3 and SrTiO3

Recently, it was established that a two-dimensional electron system can arise at the interface between two oxide insulators LaAlO3 and SrTiO3. This paradigmatic example exhibits metallic behaviour and magnetic properties between non-magnetic and insulating oxides. Despite a huge amount of theoretical and experimental work a thorough understanding has yet to be achieved. We analyzed the structural deformations of a LaAlO3 (001) slab induced by hydrogen ad-atoms and oxygen vacancies at its surface by means of density functional theory. Moreover, we investigated the influence of surface reconstruction on the density of states and determined the change of the local density of states at the Fermi level with increasing distance from the surface for bare LaAlO3 and for a conducting LaAlO3/SrTiO3 interface. In addition, the Al-atom displacements and distortions of the TiO6-octahedra were estimated.

cond-mat.str-el↗

arXiv2013

Formation of Nickel-Platinum Silicides on a Silicon Substrate: Structure, Phase Stability, and Diffusion from Ab initio Computations

The formation of Ni(Pt)silicides on a Si(001) surface is investigated using an ab initio approach. After deposition of a Ni overlayer alloyed with Pt, the calculations reveal fast diffusion of Ni atoms into the Si lattice, which leads initially to the formation of Ni2Si. At the same time Si atoms are found to diffuse into the metallic overlayer. The transformation of Ni2Si into NiSi is likely to proceed via a vacancy-assisted diffusion mechanism. Silicon atoms are the main diffusing species in this transformation, migrating from the Si substrate through the growing NiSi layer into the Ni2Si. Pt atoms have a low solubility in Ni2Si and prefer Si-sites in the NiSi lattice, thereby stabilizing the NiSi phase. The diffusivity of Pt is lower than that of Ni. Furthermore, Pt atoms have a tendency to segregate to interfaces, thereby acting as diffusion barriers.

cond-mat.mtrl-sci↗

arXiv2013

Metal-insulator transition at the LaAlO3/SrTiO3 interface revisited: A hybrid functional study

We investigate the electronic properties of the LaAlO3/SrTiO3 interface using density functional theory. In contrast to previous studies, which relied on (semi-)local functionals and the GGA+U method, we here use a recently developed hybrid functional to determine the electronic structure. This approach offers the distinct advantage of accessing both the metallic and insulating multilayers on a parameter-free equal footing. As compared to calculations based on semilocal GGA functionals, our hybrid functional calculations lead to a considerably increased band gap for the insulating systems. The details of the electronic structure show substantial deviations from those obtained by GGA calculations. This casts severe doubts on all previous results based on semilocal functionals. In particular, corrections using rigid band shifts ("scissors operator") cannot lead to valid results.

cond-mat.str-el↗

arXiv2011

VO2: A Novel View from Band Theory

New calculations for vanadium dioxide, one of the most controversely discussed materials for decades, reveal that band theory as based on density functional theory is well capable of correctly describing the electronic and magnetic properties of the metallic as well as both the insulating M1 and M2 phases. Considerable progress in the understanding of the physics of VO2 is achieved by the use of the recently developed hybrid functionals, which include part of the electron-electron interaction exactly and thereby improve on the weaknesses of semilocal exchange functionals as provided by the local density and generalized gradient approximations. Much better agreement with photoemission data as compared to previous calculations is found and a consistent description of the rutile-type early transition-metal dioxides is achieved.

cond-mat.str-el↗

arXiv2010

Two-dimensional electron liquid state at LaAlO3-SrTiO3 interfaces

Using tunneling spectroscopy we have measured the spectral density of states of the mobile, two-dimensional electron system generated at the LaAlO3-SrTiO3 interface. As shown by the density of states the interface electron system differs qualitatively, first, from the electron systems of the materials defining the interface and, second, from the two-dimensional electron gases formed at interfaces between conventional semiconductors.

cond-mat.mtrl-sci↗

arXiv2009

Intermediate-valence behavior of the transition-metal oxide CaCu$_3$Ru$_4$O$_{12}$

The transition--metal oxide CaCu$_3$Ru$_4$O$_{12}$ with perovskite--type structure shows characteristic properties of an intermediate--valence system. The temperature--dependent susceptibility exhibits a broad maximum around $150 - 160$ K. At this temperature, neutron powder diffraction reveals a small but significant volume change whereby the crystal structure is preserved. Moreover, the temperature--dependent resistivity changes its slope. NMR Knight shift measurements of Ru reveal a cross--over from high temperature paramagnetic behavior of localized moments to itinerant band states at low temperatures. Additional density--functional theory calculations can relate the structural anomaly with the $d$--electron number. The different experimental and calculational methods result in a mutually consistent description of CaCu$_3$Ru$_4$O$_{12}$ as an intermediate--valent system in the classical sense of having low--energy charge fluctuations.

cond-mat.str-el↗

arXiv2008

Suppression of the ferromagnetic state in LaCoO3 films by rhombohedral distortion

Epitaxially strained LaCoO3 (LCO) thin films were grown with different film thickness, t, on (001) oriented (LaAlO3)0.3(SrAl0.5Ta0.5O3)0.7 (LSAT) substrates. After initial pseudomorphic growth the films start to relieve their strain partly by the formation of periodic nano-twins with twin planes predominantly along the <100> direction. Nano-twinning occurs already at the initial stage of growth, albeit in a more moderate way. Pseudomorphic grains, on the other hand, still grow up to a thickness of at least several tenths of nanometers. The twinning is attributed to the symmetry lowering of the epitaxially strained pseudo-tetragonal structure towards the relaxed rhombohedral structure of bulk LCO. However, the unit-cell volume of the pseudo-tetragonal structure is found to be nearly constant over a very large range of t. Only films with t > 130 nm show a significant relaxation of the lattice parameters towards values comparable to those of bulk LCO.

cond-mat.str-el↗

arXiv2008

Evolution of Quantum Criticality in CeNi_{9-x}Cu_xGe_4

Crystal structure, specific heat, thermal expansion, magnetic susceptibility and electrical resistivity studies of the heavy fermion system CeNi_{9-x}Cu_xGe_4 (0 <= x <= 1) reveal a continuous tuning of the ground state by Ni/Cu substitution from an effectively fourfold degenerate non-magnetic Kondo ground state of CeNi_9Ge_4 (with pronounced non-Fermi-liquid features) towards a magnetically ordered, effectively twofold degenerate ground state in CeNi_8CuGe_4 with T_N = 175 +- 5 mK. Quantum critical behavior, C/T ~ χ~ -ln(T), is observed for x about 0.4. Hitherto, CeNi_{9-x}Cu_xGe_4 represents the first system where a substitution-driven quantum phase transition is connected not only with changes of the relative strength of Kondo effect and RKKY interaction, but also with a reduction of the effective crystal field ground state degeneracy.

cond-mat.str-el↗

arXiv2007

First principles investigations of the electronic, magnetic and chemical bonding properties of CeTSn (T=Rh,Ru)

The electronic structures of CeRhSn and CeRuSn are self-consistently calculated within density functional theory using the local spin density approximation for exchange and correlation. In agreement with experimental findings, the analyses of the electronic structures and of the chemical bonding properties point to the absence of magnetization within the mixed valent Rh based system while a finite magnetic moment is observed for trivalent cerium within the Ru-based stannide, which contains both trivalent and intermediate valent Ce.

cond-mat.str-el↗

arXiv2006

First principles study of the electronic and magnetic structures of the tetragonal and orthorhombic phases of Ca3Mn2O7

On the basis of density functional theory electronic band structure calculations using the augmented spherical wave method, the electronic and magnetic properties of the orthorhombic and tetragonal phases of Ca3Mn2O7 were investigated and the spin exchange interactions of the orthorhombic phase were analyzed. Our calculations show that the magnetic insulating states are more stable than the non-magnetic metallic state for both polymorphs of Ca3Mn2O7, the orthorhombic phase is more stable than the tetragonal phase, and the ground state of the orthorhombic phase is antiferromagnetic. The total energies calculated for the three spin states of the orthorhombic phase of Ca3Mn2O7 led to estimates of the spin exchange interactions Jnn = -3.36 meV and Jnnn = -0.06 meV. The accuracy of these estimates were tested by calculating the Curie-Weiss temperature within the mean-field approximation.

cond-mat.mtrl-sci↗

arXiv2006

The antiferromagnetic insulator Ca3FeRhO6: characterization and electronic structure calculations

We investigate the antiferromagnetic insulating nature of Ca3FeRhO6 both experimentally and theoretically. Susceptibility measurements reveal a Neel temperature T_N = 20 K, and a magnetic moment of 5.3 muB/f. u., while Moessbauer spectroscopy strongly suggests that the Fe ions, located in trigonal prismatic sites, are in a 3+ high spin state. Transport measurements display a simple Arrhenius law, with an activation energy of 0.2 eV. The experimental results are interpreted with LSDA band structure calculations, which confirm the Fe 3+ state, the high-spin/low-spin scenario, the antiferromagnetic ordering, and the value for the activation energy.

cond-mat.str-el↗

arXiv2005

Poly-MTO, {(CH_3)_{0.92} Re O_3}_\infty, a Conducting Two-Dimensional Organometallic Oxide

Polymeric methyltrioxorhenium, {(CH_{3})_{0.92}ReO_{3}}_{\infty} (poly-MTO), is the first member of a new class of organometallic hybrids which adopts the structural pattern and physical properties of classical perovskites in two dimensions (2D). We demonstrate how the electronic structure of poly-MTO can be tailored by intercalation of organic donor molecules, such as tetrathiafulvalene (TTF) or bis-(ethylendithio)-tetrathiafulvalene (BEDT-TTF), and by the inorganic acceptor SbF$_3$. Integration of donor molecules leads to a more insulating behavior of poly-MTO, whereas SbF$_3$ insertion does not cause any significant change in the resistivity. The resistivity data of pure poly-MTO is remarkably well described by a two-dimensional electron system. Below 38 K an unusual resistivity behavior, similar to that found in doped cuprates, is observed: The resistivity initially increases approximately as $ρ\sim$ ln$(1/T$) before it changes into a $\sqrt{T}$ dependence below 2 K. As an explanation we suggest a crossover from purely two-dimensional charge-carrier diffusion within the \{ReO$_2$\}$_{\infty}$ planes at high temperatures to three-dimensional diffusion at low temperatures in a disorder-enhanced electron-electron interaction scenario (Altshuler-Aronov correction). Furthermore, a linear positive magnetoresistance was found in the insulating regime, which is caused by spatial localization of itinerant electrons at some of the Re atoms, which formally adopt a $5d^1$ electronic configuration. X-ray diffraction, IR- and ESR-studies, temperature dependent magnetization and specific heat measurements in various magnetic fields suggest that the electronic structure of poly-MTO can safely be approximated by a purely 2D conductor.

cond-mat.mtrl-sci↗

arXiv2005

First principles investigation of the electronic structure of La2MnNiO6: A room-temperature insulating ferromagnet

Using first principles calculations within DFT based on the full potential APW+lo method, we calculated the electronic and magnetic structures for the ferromagnetic and antiferromagnetic states of La2MnNiO6 and analyzed the site projected density of states and electronic band structures. Our calculations show that the ground state of La2MnNiO6 is ferromagnetic insulating with the magnetization in agreement with Hund's first rule and experimental findings.

cond-mat.str-el↗

arXiv2005

Magnetic ordering in trigonal chain compounds

We present electronic structure calculations for the one-dimensional magnetic chain compounds Ca_3CoRhO_6 and Ca_3FeRhO_6. The calculations are based on density functional theory and the local density approximation. We use the augmented spherical wave (ASW) method. The observed alternation of low- and high-spin states along the Co-Rh and Fe-Rh chains is related to differences in the oxygen coordination of the transition metal sites. Due to strong hybridization the O 2p states are polarized, giving rise to extended localized magnetic moments centered at the high-spin sites. Strong metal-metal overlap along the chains leads to a substantial contribution of the low-spin Rh 4d_{3z^2-r^2} orbitals to the exchange coupling of the extended moments. Interestingly, this mechanism holds for both compounds, even though the coupling is ferromagnetic for the cobalt and antiferromagnetic for the iron compound. However, our results allow to understand the different types of coupling from the filling dependence of the electronic properties.

cond-mat.str-el↗

arXiv2005

Charge order and spin-singlet pairs formation in Ti4O7

Charge ordering in the low-temperature triclinic structure of titanium oxide (Ti4O7) is investigated using the local density approximation (LDA)+U method. Although the total 3d charge separation is rather small, an orbital order parameter defined as the difference between t2g occupancies of Ti$^{3+}$ and Ti$^{4+}$ cations is large and gives direct evidence for charge ordering. Ti 4s and 4p states make a large contribution to the static "screening" of the total 3d charge difference. This effective charge screening leads to complete loss of the disproportionation between the charges at 3+ and 4+ Ti sites. The occupied t2g states of Ti$^{3+}$ cations are predominantly of $d_{xy}$ character and form a spin-singlet molecular orbital via strong direct antiferromagnetic exchange coupling between neighboring Ti(1) and Ti(3) sites, whereas the role of superexchange is found to be negligible.

cond-mat.str-el↗