266 research outputs found
Electronic Structure Calculations with LDA+DMFT
The LDA+DMFT method is a very powerful tool for gaining insight into the
physics of strongly correlated materials. It combines traditional ab-initio
density-functional techniques with the dynamical mean-field theory. The core
aspects of the method are (i) building material-specific Hubbard-like many-body
models and (ii) solving them in the dynamical mean-field approximation. Step
(i) requires the construction of a localized one-electron basis, typically a
set of Wannier functions. It also involves a number of approximations, such as
the choice of the degrees of freedom for which many-body effects are explicitly
taken into account, the scheme to account for screening effects, or the form of
the double-counting correction. Step (ii) requires the dynamical mean-field
solution of multi-orbital generalized Hubbard models. Here central is the
quantum-impurity solver, which is also the computationally most demanding part
of the full LDA+DMFT approach. In this chapter I will introduce the core
aspects of the LDA+DMFT method and present a prototypical application.Comment: 21 pages, 7 figures. Chapter of "Many-Electron Approaches in Physics,
Chemistry and Mathematics: A Multidisciplinary View", eds. V. Bach and L.
Delle Site, Springer 201
Magnetic Moment Collapse-Driven Mott Transition in MnO
The metal-insulator transition in correlated electron systems, where electron
states transform from itinerant to localized, has been one of the central
themes of condensed matter physics for more than half a century. The
persistence of this question has been a consequence both of the intricacy of
the fundamental issues and the growing recognition of the complexities that
arise in real materials, even when strong repulsive interactions play the
primary role. The initial concept of Mott was based on the relative importance
of kinetic hopping (measured by the bandwidth) and on-site repulsion of
electrons. Real materials, however, have many additional degrees of freedom
that, as is recently attracting note, give rise to a rich variety of scenarios
for a ``Mott transition.'' Here we report results for the classic correlated
insulator MnO which reproduce a simultaneous moment collapse, volume collapse,
and metallization transition near the observed pressure, and identify the
mechanism as collapse of the magnetic moment due to increase of crystal field
splitting, rather than to variation in the bandwidth.Comment: 18 pages, 5 figur
Ab initio study of magnetism at the TiO2/LaAlO3 interface
In this paper we study the possible relation between the electronic and
magnetic structure of the TiO2/LaAlO3 interface and the unexpected magnetism
found in undoped TiO2 films grown on LaAlO. We concentrate on the role
played by structural relaxation and interfacial oxygen vacancies.
LaAlO3 has a layered structure along the (001) direction with alternating LaO
and AlO2 planes, with nominal charges of +1 and -1, respectively. As a
consequence of that, an oxygen deficient TiO2 film with anatase structure will
grow preferently on the AlO2 surface layer. We have therefore performed
ab-initio calculations for superlattices with TiO2/AlO2 interfaces with
interfacial oxygen vacancies. Our main results are that vacancies lead to a
change in the valence state of neighbour Ti atoms but not necessarily to a
magnetic solution and that the appearance of magnetism depends also on
structural details, such as second neighbor positions. These results are
obtained using both the LSDA and LSDA+U approximations.Comment: Accepted for publication in Journal of Materials Scienc
Oxide Heterostructures from a Realistic Many-Body Perspective
Oxide heterostructures are a new class of materials by design, that open the
possibility for engineering challenging electronic properties, in particular
correlation effects beyond an effective single-particle description. This short
review tries to highlight some of the demanding aspects and questions,
motivated by the goal to describe the encountered physics from first
principles. The state-of-the-art methodology to approach realistic many-body
effects in strongly correlated oxides, the combination of density functional
theory with dynamical mean-field theory, will be briefly introduced. Discussed
examples deal with prominent Mott-band- and band-band-insulating type of oxide
heterostructures, where different electronic characteristics may be stabilized
within a single architectured oxide material.Comment: 19 pages, 9 figure
Complex spectral evolution in a BCS superconductor, ZrB12
We investigate the electronic structure of a complex conventional superconductor, ZrB12 employing high resolution photoemission spectroscopy and ab initio band structure calculations. The experimental valence band spectra could be described reasonably well within the local density approximation. Energy bands close to the Fermi level possess t2g symmetry and the Fermi level is found to be in the proximity of quantum fluctuation regime. The spectral lineshape in the high resolution spectra is complex exhibiting signature of a deviation from Fermi liquid behavior. A dip at the Fermi level emerges above the superconducting transition temperature that gradually grows with the decrease in temperature. The spectral simulation of the dip and spectral lineshape based on a phenomenological self energy suggests finite electron pair lifetime and a pseudogap above the superconducting transition temperature
Screening of suitable cationic dopants for solar absorber material CZTS/Se: A first principles study
The earth abundant and non-toxic solar absorber material kesterite Cu2ZnSn(S/Se)(4) has been studied to achieve high power conversion efficiency beyond various limitations, such as secondary phases, antisite defects, band gap adjustment and microstructure. To alleviate these hurdles, we employed screening based approach to find suitable cationic dopant that can promote the current density and the theoretical maximum upper limit of the energy conversion efficiency (P(%)) of CZTS/Se solar devices. For this task, the hybrid functional (Heyd, Scuseria and Ernzerhof, HSE06) were used to study the electronic and optical properties of cation (Al, Sb, Ga, Ba) doped CZTS/Se. Our in-depth investigation reveals that the Sb atom is suitable dopant of CZTS/CZTSe and also it has comparable bulk modulus as of pure material. The optical absorption coefficient of Sb doped CZTS/Se is considerably larger than the pure materials because of easy formation of visible range exciton due to the presence of defect state below the Fermi level, which leads to an increase in the current density and P(%). Our results demonstrate that the lower formation energy, preferable energy gap and excellent optical absorption of the Sb doped CZTS/Se make it potential component for relatively high efficient solar cells
Universality of pseudogap and emergent order in lightly doped Mott insulators
It is widely believed that high-temperature superconductivity in the cuprates
emerges from doped Mott insulators. The physics of the parent state seems
deceivingly simple: The hopping of the electrons from site to site is
prohibited because their on-site Coulomb repulsion U is larger than the kinetic
energy gain t. When doping these materials by inserting a small percentage of
extra carriers, the electrons become mobile but the strong correlations from
the Mott state are thought to survive; inhomogeneous electronic order, a
mysterious pseudogap and, eventually, superconductivity appear. How the
insertion of dopant atoms drives this evolution is not known, nor whether these
phenomena are mere distractions specific to hole-doped cuprates or represent
the genuine physics of doped Mott insulators. Here, we visualize the evolution
of the electronic states of (Sr1-xLax)2IrO4, which is an effective spin-1/2
Mott insulator like the cuprates, but is chemically radically different. Using
spectroscopic-imaging STM, we find that for doping concentration of x=5%, an
inhomogeneous, phase separated state emerges, with the nucleation of pseudogap
puddles around clusters of dopant atoms. Within these puddles, we observe the
same glassy electronic order that is so iconic for the underdoped cuprates.
Further, we illuminate the genesis of this state using the unique possibility
to localize dopant atoms on topographs in these samples. At low doping, we find
evidence for much deeper trapping of carriers compared to the cuprates. This
leads to fully gapped spectra with the chemical potential at mid-gap, which
abruptly collapse at a threshold of around 4%. Our results clarify the melting
of the Mott state, and establish phase separation and electronic order as
generic features of doped Mott insulators.Comment: This version contains the supplementary information and small updates
on figures and tex
Satellites and large doping- and temperature-dependence of electronic properties in hole-doped BaFe2As2
Over the last years, superconductivity has been discovered in several
families of iron-based compounds. Despite intense research, even basic
electronic properties of these materials, such as Fermi surfaces, effective
electron masses, or orbital characters are still subject to debate. Here, we
address an issue that has not been considered before, namely the consequences
of dynamical screening of the Coulomb interactions among Fe-d electrons. We
demonstrate its importance not only for correlation satellites seen in
photoemission spectroscopy, but also for the low-energy electronic structure.
From our analysis of the normal phase of BaFe2As2 emerges the picture of a
strongly correlated compound with strongly doping- and temperature-dependent
properties. In the hole overdoped regime, an incoherent metal is found, while
Fermi-liquid behavior is recovered in the undoped compound. At optimal doping,
the self-energy exhibits an unusual square-root energy dependence which leads
to strong band renormalizations near the Fermi level
Small Polarons in Transition Metal Oxides
The formation of polarons is a pervasive phenomenon in transition metal oxide
compounds, with a strong impact on the physical properties and functionalities
of the hosting materials. In its original formulation the polaron problem
considers a single charge carrier in a polar crystal interacting with its
surrounding lattice. Depending on the spatial extension of the polaron
quasiparticle, originating from the coupling between the excess charge and the
phonon field, one speaks of small or large polarons. This chapter discusses the
modeling of small polarons in real materials, with a particular focus on the
archetypal polaron material TiO2. After an introductory part, surveying the
fundamental theoretical and experimental aspects of the physics of polarons,
the chapter examines how to model small polarons using first principles schemes
in order to predict, understand and interpret a variety of polaron properties
in bulk phases and surfaces. Following the spirit of this handbook, different
types of computational procedures and prescriptions are presented with specific
instructions on the setup required to model polaron effects.Comment: 36 pages, 12 figure
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