arXiv subjects

Vincenzo Fiorentini

Publications and source records attributed to Vincenzo Fiorentini.

At least 37 records · Page 2Linked to original sources

arXiv2014

Impurity-vacancy complexes and ferromagnetism in doped sesquioxides

Based on hybrid density-functional calculations, we propose that ferromagnetism in the prototypical bixbyite sesquioxide In$_2$O$_3$ doped with Cr is due to Cr-oxygen vacancy complexes, while isolated Cr cannot support carrier-mediated magnetic coupling. Our proposal is consistent with experimental facts such as the onset of ferromagnetism in O-lean conditions only, the low or vanishing net moment in unintentionally doped material, and its increase upon intentional doping.

cond-mat.mtrl-sci↗

arXiv2013

Giant electroresistance and tunable magnetoelectricity in a multiferroic junction

First-principles density functional calculations show that the $\textrm{SrRuO}_{3}/\textrm{PbTiO}_{3}/\textrm{SrRuO}_{3}$ multiferroic junction with asymmetric (RuO$_{2}$/PbO and TiO$_{2}$/SrO) interfaces has a large ferroelectric depolarizing field, whose switching changes the interface transmission probabilities for tunneling electrons, leading to electroresistance modulation over several orders of magnitude. The switching further affects the interface spin density, naturally driving magnetoresistance as well as modulated spin-dependent in-plane resistivity, which may be exploited in field-effect devices.

cond-mat.mtrl-sci↗

arXiv2013

Multiferroicity in V-doped PbTiO$_{3}$

We report \emph{ab initio} predictions on the proper multiferroic (ferromagnetic, insulating and ferroelectric) character of PbTiO$_{3}$ doped with vanadium. V impurities coupled ferromagnetically carry a magnetization of 1 $μ_{\rm B}$ each. The coupling is expected to be strong, since the paramagnetic solution is higher by 150 meV/vanadium, and no stable antiferromagnetic solution was found. The electronic gap in the doped system is about 0.2-0.3 eV in GGA, hence the system is properly multiferroic. V doping increases the spontaneous polarization in PbTiO$_{3}$, with an approximate percentual rate of 0.7 $μ$C/cm$^{2}$.

cond-mat.mtrl-sci↗

arXiv2013

Doping-dependent band structure of LaAlO$_{3}$/SrTiO$_{3}$ interfaces by soft x-ray polarization-controlled resonant angle-resolved photoemission

Polarization-controlled synchrotron radiation was used to map the electronic structure of buried conducting interfaces of LaAlO$_3$/SrTiO$_3$ in a resonant angle-resolved photoemission experiment. A strong dependence on the light polarization of the Fermi surface and band dispersions is demonstrated, highlighting the distinct Ti 3d orbitals involved in 2D conduction. Samples with different 2D doping levels were prepared and measured by photoemission, revealing different band occupancies and Fermi surface shapes. A direct comparison between the photoemission measurements and advanced first-principle calculations carried out for different 3d-band fillings is presented in conjunction with the 2D carrier concentration obtained from transport measurements.

cond-mat.str-el↗

arXiv2013

Surface antiferromagnetism and incipient metal-insulator transition in strained manganite films

Using first-principles calculations, we show that the (001) surface of the ferromagnet La$_{1-x}$Sr$_{x}$MnO$_{3}$ under epitaxial compression favors antiferromagnetic ordering in the first few surface layers, coexisting with ferromagnetic bulk order. The change in magnetic order is accompanied by a marked surface-related spectral pseudogap, signaling a metal-insulator near-transition at the surface. All surfaces exhibit huge outward relaxations an rumpling of the MnO$_{2}$ and LaO surface planes, causing a distinct shift in work function. The AF phase is an extreme surface-assisted case of the combination of in-plane AF super-exchange and vertical FM double-exchange couplings that rules magnetism in manganites under in-plane compression.

cond-mat.mtrl-sci↗

arXiv2012

Ordering and multiple phase transitions in ultra-thin nickelate superlattices

We interpret via advanced ab initio calculations the multiple phase transitions observed recently in ultra-thin LaNiO$_{3}$/LaAlO$_{3}$ superlattices. The ground state is insulating, charge-ordered, and antiferromagnetic due to concurrent structural distortion and weak valency disproportionation. We infer distinct transitions at 40 K and 150 K, respectively, from antiferromagnetic order to moment disorder, and from structurally-dimerized insulator to an undistorted metallic Pauli paramagnet (exhibiting a cuprate-like Fermi surface). The results are in satisfactory agreement with experiment.

cond-mat.mtrl-sci↗

arXiv2012

Ferromagnetism and orbital order in a topological ferroelectric

We explore via density functional calculations the magnetic doping of a topological ferroelectric as an unconventional route to multiferroicity. Vanadium doping of the layered perovskite La$_{2}$Ti$_{2}$O$_{7}$ largely preserves electric polarization and produces robust ferromagnetic order, hence proper multiferroicity. The marked tendency of dopants to cluster into chains results in an insulating character at generic doping. Ferromagnetism stems from the symmetry breaking of the multi-orbital V system via an unusual "antiferro"-orbital order, and from the host's low-symmetry layered structure.

cond-mat.mtrl-sci↗

arXiv2009

Fermi-surface pockets in magnetic underdoped cuprates from first principles

Using an innovative first-principles band theory enabling the exploration of Mott-insulating magnetic cuprates, we study the Fermi surface of underdoped Y$_{1-x}$Ca$_x$Ba$_2$Cu$_3$O$_6$ in a selection of magnetically ordered and polaronic states. All phases exhibit qualitatively similar, hole-like nodal-point small pockets. Their properties (area, masses, mass sign) only partially match those extracted from recent quantum-oscillation experiments. Ab initio calculations, therefore, do not straightforwardly support a magnetic origin of quantum oscillations.

cond-mat.supr-con↗

arXiv2009

Fermi-surface pockets in $YBa_2Cu_3O_{6.5}$ : A comparison of ab initio techniques

We study the Fermi surface of metallic, non-magnetic \textit{ortho}-II YBa$_2$Cu$_3$O$_{6.5}$ using three different density-functional-based band-structure techniques (GGA, GGA+U, PSIC). The calculated Fermi surface exhibits no pockets in GGA+U and PSIC, a minor one in GGA. Upon shifting the Fermi level in the vicinity of the calculated value, we instead observe several pocket structures. We calculate their cross-sectional areas and cyclotron masses. Overall, our calculations show no solid evidence of the existence of electron-like --nor, in fact, of any-- Fermi surface pockets in this phase. This suggests that the origin of the pockets should be sought for in other, different phases.

cond-mat.supr-con↗

arXiv2008

Chain metallicity and antiferro-paramagnetism competition in underdoped YBa$_2$Cu$_3$O$_{6+x}$: a first principles description

We describe from advanced first principles calculations the energetics of oxygen doping and its relation to insulator-metal transitions in underdoped YBa$_2$Cu$_3$O$_{6+x}$. We find a strong tendency of doping oxygens to order into non-magnetic Cu$^{1+}$O$_x$ chains at any $x$. Ordering produces one-dimensional metallic bands, while configurations with non-aligned oxygens are insulating. The Cu$^{2+}$O$_2$ planes remain insulating and antiferromagnetic up to a threshold between $x$=0.25 and 0.5, above which a paramagnetic normal-metal state prevails. The in-plane antiferro-paramagnetic competition depends on $x$, but only weakly on the ordering state of the chains.

cond-mat.supr-con↗

arXiv2008

Dielectric constant boost in amorphous sesquioxides

High-kappa dielectrics for insulating layers are a current key ingredient of microelectronics. X2O3 sesquioxide compounds are among the candidates. Here we show for a typical material of this class, ScO3, that the relatively modest dielectric constant of its crystalline phase is enhanced in the amorphous phase by over 40% (from ~15 to ~22). This is due to the disorder-induced activation of low frequency cation-related modes which are inactive or inefficient in the crystal, and by the conservation of effective dynamical charges (a measure of atomic polarizability). The analysis employs density-functional energy-force and perturbation-theory calculations of the dielectric response of amorphous samples generated by pair-potential molecular dynamics.

cond-mat.mtrl-sci↗

arXiv2008

Ab-initio description of hole localization and Zhang-Rice singlets in one-dimensional doped cuprates

We present the first ab-initio band-theory-based description of spin-compensated polarons (known as Zhang-Rice singlets) in a hole-doped cuprate, specifically one-dimensional Ca_{2+x} Y_{2-x} Cu_5 O_10. Zhang-Rice singlets are many-particle configurations relevant to the exotic behavior of hole-doped cuprates, stemming from spontaneous charge localization. They appear in our case-study material above a threshold doping, successively turning the insulating undoped antiferromagnet into a gap insulator, a singlet-rich metallic paramagnet, and finally, a singlet-saturated insulating diamagnet.

cond-mat.str-el↗

arXiv2008

Conservation of dielectric constant upon amorphization in perovskite oxides

We report calculations indicating that amorphous RAO$_3$ oxides, with R and A trivalent cations, have approximately the same static dielectric constant as their perovskite crystal phase. The effect is due to the disorder-activated polar response of non-polar crystal modes at low frequency, which compensates a moderate but appreciable reduction of the ionic dynamical charges. The dielectric response was studied via density-functional perturbation theory. Amorphous samples were generated by molecular dynamics melt-and-quench simulations.

cond-mat.mtrl-sci↗

arXiv2001

Non-linear macroscopic polarization in III-V nitride alloys

We study the dependence of macroscopic polarization on composition and strain in wurtzite III-V nitride ternary alloys using ab initio density-functional techniques. The spontaneous polarization is characterized by a large bowing, strongly dependent on the alloy microscopic structure. The bowing is due to the different response of the bulk binaries to hydrostatic pressure, and to internal strain effects (bond alternation). Disorder effects are instead minor. Deviations from parabolicity (simple bowing) are of order 10 % in the most extreme case of AlInN alloy, much less at all other compositions. Piezoelectric polarization is also strongly non-linear. At variance with the spontaneous component, this behavior is independent of microscopic alloy structure or disorder effects, and due entirely to the non-linear strain dependence of the bulk piezoelectric response. It is thus possible to predict the piezoelectric polarization for any alloy composition using the piezoelectricity of the parent binaries.

cond-mat.mtrl-sci↗

arXiv2000

Proof of the thermodynamical stability of the E' center in SiO2

The E' center is a paradigmatic radiation-induced defect in SiO2 whose peculiar EPR and hyperfine activity has been known since over 40 years. This center has been traditionally identified with a distorted, positively-charged oxygen vacancy V_O+. However, no direct proof of the stability of this defect has ever been provided, so that its identification is still strongly incomplete. Here we prove directly that distorted V_O+ is metastable and that it satisfies the key requirements for its identification as E', such as thermal and optical response, and activation-deactivation mechanisms.

cond-mat.mtrl-sci↗

arXiv2000

Band offsets and stability of BeTe/ZnSe (100) heterojunctions

We present ab-initio studies of band offsets, formation energy, and stability of (100) heterojunctions between (Zn,Be)(Se,Te) zincblende compounds, and in particular of the lattice-matched BeTe/ZnSe interface. Equal band offsets are found at Be/Se and Zn/Te abrupt interfaces, as well as at mixed interfaces, in agreement with the established understanding of band offsets at isovalent heterojunctions. Thermodynamical arguments suggest that islands of non-nominal composition may form at the interface, causing offset variations over about 0.8 eV depending on growth conditions. Our findings reconcile recent experiments on BeTe/ZnSe with the accepted theoretical description.

cond-mat.mtrl-sci↗

arXiv1999

Theory and applications of the stress density

Drawing on the theory of quantum mechanical stress, we introduce the stress density in density functional theory. In analogy with the Chetty-Martin energy density, the stress density provides a spatial resolution of the contributions to the integrated macroscopic stress tensor. We give specific prescriptions for a practical and efficient implementation in the plane wave ultrasoft pseudopotential method within the local-density approximation. We demonstrate the abilities of the stress density studying a set of representative test cases from surface and interface physics. In perspective, the stress density emerges as vastly more powerful and predictive than the integrated macroscopic stress.

cond-mat.mtrl-sci↗

arXiv1999

Spontaneous vs. piezoelectric polarization in III-V nitrides: conceptual aspects and practical consequences

Macroscopic polarization plays a major role in determining the optical and electrical properties of nitride nanostructures via polarization-induced built-in electrostatic fields. While currently fashionable, this field of endeavour is still by far in its early infancy. Here we contribute some clarifications on the conceptual issues involved in determining built-in fields in III-V nitride nanostructures, sorting out in particular the roles of spontaneous and piezoelectric polarization.

cond-mat.mtrl-sci↗