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S. Picozzi

Publications and source records attributed to S. Picozzi.

36 records · Page 2Linked to original sources
arXiv2011

Ferroelectricity due to orbital ordering in E-type undoped rare-earth manganites

Aiming at understanding the origin of the electronic contribution to ferroelectric polarization in undoped manganites, we evaluate the Berry phase of orbital-polarizable Bloch electrons as an orbital ordering (OO) establishes in the background of an antiferromagnetic E-type configuration. The onset of OO is tuned by the Jahn-Teller (JT) interaction in a tight-binding model for interacting electrons moving along zigzag chains. A finite polarization is found as soon as the JT coupling is strong enough to induce OO, supporting the large electronic contribution predicted from first principles.

cond-mat.str-el↗
arXiv2010

CdV2O4: A rare example of a collinear multiferroic spinel

By studying the dielectric properties of the geometrically frustrated spinel CdV2O4, we observe ferroelectricity developing at the transition into the collinear antiferromagnetic ground state. In this multiferroic spinel, ferroelectricity is driven by local magnetostriction and not by the more common scenario of spiral magnetism. The experimental findings are corroborated by ab-initio calculations of the electric polarization and the underlying spin and orbital order. The results point towards a charge rearrangement due to dimerization, where electronic correlations and the proximity to the insulator-metal transition play an important role.

cond-mat.str-el↗
arXiv2010

Hybrid functional study of proper and improper multiferroics

We present a detailed study of the structural, electronic, magnetic and ferroelectric properties of prototypical \textit{proper} and \textit{improper} multiferroic (MF) systems such as BiFeO$_{3}$ and orthorhombic HoMnO$_{3}$, respectively, within density functional theory (DFT) and using the Heyd-Scuseria-Ernzerhof hybrid functional (HSE). By comparing our results with available experimental data as well as with state-of-the-art GW calculations, we show that the HSE formalism is able to account well for the relevant properties of these compounds and it emerges as an accurate tool for predictive first-principles investigations on multiferroic systems. We show that effects beyond local and semilocal DFT approaches (as provided by HSE) are necessary for a realistic description of MFs. For the electric polarization, a decrease is found for MFs with magnetically-induced ferroelectricity, such as HoMnO$_3$, where the calculated polarization changes from $\sim$ 6 $μ C/cm^2$ using Perdew-Burke-Ernzerhof (PBE) to $\sim$ 2 $μ C/cm^2$ using HSE. However, for \textit{proper} MFs, such as BiFeO$_{3}$, the polarization slightly increases upon introduction of exact exchange. Our findings therefore suggest that a general trend for the HSE correction to bare density functional cannot be extracted; rather, a specific investigation has to be carried out on each compound.

cond-mat.mtrl-sci↗
arXiv2007

Magneto-optical properties of (Ga,Mn)As: an ab--initio determination

The magneto-optical properties of (Ga,Mn)As have been determined within density functional theory using the highly precise full-potential linear augmented plane wave (FLAPW) method. A detailed investigation of the electronic and magnetic properties in connection to the magneto-optic effects is reported. The spectral features of the optical tensor in the 0-10 eV energy range are analyzed in terms of the band structure and density of states and the essential role of the dipole matrix elements is highlighted by means of Brillouin zone dissection. Using an explicit representation of the Kerr angle in terms of real and imaginary parts of the tensor components, a careful analysis of the Kerr spectra is also presented. The results of our study can be summarized as follows: i) different types of interband transitions do contribute in shaping the conductivity tensor; ii) the dipole matrix elements are important in obtaining the correct optical spectra; iii) different regions in the irreducible Brillouin zone contribute to the conductivity very differently; iv) a minimum in the Re $σ_{xx}$ spectra can give rise to a large Kerr rotation angle in the same energy region; and v) materials engineering via the magneto-optical Kerr effect is possible provided that the electronic structure of the material can be tuned in such a way as to \emph{enhance} the depth of the minima of Re $σ_{xx}$.

cond-mat.mtrl-sci↗
arXiv2007

Optical and magneto-optical properties of ferromagnetic full-Heusler films: experiments and first-principles calculations

We report a joint theoretical and experimental study focused on understanding the optical and magneto-optical properties of Co-based full-Heusler compounds. We show that magneto-optical spectra calculated within ab-initio density functional theory are able to uniquely identify the features of the experimental spectra in terms of spin resolved electronic transitions. As expected for 3d-based magnets, we find that the largest Kerr rotation for these alloys is of the order of 0.3o in polar geometry. In addition, we demonstrate that (i) multilayered structures have to be carefully handled in the theoretical calculations in order to improve the agreement with experiments, and (ii) combined theoretical and experimental investigations constitute a powerful approach to designing new materials for magneto-optical and spin-related applications

cond-mat.mtrl-sci↗
arXiv2006

First-principles stabilization of an unconventional collinear magnetic ordering in distorted manganites

First-principles calculations have been performed for different collinear magnetic orderings in orthorhombic manganites, such as HoMnO3, TbMnO3 and YMnO3, showing large GdFeO3-like distortions. Our results suggest that the AFM-E type ordering, experimentally observed in HoMnO3 and recently proposed from model hamiltonian studies as a potentially novel phase, is indeed the magnetic ground state. Its stability is strongly connected with octahedral distortions and points to the relevance of structural more than chemical effects. The calculated exchange constants, extracted from a Heisenberg model used to fit the first-principles total energies, show that the ferromagnetic in-plane nearest-neighbour coupling is reduced compared to less-distorted manganites, such as LaMnO3. In parallel, the antiferromagnetic next-nearest-neighbour coupling along planar Mn-O-O-Mn paths in highly-distorted manganites plays a relevant role in the stabilization of the AFM-E spin configuration. In agreement with experiments, the density of states shows that this phase is insulating with an indirect band-gap of about 0.5 eV.

cond-mat.mtrl-sci↗
arXiv2006

Electronic structure and exchange constants in magnetic semiconductors digital alloys: chemical and band-gap effects

First-principles simulations have been performed for [001]-ordered Mn/Ge and Mn/GaAs "digital alloys", focusing on the effects of i) a larger band-gap and ii) a different semiconducting host on the electronic structure of the magnetic semiconductors of interest. Our results for the exchange constants in Mn/Ge, evaluated using a frozen-magnon scheme, show that a larger band-gap tends to give a stronger nearest-neighbor ferromagnetic coupling and an overall enhanced in-plane ferromagnetic coupling even for longer-ranged coupling constants. As for the chemical effects on the exchange constants, we show that Mn/GaAs shows a smaller nearest-neighbor ferromagnetic coupling than Mn/Ge, but exchange constants for higher Mn-Mn distance show an overall increased ferromagnetic behavior in Mn/GaAs. As a result, from the magnetic-coupling point of view, the two systems behave on average rather similarly.

cond-mat.mtrl-sci↗
arXiv2005

Magneto-optics in pure and defective Ga_{1-x}Mn_xAs from first-principles

The magneto-optical properties of Ga$_{1-x}$Mn$_{x}$As including their most common defects were investigated with precise first--principles density-functional FLAPW calculations in order to: {\em i}) elucidate the origin of the features in the Kerr spectra in terms of the underlying electronic structure; {\em ii}) perform an accurate comparison with experiments; and {\em iii}) understand the role of the Mn concentration and occupied sites in shaping the spectra. In the substitutional case, our results show that most of the features have an interband origin and are only slightly affected by Drude--like contributions, even at low photon energies. While not strongly affected by the Mn concentration for the intermediately diluted range ($x\sim$ 10%), the Kerr factor shows a marked minimum (up to 1.5$^o$) occurring at a photon energy of $\sim$ 0.5 eV. For interstitial Mn, the calculated results bear a striking resemblance to the experimental spectra, pointing to the comparison between simulated and experimental Kerr angles as a valid tool to distinguish different defects in the diluted magnetic semiconductors framework.

cond-mat.mtrl-sci↗
arXiv2004

First-principles characterization of ferromagnetic Mn5Ge3 for spintronic applications

In the active search for potentially promising candidates for spintronic applications, we focus on the intermetallic ferromagnetic Mn5Ge3 compound and perform accurate first-principles FLAPW calculations within density functional theory. Through a careful investigation of the bulk electronic and magnetic structure, our results for the total magnetization, atomic magnetic moments, metallic conducting character and hyperfine fields are found to be in good agreement with experiments, and are elucidated in terms of a hybridization mechanism and exchange interaction. In order to assess the potential of this compound for spin-injection purposes, we calculate Fermi velocities and degree of spin-polarization; our results predict a rather high spin-injection efficiency in the diffusive regime along the hexagonal c-axis. Magneto-optical properties, such as L_2,3 X-ray magnetic circular dichroism, are also reported and await comparison with experimental data.

cond-mat.mtrl-sci↗
arXiv2002

Accurate first principles detailed balance determination of Auger recombination and impact ionization rates in semiconductors

The technologically important problem of predicting Auger recombination lifetimes in semiconductors is addressed by means of a fully first--principles formalism. The calculations employ highly precise energy bands and wave functions provided by the full--potential linearized augmented plane wave (FLAPW) code based on the screened exchange local density approximation. The minority carrier Auger lifetime is determined by two closely related approaches: \emph{i}) a direct evaluation of the Auger rates within Fermi's Golden Rule, and \emph{ii}) an indirect evaluation, based on a detailed balance formulation combining Auger recombination and its inverse process, impact ionization, in a unified framework. Calculated carrier lifetimes determined with the direct and indirect methods show excellent consistency \emph{i}) between them for $n$-doped GaAs and \emph{ii}%) with measured values for GaAs and InGaAs. This demonstrates the validity and accuracy of the computational formalism for the Auger lifetime and indicates a new sensitive tool for possible use in materials performance optimization.

cond-mat.mtrl-sci↗
arXiv2001

Impact ionization in GaAs: a screened exchange density functional approach

Results are presented of a fully ab-initio calculation of impact ionization rates in GaAs within the density functional theory framework, using a screened-exchange formalism and the highly precise all-electron full-potential linearized augmented plane wave (FLAPW) method. The calculated impact ionization rates show a marked orientation dependence in {\bf k} space, indicating the strong restrictions imposed by the conservation of energy and momentum. This anisotropy diminishes as the impacting electron energy increases. A Keldysh type fit performed on the energy-dependent rate shows a rather soft edge and a threshold energy greater than the direct band gap. The consistency with available Monte Carlo and empirical pseudopotential calculations shows the reliability of our approach and paves the way to ab-initio calculations of pair production rates in new and more complex materials.

cond-mat.mtrl-sci↗
arXiv2001

Role of structural relaxations, chemical substitutions and polarization fields on the potential line-up in [0001] wurtzite GaN/Al systems

First-principles full-potential linearized augmented plane wave (FLAPW) calculations are performed to clarify the role of the interface geometry on piezoelectric fields and on potential line-ups at the [0001]-wurtzite and [111]-zincblende GaN/Al junctions. The electric fields (polarity and magnitude) are found to be strongly affected by atomic relaxations in the interface region. A procedure is tested to evaluate the Schottky barrier in the presence of electric fields and used to show that their effect is quite small (a few tenths of an eV). These calculations assess the rectifying behaviour of the GaN/Al contact, giving very good agreement with experimental values for the barrier. Stimulated by the complexity of the problem, we disentangle chemical and structural effects on the relevant properties (such as the potential discontinuity and electric fields) by studying auxiliary unrelaxed nitride/metal systems. Focusing on simple electronegativity arguments, we outline the leading mechanisms that result in the final values of the electric fields and Schottky barriers in these ideal interfaces. Finally, the transitivity rule in the presence of two inequivalent junctions is proved to give reliable results.

cond-mat.mtrl-sci↗
arXiv2001

Coordination and chemical effects on the structural, electronic and magnetic properties in Mn pnictides

Simple structures of MnX binary compounds, namely hexagonal NiAs and zincblende, are studied as a function of the anion (X = Sb, As, P) by means of the all-electron FLAPW method within local spin density and generalized gradient approximations. An accurate analysis of the structural, electronic and magnetic properties reveals that the cubic structure greatly favours the magnetic alignment in these compounds leading to high magnetic moments and nearly half-metallic behaviour for MnSb and MnAs. The effect of the anion chemical species is related to both its size and the possible hybridization with the Mn $d$ states; both contributions are seen to hinder the magnitude of the magnetic moment for small and light anions. Our results are in very good agreement with experiment - where available - and show that the generalized gradient approximation is essential to correctly recover both the equilibrium volume and magnetic moment.

cond-mat.mtrl-sci↗
arXiv2000

Metal induced gap states and Schottky barrier heights at non-reactive GaN/noble metal interfaces

We present ab-initio local density FLAPW calculations on non-reactive N-terminated [001] ordered GaN/Ag and GaN/Au interfaces and compare the results (such as metal induced gap states and Schottky barrier heights) with those obtained for GaN/Al, in order to understand the dependence of the relevant electronic properties on the deposited metal. Our results show that the density of gap states is appreciable only in the first semiconductor layer close to the interface. The decay length of the gap states in the semiconductor side is about 2.0 $\pm$ 0.1 Å$\:$ and is independent of the deposited metal, therefore being to a good extent a bulk property of GaN. Our calculated values of the Schottky barrier heights are $Φ_{B_p}(GaN/Ag)$ = 0.87 eV and $Φ_{B_p}(GaN/Au)$ = 1.08 eV; both values are smaller than the GaN/Al value ($Φ_{B_p}(GaN/Al)$ = 1.51 eV) and this quite large spread of values excludes the possibility of a Fermi level pinning within the GaN band gap. Because of the low screening in GaN, the potential barrier at the junction is strongly affected by the structural arrangement of the first metal layer at the interface. This leads to quite large variations of the Schottky barrier height as a function of the metal, in contrast with the behavior of GaAs/metal interfaces.

cond-mat.mtrl-sci↗
arXiv1998

Influence of the exchange reaction on the electronic structure of GaN/Al junctions

Ab-initio calculations have been used to study the influence of the interface morphology and, notably, of the exchange reaction on the electronic properties of Al/GaN (100) interfaces. In particular, the effects of interface structure (i.e. interfacial bond lengths, semiconductor surface polarity, and reacted intralayers) on the SBH at the Al/GaN (001) junction are specifically addressed. The electronic structure of the following atomic configurations have been investigated theoretically: (i) an abrupt, relaxed GaN/Al interface; (ii) an interface which has undergone one monolayer of exchange reaction; and interfaces with a monolayer-thick interlayer of (iii) AlN and (iv) Ga$_{0.5}$Al$_{0.5}$N. Intermixed interfaces are found to pin the interface Fermi level at a position not significantly different from that of an abrupt interface. Our calculations also show that the interface band line--up is not strongly dependent on the interface morphology changes studied. The p-type SBH is reduced by less than 0.1 eV if the GaN surface is Ga-terminated compared to the N-terminated one. Moreover, we show that both an ultrathin Ga$_x$Al$_{1-x}$N ($x$ = 0, 0.5) intralayer and a Ga$\leftrightarrow$Al atomic swap at the interface does not significantly affect the Schottky barrier height.

cond-mat.mtrl-sci↗
arXiv1997

Electric fields and valence band offsets at strained [111] heterojunctions

[111] ordered common atom strained layer superlattices (in particular the common anion GaSb/InSb system and the common cation InAs/InSb system) are investigated using the ab initio full potential linearized augmented plane wave (FLAPW) method. We have focused our attention on the potential line-up at the two sides of the homopolar isovalent heterojunctions considered, and in particular on its dependence on the strain conditions and on the strain induced electric fields. We propose a procedure to locate the interface plane where the band alignment could be evaluated; furthermore, we suggest that the polarization charges, due to piezoelectric effects, are approximately confined to a narrow region close to the interface and do not affect the potential discontinuity. We find that the interface contribution to the valence band offset is substantially unaffected by strain conditions, whereas the total band line-up is highly tunable, as a function of the strain conditions. Finally, we compare our results with those obtained for [001] heterojunctions.

cond-mat.mtrl-sci↗
arXiv1997

Influence of growth direction and strain conditions on the band line-up at GaSb/InSb and InAs/InSb interfaces

First-principles full potential linearized augmented plane wave (FLAPW) calculations have been performed for lattice-mismatched common-atom III-V interfaces. In particular, we have examined the effects of epitaxial strain and ordering direction on the valence band offset in [001] and [111] GaSb/InSb and InAs/InSb superlattices, and found that the valence band maximum is always higher at the InSb side of the heterojunction, except for the common-anion system grown on an InSb substrate. The comparison between equivalent structures having the same substrate lattice constant, but different growth axis, shows that for comparable strain conditions, the ordering direction slightly influences the band line-up, due to small differences of the charge readjustment at the [001] and [111] interfaces. On the other hand, strain is shown to strongly affect the VBO; in particular, as the pseudomorphic growth conditions are varied, the bulk contribution to the band line-up changes markedly, whereas the interface term is almost constant. On the whole, our calculations yield a band line-up that decreases linearly as the substrate lattice constant is increased, showing its high tunability as a function of different pseudomorphic growth conditions. Finally, the band line-up at the lattice matched InAs/GaSb interface determined using the transitivity rule gave perfect agreement between predicted and experimental results.

cond-mat.mtrl-sci↗
arXiv1997

Effects of epitaxial strain and ordering direction on the electronic properties of (GaSb)_1/(InSb)_1 and (InAs)_1/(InSb)_1 superlattices

The structural and electronic properties in common anion (GaSb)_1/(InSb)_1 and common cation (InAs)_1/(InSb)_1 [111] ordered superlattices have been determined using the local density total energy full potential linearized augmented plane wave method. The influence of the ordering direction, strain conditions and atomic substitution on the electronic properties of technological and experimental interest (such as energy band-gaps and charge carrier localization in the different sublattices) were determined. The results show an appreciable energy band-gap narrowing compared to the band-gap averaged over the constituent binaries, either in [001] ordered structures or (more markedly) in the [111] systems; moreover energy band-gaps show an increasing trend as the substrate lattice parameter is decreased. Finally, the systems examined offer interesting opportunities for band-gap tuning as a function of the growth condition (about 0.7 eV in (GaSb)_1/(InSb)_1 and 0.3 eV in (InAs)_1/(InSb)_1).

cond-mat.mtrl-sci↗