arXiv subjects

J. M. Pruneda

Publications and source records attributed to J. M. Pruneda.

17 recordsLinked to original sources

arXiv2012

Ab initio study of helium and hydrogen interactions in $α$-Fe

Density Functional Theory (DFT) calculations show a weak interaction between hydrogen and helium in iron, in contrast to previous reports of a strong trapping of hydrogen at helium. The strong preference of He and H to occupy regions with low electronic density (such as vacancies) explains this discrepancy, with vacancy-He and vacancy-H binding forces concealing the repulsive interaction between He and H. Furthermore, Rate Theory simulations based on our DFT-calculated V$_n$He$_m$H$_p$ cluster energetics predict, as it is observed in some experiments, that synergetic effects could be expected between H and He in iron under irradiation.

cond-mat.mtrl-sci↗

arXiv2012

One-dimensional half-metallic interfaces of two-dimensional honeycomb insulators

We study zigzag interfaces between insulating compounds that are isostructural to graphene, specifically II-VI, III-V and IV-IV two-dimensional (2D) honeycomb insulators. We show that these one-dimensional interfaces are polar, with a net density of excess charge that can be simply determined by using the ideal (integer) formal valence charges, regardless of the predominant covalent character of the bonding in these materials. We justify this finding on fundamental physical grounds, by analyzing the topology of the formal polarization lattice in the parent bulk materials. First principles calculations elucidate an electronic compensation mechanism not dissimilar to oxide interfaces, which is triggered by a Zener-like charge transfer between interfaces of opposite polarity. In particular, we predict the emergence of one dimensional electron and hole gases (1DEG), which in some cases are ferromagnetic half-metallic.

cond-mat.mes-hall↗

arXiv2012

Electrochemical ferroelectric switching: The origin of polarization reversal in ultrathin films

Against expectations, robust switchable ferroelectricity has been recently observed in ultrathin (1 nm) ferroelectric films exposed to air [V. Garcia $et$ $al.$, Nature {\bf 460}, 81 (2009)]. Based on first-principles calculations, we show that the system does not polarize unless charged defects or adsorbates form at the surface. We propose electrochemical processes as the most likely origin of this charge. The ferroelectric polarization of the film adapts to the bound charge generated on its surface by redox processes when poling the film. This, in turn, alters the band alignment at the bottom electrode interface, explaining the observed tunneling electroresistance. Our conclusions are supported by energetics calculated for varied electrochemical scenarios.

cond-mat.mes-hall↗

arXiv2011

Native defects in hybrid C/BN nanostructures

First-principles calculations of substitutional defects and vacancies are performed for zigzag-edged hybrid C/BN nanosheets and nanotubes which recently have been proposed to exhibit half-metallic properties. The formation energies show that defects form preferentially at the interfaces between graphene and BN domains rather than in the middle of these domains, and that substitutional defects dominate over vacancies. Chemical control can be used to favor localization of defects at C- B interfaces (nitrogen-rich environment) or C-N interfaces (nitrogen-poor environment). Although large defect concentrations have been considered here (106 cm-1), half-metallic properties can subsist when defects are localized at the C-B interface and for negatively charged defects localized at the C- N interface, hence the promising magnetic properties theoretically predicted for these zigzag-edged nanointerfaces might not be destroyed by point defects if these are conveniently engineered during synthesis.

cond-mat.mtrl-sci↗

arXiv2010

Origin of half-semimetallicity induced at interfaces of C-BN heterostructures

First-principles density functional calculations are performed in C-BN heterojunctions. It is shown that the magnetism of the edge states in zigzag shaped graphene strips and polarity effects in BN strips team up to give a spin asymmetric screening that induces half-semimetallicity at the interface, with a gap of at least a few tenths of eV for one spin orientation and a tiny gap of hundredths of eV for the other. The dependence with ribbon widths is discussed, showing that a range of ribbon widths is required to obtain half-semimetallicity. These results open new routes for tuning electronic properties at nanointerfaces and exploring new physical effects similar to those observed at oxide interfaces, in lower dimensions.

cond-mat.mtrl-sci↗

arXiv2009

He-LiF surface potential from fast atom diffraction under grazing incidence

Diffraction patterns produced by grazing scattering of fast atoms from insulator surfaces are used to examine the atom-surface interaction. The method is applied to He atoms colliding with a LiF(001) surface along axial crystallographic channels. The projectile-surface potential is obtained from an accurate DFT calculation, which includes polarization and surface relaxation. For the description of the collision process we employ the surface eikonal approximation, which takes into account quantum interference between different projectile paths. The dependence of projectile spectra on the parallel and perpendicular incident energies is experimentally and theoretically analyzed, determining the range of applicability of the proposed model.

cond-mat.other↗

arXiv2008

Nonadiabatic wavepacket dynamics: k-space formulation

The time evolution of wavepackets in crystals in the presence of a homogeneous electric field is formulated in k-space in a numerically tractable form. The dynamics is governed by separate equations for the motion of the waveform in k-space and for the evolution of the underlying Bloch-like states. A one-dimensional tight-binding model is studied numerically, and both Bloch oscillations and Zener tunneling are observed. The long-lived Bloch oscillations of the wavepacket center under weak fields are accompanied by oscillations in its spatial spread. These are analyzed in terms of a k-space expression for the spread having contributions from both the quantum metric and the Berry connection of the Bloch states. We find that when sizeable spread oscillations do occur, they are mostly due to the latter term.

cond-mat.mtrl-sci↗

arXiv2008

Understanding the Unique Structural and Electronic Properties of SrFeO2

We report a first-principles study of SrFeO$_2$, an infinite-layer oxide with Fe atoms in a perfect square-planar coordination down to essentially 0 K. Our results reveal this striking behavior relies on the double occupation of the 3$d_{z^2}$ orbitals of high-spin Fe$^{2+}$. Such an electronic state results from the hybridization of iron's 3$d_{z^2}$ and 4$s$ orbitals, which enables a large reduction of the intra-atomic exchange splitting of the $z^2$ electrons. The generality of the phenomenon is discussed.

cond-mat.mtrl-sci↗

arXiv2007

Electronic stopping power in insulators from first principles

Using time-dependent density-functional theory we calculate from first principles the rate of energy transfer from a moving proton or antiproton to the electrons of an insulating material, LiF. The behavior of the electronic stopping power versus projectile velocity displays an effective threshold velocity of ~0.2 a.u. for the proton, consistent with recent experimental observations, and also for the antiproton. The calculated proton/antiproton stopping-power ratio is ~2.4 at velocities slightly above the threshold (v~0.4 a.u.), as compared to the experimental value of 2.1. The projectile energy loss mechanism is observed to be stationary and extremely local.

cond-mat.mtrl-sci↗

arXiv2007

Ferrodistortive instability at the (001) surface of half-metallic manganites

We present the structure of the fully relaxed (001) surface of the half-metallic manganite La0.7Sr0.3MnO3, calculated using density functional theory within the generalized gradient approximation (GGA). Two relevant ferroelastic order parameters are identified and characterized: The tilting of the oxygen octahedra, which is present in the bulk phase, oscillates and decreases towards the surface, and an additional ferrodistortive Mn off-centering, triggered by the surface, decays monotonically into the bulk. The narrow d-like energy band that is characteristic of unrelaxed manganite surfaces is shifted down in energy by these structural distortions, retaining its uppermost layer localization. The magnitude of the zero-temperature magnetization is unchanged from its bulk value, but the effective spin-spin interactions are reduced at the surface.

cond-mat.mtrl-sci↗

arXiv2005

Density functionals and half-metalicity in La2/3Sr1/3MnO3

The electronic structure and equilibrium geometry of La2/3Sr1/3MnO3 are studied theoretically by means of density functional calculations. The doping is treated by introducing holes and a compensating jellium background. The results for the local density approximation (LDA) agree with previous LDA calculations, with an equilibrium volume 5.3% too small and with both majority and minority spin states present at the Fermi level for the relaxed system. The generalised gradient approximation (GGA) offers a qualitatively improved description of the system, with a more realistic volume, and a half-metallic behaviour for the relaxed structure, which enables studies needing theoretical relaxation.The ideal MnO2-terminated (001) surface is then described with explicit doping.

cond-mat.mtrl-sci↗

arXiv2005

First-principles study of structural, elastic, and bonding properties of pyrochlores

Density Functional Theory calculations have been performed to obtain lattice parameters, elastic constants, and electronic properties of ideal pyrochlores with the composition A$_2$B$_2$O$_7$ (where A=La,Y and B=Ti,Sn,Hf, Zr). Some thermal properties are also inferred from the elastic properties. A decrease of the sound velocity (and thus, of the Debye temperature) with the atomic mass of the B ion is observed. Static and dynamical atomic charges are obtained to quantify the degree of covalency/ionicity. A large anomalous contribution to the dynamical charge is observed for Hf, Zr, and specially for Ti. It is attributed to the hybridization between occupied $2p$ states of oxygen and unoccupied d states of the B cation. The analysis based on Mulliken population and deformation charge integrated in the Voronoi polyhedra indicates that the ionicity of these pyrochlores increases in the order Sn--Ti--Hf--Zr. The charge deformation contour plots support this assignment.

cond-mat.mtrl-sci↗

arXiv2004

Energetics of intrinsic point defects in ZrSiO$_4$

Using first principles calculations we have studied the formation energies, electron and hole affinities, and electronic levels of intrinsic point defects in zircon. The atomic structures of charged interstitials, vacancies, Frenkel pairs and anti-site defects are obtained. The limit of high concentration of point defects, relevant for the use of this material in nuclear waste immobilization, was studied with a variable lattice relaxation that can simulate the swelling induced by radiation damage. The limit of low concentration of defects is simulated with larger cells and fixed lattice parameters. Using known band offset values at the interface of zircon with silicon, we analyze the foreseeable effect of the defects on the electronic properties of zircon used as gate in metal-oxide-semiconductor devices.

cond-mat.mtrl-sci↗

arXiv2004

First principles simulations of the magnetic and structural properties of Iron

We have implemented non-collinear GGA and a generalized Bloch's theorem to simulate unconmensurate spiral arrangements of spins in a Density Functional Theory code based on localized wave functions. We have subsequently performed a thorough study of the different states of bulk Iron. We determine the minimal basis set required to obtain reliable orderings of ground and excited states. We find that the most stable fcc phase is a spiral with an equilibrium lattice constant 3.56 A.

cond-mat.mtrl-sci↗

arXiv2004

Short range repulsive interatomic interactions in energetic processes in solids

The repulsive interaction between two atoms at short distances is studied in order to explore the range of validity of standard first-principles simulation techniques and improve the available short-range potentials for the description of energetic collision cascades in solids. Pseudopotentials represent the weakest approximation, given their lack of explicit Pauli repulsion in the core-core interactions. The energy (distance) scale realistically accessible is studied by comparison with all-electron reference calculations in some binary systems. Reference calculations are performed with no approximations related to either core (frozen core, augmentation spheres) or basis set. This is important since the validity of such approximations, even in all-electron calculations, rely on the small core perturbation usual in low-energy studies. The expected importance of semicore states is quantified. We propose a scheme for improving the electronic screening given by pseudopotentials for very short distances. The results of this study are applied to the assessment and improvement of existing repulsive empirical potentials.

cond-mat.mtrl-sci↗

arXiv2004

Intrinsic point defects and volume swelling in ZrSiO4 under irradiation

The effects of high concentration of point defects in crystalline ZrSiO4 as originated by exposure to radiation, have been simulated using first principles density functional calculations. Structural relaxation and vibrational studies were performed for a catalogue of intrinsic point defects, with different charge states and concentrations. The experimental evidence of a large anisotropic volume swelling in natural and artificially irradiated samples is used to select the subset of defects that give similar lattice swelling for the concentrations studied, namely interstitials of O and Si, and the anti-site Zr(Si), Calculated vibrational spectra for the interstitials show additional evidence for the presence of high concentrations of some of these defects in irradiated zircon.

cond-mat.mtrl-sci↗

arXiv2001

ab inito local vibrational modes of light impurities in silicon

We have developed a formulation of density functional perturbation theory for the calculation of vibrational frequencies in molecules and solids, which uses numerical atomic orbitals as a basis set for the electronic states. The (harmonic) dynamical matrix is extracted directly from the first order change in the density matrix with respect to infinitesimal atomic displacements from the equilibrium configuration. We have applied this method to study the vibrational properties of a number of hydrogen-related complexes and light impurities in silicon. The diagonalization of the dynamical matrix provides the vibrational modes and frequencies, including the local vibrational modes (LVMs) associated with the defects. In addition to tests on simple molecules, results for interstitial hydrogen, hydrogen dimers, vacancy-hydrogen and self-interstitial-hydrogen complexes, the boron-hydrogen pair, substitutional C, and several O-related defects in c-Si are presented. The average error relative to experiment for the aprox.60 predicted LVMs is about 2% with most highly harmonic modes being extremely close and the more anharmonic ones within 5-6% of the measured values.

cond-mat.mtrl-sci↗