M. A. Marques - CEA-DEN

M. A. Marques
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M. A. Marques

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Physics - Materials Science (20)
High Energy Physics - Theory (12)
High Energy Physics - Phenomenology (6)
Physics - Chemical Physics (6)
Physics - Other (6)
Physics - Strongly Correlated Electrons (5)
Physics - Computational Physics (4)
Physics - Superconductivity (4)
General Relativity and Quantum Cosmology (3)
Physics - Mesoscopic Systems and Quantum Hall Effect (2)
Mathematics - Mathematical Physics (2)
Mathematical Physics (2)
Physics - Atomic Physics (2)
Quantum Physics (2)
Statistics - Theory (1)
Physics - Biological Physics (1)
Quantitative Biology - Biomolecules (1)
Mathematics - Statistics (1)
Physics - Atomic and Molecular Clusters (1)
Nonlinear Sciences - Pattern Formation and Solitons (1)
Physics - Optics (1)
Physics - Disordered Systems and Neural Networks (1)
Physics - Statistical Mechanics (1)

Publications Authored By M. A. Marques

In this work we deal with a non-canonical scalar field in the two-dimensional spacetime. We search for a generalized model that is twin of the standard model, supporting the same defect structure with the same energy density. We also study the stability of the defect solution under small fluctuations, which is governed by a Sturm-Liouville equation, and show how to make it stable. Read More

We describe a classical thermodynamic model that reproduces the main features of the solid hydrogen phase diagram. In particular, we show how the general structure types that are found by electronic structure calculations and the quantum nature of the protons can also be understood from a classical viewpoint. The model provides a picture not only of crystal structure, but also for the anomalous melting curve and insights into isotope effects, liquid metallisation and InfraRed activity. Read More

The concept of correlation is central to all approaches that attempt the description of many-body effects in electronic systems. Multipartite correlation is a quantum information theoretical property that is attributed to quantum states independent of the underlying physics. In quantum chemistry, however, the correlation energy (the energy not seized by the Hartree-Fock ansatz) plays a more prominent role. Read More

This work deals with twinlike models that support topological structures such as kinks, vortices and monopoles. We investigate the equations of motion and develop the first order framework to show how to build distinct models with the same solution and energy density, as required to make them twinlike models. We also investigate how the stability under small fluctuations behaves and introduce the conditions to get the same stability on general grounds. Read More

We investigate the presence of non-topological solutions of the Q-ball type in (1, 1) spacetime dimensions. The model engenders the global U(1) symmetry and is of the k-field type, since it contains a new term, of the fourth-order power in the derivative of the complex scalar field. It supports analytical solution of the Q-ball type which is stable quantum mechanically. Read More

We study a family of Maxwell-Higgs models, described by the inclusion of a function of the scalar field that represent generalized magnetic permeability. We search for vortex configurations which obey first-order differential equations that solve the equations of motion. We first deal with the asymptotic behavior of the field configurations, and then implement a numerical study of the solutions, the energy density and the magnetic field. Read More

How fast can a laser pulse ionize an atom? We address this question by considering pulses that carry a fixed time-integrated energy per-area, and finding those that achieve the double requirement of maximizing the ionization that they induce, while having the shortest duration. We formulate this double-objective quantum optimal control problem by making use of the Pareto approach to multi-objetive optimization, and the differential evolution genetic algorithm. The goal is to find out how much a precise time-profiling of ultra-fast, large-bandwidth pulses may speed up the ionization process with respect to simple-shape pulses. Read More

We investigate the possibility of achieving high-temperature superconductivity in hydrides under pressure by inducing metallization of otherwise insulating phases through doping, a path previously used to render standard semiconductors superconducting at ambient pressure. Following this idea, we study H$_2$O, one of the most abundant and well-studied substances, we identify nitrogen as the most likely and promising substitution/dopant. We show that for realistic levels of doping of a few percent, the phase X of ice becomes superconducting with a critical temperature of about 60 K at 150GPa. Read More

In this work we deal with non-topological solutions of the Q-ball type in two space-time dimensions, in models described by a single complex scalar field that engenders global symmetry. The main novelty is the presence of stable Q-balls solutions that live in a compact interval of the real line and appear from a family of models controlled by two distinct parameters. We find analytical solutions and study their charge and energy, and show how to control the parameters to make the Q-balls classically and quantum mechanically stable. Read More

In this work we deal with nontopological solutions of the Q-ball type in two spacetime dimensions. We study models of current interest, described by a Higgs-like and other, similar potentials which unveil the presence of exact solutions. We use the analytic results to investigate how to control the energy and charge to make the Q-balls stable. Read More

We deal with relativistic models described by a single real scalar field, searching for topological structures that behave asymmetrically, connecting minima with distinct profile. We use such features to build a new braneworld scenario, in which the source scalar field contributes to generate asymmetric hybrid brane. Read More

We study the presence of lumplike solutions in models described by a single real scalar field with standard kinematics in two-dimensional spacetime. The results show several distinct models that support the presence of bell-shaped, lumplike structures which may live in a compact space. Read More

Silicon materials play a key role in many technologically relevant fields, ranging from the electronic to the photovoltaic industry. A systematic search for silicon allotropes was performed by employing a modified ab initio minima hopping crystal structure prediction method. The algorithm was optimized to specifically investigate the hitherto barely explored low-density regime of the silicon phase diagram by imitating the guest-host concept of clathrate compounds. Read More

We use ab initio global structural prediction, and specifically the minima hopping method, to explore the periodic table in search of novel oxide phases. In total, we study 183 different compositions of the form MXO2, where M=(Cu, Ag, Au) and X is an element of the periodic table. This set includes the well-known Cu delafossite compounds that are, up to now, the best p-type transparent conductive oxides known to mankind. Read More

Functionals of the one-body reduced density matrix (1-RDM) are routinely minimized under Coleman's ensemble $N$-representability conditions. Recently, the topic of pure-state $N$-representability conditions, also known as generalized Pauli constraints, received increased attention following the discovery of a systematic way to derive them for any number of electrons and any finite dimensionality of the Hilbert space. The target of this work is to assess the potential impact of the enforcement of the pure-state conditions on the results of reduced density-matrix functional theory calculations. Read More

Real-space grids are a powerful alternative for the simulation of electronic systems. One of the main advantages of the approach is the flexibility and simplicity of working directly in real space where the different fields are discretized on a grid, combined with competitive numerical performance and great potential for parallelization. These properties constitute a great advantage at the time of implementing and testing new physical models. Read More

We study braneworld models in the presence of auxiliary fields. We use the first-order framework to investigate several distinct possibilities, where the standard braneworld scenario changes under the presence of the parameter that controls the auxiliary fields introduced to modify Einstein's equation. The results add to previous ones, to show that the minimal modification that we investigate contributes to change quantitatively the thick braneworld profile, although no new qualitative effect is capable of being induced by the minimal modification here considered. Read More

For some insulators we present a procedure to determine an electronic density leading to a lower energy than that of the Kohn-Sham ground state. Read More

This work deals with the presence of localized structures in relativistic systems described by a single real scalar field in two-dimensional spacetime. We concentrate on kinks and compactons in models with standard kinematics, and we develop a procedure that help us to smoothly go from kinks to compactons in the suggested scenario. We also show how the procedure works in the braneworld scenario, for flat brane in the five-dimensional spacetime with a single extra dimension of infinite extent. Read More

We investigate the presence of static solutions in models described by real scalar field in two-dimensional spacetime. After taking advantage of a procedure introduced sometime ago, we solve intricate nonlinear ordinary differential equations and illustrate how to find compact structures in models engendering standard kinematics. In particular, we study linear stability and show that all the static solutions we have found are linearly stable. Read More

We construct a generalized-gradient approximation for the exchange-energy density of finite two-dimensional systems. Guided by non-empirical principles, we include the proper small-gradient limit and the proper tail for the exchange-hole potential. The observed performance is superior to that of the two-dimensional local-density approximation, which underlines the usefulness of the approach in practical applications. Read More

The effect of spatial correlations on the Purcell effect in a bidimensional dispersion of resonant nanoparticles is analyzed. We perform extensive calculations on the fluorescence decay rate of a point emitter embedded in a system of nanoparticles statistically distributed according to a simple 2D lattice-gas model near the critical point. For short-range correlations (high temperature thermalization) the Purcell factors present a long-tailed statistic which evolves towards a bimodal distribution when approaching the critical point where the spatial correlation length diverges. Read More

We assess the validity of various exchange-correlation functionals for computing the structural, vibrational, dielectric, and thermodynamical properties of materials in the framework of density-functional perturbation theory (DFPT). We consider five generalized-gradient approximation (GGA) functionals (PBE, PBEsol, WC, AM05, and HTBS) as well as the local density approximation (LDA) functional. We investigate a wide variety of materials including a semiconductor (silicon), a metal (copper), and various insulators (SiO$_2$ $\alpha$-quartz and stishovite, ZrSiO$_4$ zircon, and MgO periclase). Read More

Systematic ab initio structure prediction was applied for the first time to predict low energy surface reconstructions by employing the minima hopping method on the \alpha-boron (111) surface. Novel reconstruction geometries were identified and carefully characterized in terms of structural and electronic properties. Our calculations predict the formation of a planar, mono-layer sheet at the surface, which is responsible for conductive surface states. Read More

According to previous interpretations of experimental data, sodium-scandium double-cation borohydride NaSc(BH$_4$)$_4$ crystallizes in the crystallographic space group $Cmcm$ where each sodium (scandium) atom is surrounded by six scandium (sodium) atoms. A careful investigation of this phase based on \textit{ab initio} calculations indicates that the structure is dynamically unstable and gives rise to an energetically and dynamically more favorable phase with $C222_1$ symmetry and nearly identical x-ray diffraction pattern. By additionally performing extensive structural searches with the minima-hopping method we discover a class of new low-energy structures exhibiting a novel structural motif in which each sodium (scandium) atom is surrounded by four scandium (sodium) atoms arranged at the corners of either a rectangle with nearly equal sides or a tetrahedron. Read More

The self-consistent GW band gaps are known to be significantly overestimated. We show that this overestimation is, to a large extent, due to the neglect of the contribution of the lattice polarization to the screening of the electron-electron interaction. To solve this problem, we derive within the GW formalism a generalized plasmon-pole model that accounts for lattice polarization. Read More

Low-energy structures of alanates are currently known to be described by patterns of isolated, nearly ideal tetrahedral [AlH$_4$] anions and metal cations. We discover that the novel polymeric motif recently proposed for LiAlH$_4$ plays a dominant role in a series of alanates, including LiAlH$_4$, NaAlH$_4$, KAlH$_4$, Mg(AlH$_4$)$_2$, Ca(AlH$_4$)$_2$ and Sr(AlH$_4$)$_2$. In particular, most of the low-energy structures discovered for the whole series are characterized by networks of corner-sharing [AlH$_6$] octahedra, forming wires and/or planes throughout the materials. Read More

The Bethe-Salpeter equation is a widely used approach to describe optical excitations in bulk semiconductors. It leads to spectra that are in very good agreement with experiment, but the price to pay for such accuracy is a very high computational burden. One of the main bottlenecks is the large number of k-points required to obtain converged spectra. Read More

We present a time-dependent density-functional method able to describe the photoelectron spectrum of atoms and molecules when excited by laser pulses. This computationally feasible scheme is based on a geometrical partitioning that efficiently gives access to photoelectron spectroscopy in time-dependent density-functional calculations. By using a geometrical approach, we provide a simple description of momentum-resolved photoe- mission including multi-photon effects. Read More

In the framework of density-functional theory, several popular density functionals for exchange and correlation have been constructed to satisfy a local form of the Lieb-Oxford bound. In its original global expression, the bound represents a rigorous lower limit for the indirect Coulomb interaction energy. Here we employ exact-exchange calculations for the G2 test set to show that the local form of the bound is violated in an extensive range of both the dimensionless gradient and the average electron density. Read More

We present state-of-the-art first-principle calculations of the electronic and optical properties of silicon allotropes with interesting characteristics for applications in thin-film solar cells. These new phases consist of distorted sp$^3$ silicon networks and have a lower formation energy than other experimentally produced silicon phases. Some of these structures turned out to have quasi-direct and dipole-allowed band gaps in the range 0. Read More

The central quantity of density functional theory is the so-called exchange-correlation functional. This quantity encompasses all non-trivial many-body effects of the ground-state and has to be approximated in any practical application of the theory. For the past 50 years, hundreds of such approximations have appeared, with many successfully persisting in the electronic structure community and literature. Read More

A novel allotrope of carbon with $P2/m$ symmetry was identified during an \emph{ab-initio} minima-hopping structural search which we call $M10$-carbon. This structure is predicted to be more stable than graphite at pressures above 14.4 GPa and consists purely of $sp^3$ bonds. Read More

We derive the semiclassical Kirzhnits expansion of the D-dimensional one-particle density matrix up to the second order in $\hbar$. We focus on the two-dimensional (2D) case and show that all the gradient corrections both to the 2D one-particle density and to the kinetic energy density vanish. However, the 2D Kirzhnits expansion satisfies the consistency criterion of Gross and Proetto [J. Read More

A systematic ab initio search for low enthalpy phases of disilane (Si_2H_6) at high pressures was performed based on the minima hopping method. We found a novel metallic phase of disilane with Cmcm symmetry, which is enthalpically more favorable than the recently proposed structures of disilane up to 280 GPa, but revealing compositional instability below 190 GPa. The Cmcm phase has a moderate electron-phonon coupling yielding a superconducting transition temperature T_c of around 20 K at 100 GPa, decreasing to 13 K at 220 GPa. Read More

Through a systematic structural search we found an allotrope of carbon with Cmmm symmetry which we predict to be more stable than graphite for pressures above 10 GPa. This material, which we refer to as Z-carbon, is formed by pure sp3 bonds and is the only carbon allotrope which provides an excellent match to unexplained features in experimental X-ray diffraction and Raman spectra of graphite under pressure. The transition from graphite to Z-carbon can occur through simple sliding and buckling of graphene sheets. Read More

We studied the dynamics of magnetization through an investigation of the magnetoimpedance effect in CoFeB/(Ta, Ag, Cu) multilayered thin films grown by magnetron sputtering. Impedance measurements were analyzed in terms of the mechanisms responsible for their variations at different frequency intervals and the magnetic and structural properties of the multilayers. Analysis of the mechanisms responsible for magnetoimpedance according to frequency and external magnetic field showed that for the CoFeB/Cu multilayer, ferromagnetic resonance (FMR) contributes significantly to the magnetoimpedance effect at frequencies close to 470 MHz. Read More

We present a local density approximation (LDA) for one-dimensional (1D) systems interacting via the soft-Coulomb interaction based on quantum Monte-Carlo calculations. Results for the ground-state energies and ionization potentials of finite 1D systems show excellent agreement with exact calculations, obtained by exploiting the mapping of an $N$-electron system in $d$ dimensions, onto a single electron in $N\times d$ dimensions properly symmetrized by the Young diagrams. We conclude that 1D LDA is of the same quality as its three-dimensional (3D) counterpart, and we infer conclusions about 3D LDA. Read More

Quantum optimal control theory is a powerful tool for engineering quantum systems subject to external fields such as the ones created by intense lasers. The formulation relies on a suitable definition for a target functional, that translates the intended physical objective to a mathematical form. We propose the use of target functionals defined in terms of the one-particle density and its current. Read More

We present a joint experimental and theoretical study of the superconducting phase of the layered binary silicide BaSi2. Compared with the layered AlB2 structure of graphite or diboride-like superconductors, in the hexagonal structure of binary silicides the sp3 arrangement of silicon atoms leads to corrugated sheets. Through a high-pressure synthesis procedure we are able to modify the buckling of these sheets, obtaining the enhancement of the superconducting transition temperature from 4 K to 8. Read More

We test local and semi-local density functionals for the electronic exchange for a variety of systems including atoms, molecules, and atomic chains. In particular, we focus on a recent universal extension of the Becke-Johnson exchange potential [E. R\"as\"anen, S. Read More

Affiliations: 1CEA-DEN, 2CEA-DEN, 3Méthodes d'Analyse Stochastique des Codes et Traitements Numériques, 4CEA-DEN

To perform uncertainty, sensitivity or optimization analysis on scalar variables calculated by a cpu time expensive computer code, a widely accepted methodology consists in first identifying the most influential uncertain inputs (by screening techniques), and then in replacing the cpu time expensive model by a cpu inexpensive mathematical function, called a metamodel. This paper extends this methodology to the functional output case, for instance when the model output variables are curves. The screening approach is based on the analysis of variance and principal component analysis of output curves. Read More

A very popular ab-initio scheme to calculate electronic properties in solids is the use of hybrid functionals in density functional theory (DFT) that mixes a portion of Fock exchange with DFT functionals. In spite of their success, a major problem still remains, related to the use of one single mixing parameter for all materials. Guided by physical arguments that connect the mixing parameter to the dielectric properties of the solid, and ultimately to its band gap, we propose a method to calculate this parameter from the electronic density alone. Read More

We propose the heterojunction effect in the analysis of the fluorescence mechanism of the firefly chromophore. Following this analysis, and with respect to the HOMO-LUMO gap alignment between the chromophore's functional fragments, three main heterojunction types (I, II, and I*) are identified. Time-dependent density-functional theory optical absorption calculations for the firefly chromophore show that the strongest excitation appears in the deprotonated anion state of the keto form. Read More

Using a first-principle approach beyond density functional theory we calculate the electronic and optical properties of small diameter CdSe nanowires.Our results demonstrate how some approximations commonly used in bulk systems fail at this nano-scale level and how indispensable it is to include crystal local fields and excitonic effects to predict the unique optical properties of nanowires. From our results, we then construct a simple model that describes the optical gap as a function of the diameter of the wire, that turns out to be in excellent agreement with experiments for intermediate and large diameters. Read More

We present a practical and accurate density functional for the exchange-correlation energy of electrons in two dimensions. The exchange part is based on a recent two-dimensional generalized-gradient approximation derived by considering the limits of small and large density gradients. The fully local correlation part is constructed following the Colle-Salvetti scheme and a Gaussian approximation for the pair density. Read More

Recent numerical investigations have uncovered a surprising result: Reissner-Nordstrom-de Sitter black holes are unstable for spacetime dimensions larger than 6. Here we prove the existence of such instability analytically, and we compute the timescale in the near-extremal limit. We find very good agreement with the previous numerical results. Read More

We use hybrid functionals and restricted self-consistent GW, state-of-the-art theoretical approaches for quasiparticle band structures, to study the electronic states of delafossite Cu(Al,In)O$_2$, the first p-type and bipolar transparent conductive oxides. We show that self-consistent GW gives remarkably wider band gaps than all the other approaches used so far. Accounting for polaronic effects in the GW scheme we recover a very nice agreement with experiments. Read More

The band structure of a strongly correlated semiconductor as NiO has been the object of much debate [PRL 103, 036404 (2009); PRL 102, 226401 (2009)]. Most authors, using computational techniques well beyond the simple density functional theory and the approximations GGA or LDA, claim that the band gap is about 4.0 eV and that the conduction band is of Ni-3d nature. Read More

The addition of transition metals (TM) to III-V semiconductors radically changes their electronic, magnetic and structural properties. In contrast to the conventional semiconductor alloys, the lattice parameter in magnetic semiconductor alloys, including the ones with diluted concentration (the diluted magnetic semiconductors - DMS), cannot be determined uniquely from the composition. By using first-principles calculations, we find a direct correlation between the magnetic moment and the anion-TM bond lengths. Read More