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Dario A. Leon

Publications and source records attributed to Dario A. Leon.

16 recordsLinked to original sources

Plasmonic properties and correlation energies from a compact multipole representation of the dielectric response in 2D metals

Multipole-Padé approximants provide a compact representation of dynamical response functions in terms of a small number of collective modes. Here, we generalize this framework to incorporate momentum dependence across the full Brillouin zone of 2D metals by constructing a symmetry-conserving, anisotropic representation of the inverse dielectric function. This analytic form enables efficient and accurate evaluation of quantities involving dynamical screening, including spectral features and correlation energies. We construct such compact representations for a set of seven two dimensional metals spanning distinct electronic regimes, and show that a small number of dispersive plasmonic modes suffices to accurately describe the dielectric response across the full Brillouin zone, while also yielding accurate correlation energies. The proposed representation therefore establishes a direct bridge between {\it ab initio} calculations and analytical models of screening, opening new avenues for applications in condensed matter systems.

cond-mat.mtrl-sci↗

Bulk plasmons in elemental metals

The spectral properties, momentum dispersion, and broadening of bulk plasmonic excitations of 26 elemental metals are studied from first principles calculations in the random-phase approximation. Spectral band structures are constructed from the resulting momentum- and frequency-dependent inverse dielectric function. We develop an effective analytical representation of the main collective excitations in the dielectric response, extending our earlier model based on multipole-Padé approximants (MPAs) to incorporate both momentum and frequency dependence [MPA($\q$)]. With this representation, we identify plasmonic quasiparticle dispersions exhibiting complex features, including non-parabolic energy and intensity dispersions, discontinuities due to anisotropy, and overlapping effects that lead to band crossings and anti-crossings. Comparing with available experimental data, mainly in the optical limit, we find good agreement with the computed spectra. The results for elemental metals and their effective MPA($\q$) representation establish a reference point that can guide both fundamental studies and practical applications in plasmonics and spectroscopy.

physics.optics↗

Momentum- and frequency-resolved collective electronic excitations in solids: insights from spectroscopy and first-principles calculations

Collective electronic excitations, including plasmons, excitons, and intra- and interband transitions, play a central role in determining the dynamic screening, optical response, and energy transport properties of materials. Recent advances in momentum- and frequency-resolved spectroscopies, such as electron energy-loss spectroscopy (EELS) and inelastic x-ray scattering (IXS), together with progress in first-principles many-body perturbation theory (MBPT) calculations, now allow collective excitations to be mapped with considerable precision across the Brillouin zone. This topical review surveys current developments in the representation and interpretation of both experimental and theoretical dielectric-response spectra. Particular emphasis is placed on recent ways of representing spectral band structures (SBS) of the direct and inverse dielectric functions, such as analytical approaches based on multipole-Padé approximants in momentum and frequency (MPA($\q$)), which provide a combined band-like description of the dispersion of the main collective excitations. We discuss how features observed in metals, semiconductors, and low dimensional systems reflect the interplay between electronic structure, screening strength, and local-field effects, and how post-processing procedures can improve the quantitative comparison between experiment and theory. Finally, we provide perspectives on open challenges and potential developments in quantitative dielectric-function analyses.

cond-mat.mtrl-sci↗

Self-consistent layer-projected scissors operator for band structures of complex 2D van der Waals materials

We introduce a computationally efficient method to calculate the quasiparticle (QP) band structure of general van der Waals (vdW) heterostructures. A layer-projected scissors (LAPS) operator, which depends on the one-body density matrix, is added to the density functional theory (DFT) Hamiltonian. The LAPS operator corrects the band edges of the individual layers for self-energy effects (both intralayer and interlayer) and unphysical strain fields stemming from the use of model supercells. The LAPS operator is treated self-consistently whereby charge redistribution and interlayer hybridization occurring in response to the band energy corrections are properly accounted for. We present several examples illustrating both the qualitative and quantitative performance of the method, including MoS$_2$ films with up to 20 layers, bilayer MoS$_2$ in an electric field, lattice-matched MoS$_2$/WS$_2$ and MoSe$_2$/WSe$_2$ bilayers, and MoSe$_2$/WS$_2$ moiré structures. Our work opens the way for predictive modeling of electronic, optical, and topological properties of complex and experimentally relevant vdW materials.

cond-mat.mtrl-sci↗

Spectral properties from an efficient analytical representation of the $GW$ self-energy within a multipole approximation

We propose an efficient analytical representation of the frequency-dependent $GW$ self-energy $Σ$ via a multipole approximation (MPA-$Σ$). The multipole-Padé model for the self-energy is interpolated from a small set of numerical evaluations of $Σ$ in the complex frequency plane, similarly to the previously multipole representation developed for the screened Coulomb interaction (MPA-$W$) [Phys. Rev. B \textbf{104}, 115157 (2021)]. We show that, likewise MPA-$W$, an appropriate choice of frequency sampling in MPA-$Σ$ is critical to guarantee computational efficiency and high accuracy. The combined MPA-$W$ and MPA-$Σ$ scheme considerably reduces the cost of full-frequency self-energy calculations, especially for spectral band structures over a wide energy range. Crucially, MPA-$Σ$ enables a multipole representation for the interacting Green's function $G$ (MPA-$G$), providing a straightforward evaluation of all the spectral properties, and a more general way to define the renormalization factor $Z$. We validate the MPA-$Σ$ and MPA-$G$ approaches for diverse systems: bulk Si, Na and Cu, monolayer MoS$_2$, the NaCl ion-pair and the F$_2$ molecule. Moreover, we introduce toy MPA-$Σ$/$G$ models to examine the quasiparticle picture in different regimens of weak and strong correlation. With these models, we expose limitations in defining $Z$ from the local derivative of $Σ$.

cond-mat.mtrl-sci↗

Unraveling many-body effects in ZnO: Combined study using momentum-resolved electron energy-loss spectroscopy and first-principles calculations

We present a detailed study of the dielectric response of ZnO using a combination of low-loss momentum-resolved electron energy-loss spectroscopy (EELS) and first-principles calculations at several levels of theory, from the independent particle and the random phase approximation with different variants of density functional theory (DFT), including hybrid and DFT$+U$ schemes; to the Bethe-Salpeter equation (BSE). We use a method based on the $f$-sum rule to obtain the momentum-resolved experimental loss function and absorption spectra from EELS measurements. We characterize the main features in the direct and inverse dielectric functions of ZnO and their dispersion, associating them to single-particle features in the electronic band structure, while highlighting the important role of many-body effects such as plasmons and excitons. We discuss different signatures of the high anisotropy in the response function of ZnO, including the symmetry of the excitonic wave-functions.

cond-mat.mtrl-sci↗

Efficient GW calculations via the interpolation of the screened interaction in momentum and frequency space: The case of graphene

The GW self-energy may become computationally challenging to evaluate because of frequency and momentum convolutions. These difficulties were recently addressed by the development of the multipole approximation (MPA) and the W-av methods: MPA accurately approximates full-frequency response functions using a small number of poles, while W-av improves the convergence with respect to the k-point sampling in 2D materials. In this work we (i) present a theoretical scheme to combine them, and (ii) apply the newly developed approach to the paradigmatic case of graphene. Our findings show an excellent agreement of the calculated QP band structure with angle resolved photoemission spectroscopy (ARPES) data. Furthermore, the computational efficiency of MPA and W-av allows us to explore the logarithmic renormalization of the Dirac cone. To this aim, we develop an analytical model, derived from a Dirac Hamiltonian, that we parameterize using ab-initio data. The comparison of the models obtained with PPA and MPA results highlights an important role of the dynamical screening in the cone renormalization.

cond-mat.mtrl-sci↗

Efficient full frequency GW for metals using a multipole approach for the dielectric screening

The properties of metallic systems with important and structured excitations at low energies, such as Cu, are challenging to describe with simple models like the plasmon pole approximation (PPA), and more accurate and sometimes prohibitive full frequency approaches are usually required. In this paper we propose a numerical approach to $GW$ calculations on metals that takes into account the frequency dependence of the screening via the multipole approximation (MPA), an accurate and efficient alternative to current full-frequency methods that was recently developed and validated for semiconductors and overcomes several limitations of PPA. We now demonstrate that MPA can be successfully extended to metallic systems by optimizing the frequency sampling for this class of materials and introducing a simple method to include the $\mathbf{q}\to 0$ limit of the intra-band contributions. The good agreement between MPA and full frequency results for the calculations of quasi-particle energies, polarizability, self-energy and spectral functions in different metallic systems confirms the accuracy and computational efficiency of the method. Finally, we discuss the physical interpretation of the MPA poles through a comparison with experimental electron energy loss spectra for Cu.

cond-mat.mtrl-sci↗

Graphene decoupling through oxygen intercalation on Gr/Co and Gr/Co/Ir interfaces

We perform a density functional theory study of the effects of oxygen adsorption on the structural and electronic properties of Gr/Co(0001) and Gr/Co/Ir(111) interfaces. In both interfaces, the graphene-Co distance increases with increasing O concentration. The oxygen intercalation effectively decreases the electronic interaction, preventing the hybridization of graphene states with Co $d$-orbitals, hence (partly) restoring the typical Dirac cone of pristine graphene. In the case of graphene/Co 1ML/Ir(111), which presents a moiré pattern, the interplay between the O distribution and the continuous change of the graphene-Co registry can be used to tune graphene corrugation and electronic properties. The computed electronic properties are in very good agreement with previously reported angle resolved photoemission spectroscopy and photoemission electron microscopy measurements for Gr/Co(0001).

cond-mat.mtrl-sci↗

Estimating the number of available states for normal and tumor tissues in gene expression space

The topology of gene expression space for a set of 12 cancer types is studied by means of an entropy-like magnitude, which allows the characterization of the regions occupied by tumor and normal samples. The comparison indicates that the number of available states in gene expression space is much greater for tumors than for normal tissues, suggesting the irreversibility of the progression to the tumor phase. The entropy is nearly constant for tumors, whereas exhibits a higher variability in normal tissues, probably due to tissue differentiation. In addition, we show an interesting correlation between the fraction of available states and the overlapping between the tumor and normal sample clouds, interpreted as a way of reducing the decay rate to the tumor phase in more ordered or structured tissues.

q-bio.TO↗

Frequency dependence in GW made simple using a multi-pole approximation

In the $GW$ approximation, the screened interaction $W$ is a non-local and dynamical potential that usually has a complex frequency dependence. A full description of such dependence is possible but often computationally demanding. For this reason, it is still common practice to approximate $W(ω)$ using a plasmon pole (PP) model. Such approach, however, may deliver an accuracy limited by its simplistic description of the frequency dependence of the polarizability, i.e. of $W$. In this work we explore a multi-pole approach (MPA) and develop an effective representation of the frequency dependence of $W$. We show that an appropriate sampling of the polarizability in the frequency complex plane and a multi-pole interpolation can lead to a level of accuracy comparable with full-frequency methods at much lower computational cost. Moreover, both accuracy and cost are controllable by the number of poles used in MPA. Eventually we validate the MPA approach in selected prototype systems, showing that full-frequency quality results can be obtained with a limited number of poles.

cond-mat.mtrl-sci↗

Narrowing of d bands of FeCo layers intercalated under graphene

We report on the electronic properties of an artificial system obtained by the intercalation of equiatomic FeCo layers under graphene grown on Ir(111). Upon intercalation, the FeCo film grows epitaxially on Ir(111), resulting in a lattice-mismatched system. By performing Density Functional Theory calculations, we show that the intercalated FeCo layer leads to a pronounced corrugation of the graphene film. At the same time, the FeCo intercalated layers induce a clear transition from a nearly undisturbed to a strongly hybridized graphene π-band, as measured by angle-resolved photoemission spectroscopy. A comparison of experimental results with the computed band structure and the projected density of states unveils a spin-selective hybridization between the π band of graphene and FeCo-3d states. Our results demonstrate that the reduced dimensionality, as well as the hybridization within the FeCo layers, induce a narrowing and a clear splitting of Fe 3d-up and Fe 3d-down spin bands of the confined FeCo layers with respect to bulk Fe and Co.

cond-mat.mtrl-sci↗

Magnetic response and electronic states of well defined Graphene/Fe/Ir(111) heterostructure

We investigate a well defined heterostructure constituted by magnetic Fe layers sandwiched between graphene (Gr) and Ir(111). The challenging task to avoid Fe-C solubility and Fe-Ir intermixing has been achieved with atomic controlled Fe intercalation at moderate temperature below 500 K. Upon intercalation of a single ordered Fe layer in registry with the Ir substrate, an intermixing of the Gr bands and Fe d states breaks the symmetry of the Dirac cone, with a downshift in energy of the apex by about 3 eV, and well-localized Fe intermixed states induced in the energy region just below the Fermi level. First principles electronic structure calculations show a large spin splitting of the Fe states, resulting in a majority spin channel almost fully occupied and strongly hybridized with Gr π states. X-ray magnetic circular dichroism on the Gr/Fe/Ir heterostructure reveals an ordered spin configuration with a ferromagnetic response of Fe layer(s), with enhanced spin and orbital configurations with respect to the bcc-Fe bulk values. The magnetization switches from a perpendicular easy magnetization axis when the Fe single layer is lattice matched with the Ir(111) surface to a parallel one when the Fe thin film is almost commensurate with graphene.

cond-mat.mtrl-sci↗

Levy model of cancer

A small portion of a tissue defines a microstate in gene expression space. Mutations, epigenetic events or external factors cause microstate displacements which are modeled by combining small independent gene expression variations and large Levy jumps, resulting from the collective variations of a set of genes. The risk of cancer in a tissue is estimated as the microstate probability to transit from the normal to the tumor region in gene expression space. The formula coming from the contribution of large Levy jumps seems to provide a qualitatively correct description of the lifetime risk of cancer, and reveals an interesting connection between the risk and the way the tissue is protected against infections.

q-bio.PE↗

Modeling evolution in a Long Time Evolution Experiment with E. Coli

Taking into account an evolutionary model of mutations in term of Levy Fights that was previously constructed, we designed an algorithm to reproduce the evolutionary dynamics of the Long-Term Evolution Experiment (LTEE) with E. Coli bacteria. The algorithm enables us to simulate mutations under natural selection conditions. The results of simulations on competition of clones, mean fitness, etc., are compared with experimental data. We attained to reproduce the behavior of the mean fitness of the bacteria cultures, get our own interpretations and more tuned descriptions of some phenomena taking part within the experiment, such as fixation and drift processes, clonal interference and epistasis.

q-bio.PE↗

Modeling mutations in bacteria and human tissues

This thesis is aimed at studying mutations, understood as trajectories in the DNA configuration space. An evolutive model of mutations in terms of Levy flights is proposed. The parameters of the model are estimated by means of data from the Long-Term Evolution Experiment (LTEE) with {\it E. Coli} bacteria. The results of simulations on competition of clones, mean fitness, etc are compared with experimental data. We discuss the qualitative analogy found between the bacterial mutator phenotype and the cancerous cells. The role of radiation as source of mutations is analyzed. We focus on the case of Radon's decay in the lungs in breathing.

q-bio.PE↗