arXiv subjects

Emilio Artacho

Publications and source records attributed to Emilio Artacho.

At least 19 recordsLinked to original sources

arXiv2026

Z1 oscillations and charge state in electronic stopping power from first principles

The energy transfer rate from a projectile nucleus to the electrons of the matter it traverses depends on the charge of that projectile, Q= e Z1. At low projectile velocities the friction coefficient is known to oscillate with atomic number Z1, since core electrons travel with the projectile screening its charge. The effective charge increases with velocity and oscillations disappear. That effect is studied here calculating electronic stopping power from first principles for O and Mg projectiles shooting through bulk Al, using real-time time-dependent density-functional theory. Both projectiles represent maximum and minimum of the first Z1 oscillation, respectively. The oscillation is found to be very sensitive to the direction of propagation, in spite of Al being quite an ideal metal for many purposes. The critical velocity for the oscillation disappearance ranges between below 0.1 a.u. and beyond 1 a.u. for the explored trajectories. The charge state is independently quantified with Hirshfeld and Voronoi analyses, offering remarkably consistent results in spite of their very different partition methods, as well as with an effective definition based on the stopping power itself. They display a gradual undressing of the projectile's core electrons with increasing velocity in qualitative accordance with expectations. However, electron density plots in real space present a richer picture in which the undressing is partly due to the electrons trailing behind the projectile, suggesting possible phenomenological descriptions correcting for the deformation of the density in terms of multipoles beyond the net charge. The plots also offer insights into dissipation by core electrons.

cond-mat.mtrl-sci↗

arXiv2026

Dual role of core electrons in electronic friction

Non-equilibrium energy dissipation in multi-shell swift-ion/matter systems remains a fundamental yet incompletely understood problem, with electronic stopping power $\mathcal{S}_\text{e}$ as a relevant observable for electronic friction. Using real-time time-dependent density functional theory, we perform first-principles calculations of $\mathcal{S}_\text{e}$ for beryllium self-irradiation with explicit treatment of all electrons. Our results reveal a Bragg peak exhibiting a distinct structure which lies beyond the reach of standard models. We attribute its appearance to a dual effect of the presence of core electrons, by which their excitation provides an additional dissipation channel while simultaneously suppressing valence electron excitations, contrary to earlier proposals. Electron capture by the projectile's core from the host cores is behind such suppression rather than Pauli blocking.

cond-mat.mtrl-sci↗

arXiv2025

Degenerate monolayer Ising superconductors via chiral-achiral molecule intercalation

Engineering unconventional superconductors is a central challenge in condensed matter physics. Molecule-intercalated TaS2 superlattices have recently been reported to host such states, yet their origin remains debated, underscoring the urgent need for controlled, device-integrated studies. Here, we report that nanometer-thick TaS2 and NbSe2 intercalated with chiral and achiral organic cations instead exhibit robust monolayer-like Ising superconductivity, with no evidence of unconventional pairing. Using high-quality superlattices integrated into devices, we disentangle the roles of interlayer coupling and charge transfer in shaping their superconducting behavior. In TaS2, intercalation induces interlayer decoupling regardless of molecular size or symmetry, yielding monolayer-like Ising superconductivity. NbSe2 instead retains quasi-three-dimensional transport, with a gradual Ising enhancement and near-monolayer behavior only at the largest interlayer spacing. Transport remains reciprocal across all superlattices, consistent with preserved inversion symmetry and incompatible with parity-breaking superconductivity and noncentrosymmetric monolayers. We attribute the behavior to electronically detached monolayers with opposite spin-split bands, coupled through thermal and tunneling processes, which overall preserve inversion symmetry. These findings establish molecular intercalation compounds as a robust, device-ready, platform for engineering advanced superconducting superlattices.

cond-mat.supr-con↗

arXiv2025

First-Principles Nanocapacitor Simulations of the Optical Dielectric Constant in Water Ice

We introduce a combined density functional theory (DFT) and non-equilibrium Green's function (NEGF) framework to compute the capacitance of nanocapacitors and directly extract the dielectric response of a sub-nanometer dielectric under bias. We identify that at the nanoscale conventional capacitance evaluations based on stored charge per unit voltage suffer from an ill-posed partitioning of electrode and dielectric charge. This partitioning directly impacts the geometric definition of capacitance through the capacitor width, which in turn makes the evaluation of dielectric response uncertain. This ambiguous separation further induces spurious interfacial polarizability when analyzed via maximally localized Wannier functions. Focusing on crystalline ice, we develop a robust charge-separation protocol that yields unique capacitance-derived polarizability and dielectric constants, unequivocally demonstrating that confinement neither alters ice's intrinsic electronic response nor its insensitivity to proton order. Our results lay the groundwork for rigorous interpretation of capacitor measurements in low-dimensional dielectric materials.

cond-mat.mes-hall↗

arXiv2025

On-surface Synthesis of a Ferromagnetic Molecular Spin Trimer

Triangulenes are prototypical examples of open-shell nanographenes. Their magnetic properties, arising from the presence of unpaired $\pi$ electrons, can be extensively tuned by modifying their size and shape or by introducing heteroatoms. Different triangulene derivatives have been designed and synthesized in recent years, thanks to the development of on-surface synthesis strategies. Triangulene-based nanostructures with polyradical character, hosting several interacting spin units, can be challenging to fabricate but are particularly interesting for potential applications in carbon-based spintronics. Here, we combine pristine and N-doped triangulenes into a more complex nanographene, \textbf{TTAT}, predicted to possess three unpaired $\pi$ electrons delocalized along the zigzag periphery. We generate the molecule on an Au(111) surface and detect direct fingerprints of multi-radical coupling and high-spin state using scanning tunneling microscopy and spectroscopy. With the support of theoretical calculations, we show that its three radical units are localized at distinct parts of the molecule and couple via symmetric ferromagnetic interactions, which result in a $S=3/2$ ground state, thus demonstrating the realization of a molecular ferromagnetic Heisenberg-like spin trimer

cond-mat.mes-hall↗

arXiv2025

Rototranslational sum rules for nuclear dynamics via traveling pseudopotentials

We establish a set of exact sum rules that relate the interatomic force constants to the frequency-dependent electromagnetic susceptibility of a solid or molecule, thereby generalizing the long-established principles of rototranslational symmetry to the nonadiabatic regime. Crucially, we show that in practical numerical implementations these sum rules are violated, unless special precautions are taken in the treatment of the atomic pseudopotentials. We solve these issues once and for all by correctly adapting the pseudopotential to the motion of the corresponding nucleus, with a velocity dependence of the nonlocal operator. This prescription restores the correct Galilean covariance of the Schr\"odinger equation, and the expected identity between mechanical rototranslations and electromagnetic perturbations. These results conclusively fix a number of worrisome inconsistencies that were pointed out over the years in the context of linear-response theory restoring, e.g., the validity of the Larmor theorem, and the equivalence between the inertial and electrical definitions of the Drude weight in metals.

cond-mat.mtrl-sci↗

arXiv2025

Excess energy and countercurrents after a quantum kick

A quantum system of interacting particles under the effect of a static external potential is hereby described as kicked when that potential suddenly starts moving with a constant velocity v. If initially in a stationary state, the excess energy at any time after the kick equals $v \langle P \rangle (t)$, with P being the total momentum of the system. If the system is finite and remains bound, the long time average of the excess energy tends to $Mv^2$, with M the system's total mass, or a related expression if there is particle emission. $Mv^2$ is twice what expected from an infinitely smooth onset of motion, and any monotonic onset is expected to increase the average energy to a value within both limits. In a macroscopic system, a particle flow emerges countering the potential's motion when electrons stay partially behind. For charged particles the described kinetic kick is equivalent to the kick given by the infinitely short electric-field pulse $E = \frac{m}{q} v \delta (t)$ to the system at rest, useful as a formal limit in ultrafast phenomena. A linear-response analysis of low-v countercurrents in kicked metals shows that the coefficient of the linear term in v is the Drude weight. Non-linear in v countercurrents are expected for insulators through the electron-hole excitations induced by the kick, going as $v^3$ at low v for centrosymmetric ones. First-principles calculations for simple solids are used to ratify those predictions, although the findings apply more generally to systems such as Mott insulators or cold lattices of bosons or fermions.

cond-mat.mtrl-sci↗

arXiv2025

Anomalies in the electronic stopping of slow antiprotons in LiF

We present first-principles theoretical calculations for the electronic stopping power (SP) of both protons and anti-protons in LiF. Our results show the presence of the Barkas effect: a higher stopping for positively charged particles than their negatively charged antiparticles. In contrast, a previous study has predicted an anti-Barkas effect (higher stopping for negative charges) at low velocity [Qi, Bruneval and Maliyov, Phys. Rev. Lett. 128, 043401 (2022)]. We explain this discrepancy by showing that this anti-Barkas effect appears for highly symmetric trajectories and disappears when considering trajectories that better reproduce the experimental setup. Our low-velocity results show that the SP of both protons and anti-proton vanish for velocities under 0.1 a.u. .

cond-mat.other↗

arXiv2024

Redefining the dielectric response of nanoconfined liquids: insights from water

Recent experiments show that the relative dielectric constant $\epsilon$ of water confined to a film of nanometric thickness reaches a strikingly low value of 2.1, barely above the bulk's 1.8 value for the purely electronic response. We argue that $\epsilon$ is not a well-defined measure for dielectric properties at sub-nanometer scales due to the ambiguous definition of confinement width. Instead we propose the 2D polarizability $\alpha_{\perp}$ as the appropriate, well-defined response function whose magnitude can be directly obtained from both measurements and computations. Once the appropriate description is used, understanding the interplay between electronic and ionic contributions becomes critical, contrary to what is widely assumed. This highlights the importance of electronic degrees of freedom in interpreting the dielectric response of polar fluids under nanoconfinement conditions, as revealed by molecular dynamics simulations.

cond-mat.mes-hall↗

arXiv2024

Pseudo-proper two-dimensional electron gas formation

In spite of the interest in the two-dimensional electron gases (2DEGs) experimentally found at surfaces and interfaces, important uncertainties remain about the observed insulator--metal transitions (IMTs). Here we show how an explicit improper coupling of carrier sources with a relevant soft mode significantly affects the transition. The analysis presented here for 2DEGs at polar interfaces is based on group theory, Landau-Ginzburg theory, and illustrated with first-principles calculations for the prototypical case of the LaAlO$_3$/SrTiO$_3$ interface, for which such a structural transition has recently been observed. This direct coupling implies that the appearance of the soft mode is always accompanied by carriers. For sufficiently strong coupling an avalanche-like first-order IMT is predicted.

cond-mat.mes-hall↗

arXiv2023

On-Surface Synthesis and Characterization of a High-Spin Aza-[5]-Triangulene

Triangulenes are open-shell triangular graphene flakes with total spin increasing with their size. In the last years, on-surface-synthesis strategies have permitted fabricating and engineering triangulenes of various sizes and structures with atomic precision. However, direct proof of the increasing total spin with their size remains elusive. In this work, we report the combined in-solution and on-surface synthesis of a large nitrogen-doped triangulene (aza-[5]-triangulene) and the detection of its high spin ground state on a Au(111) surface. Bond-resolved scanning tunneling microscopy images uncovered radical states distributed along the zigzag edges, which were detected as weak zero-bias resonances in scanning tunneling spectra. These spectral features reveal the partial Kondo screening of a high spin state. Through a combination of several simulation tools, we find that the observed distribution of radical states is explained by a quintet ground state (S = 2), instead of the expected quartet state (S = 3/2), confirming the positively charged state of the molecule on the surface. We further provide a qualitative description of the change of (anti)aromaticity introduced by N-substitution, and its role in the charge stabilization on a surface, resulting in a S = 2 aza-[5]-triangulene on Au(111).

cond-mat.mes-hall↗

arXiv2023

Modular implementation of the linear and cubic-scaling orbital minimization methods in electronic structure codes using atomic orbitals

We present a code modularization approach to design efficient and massively parallel cubic and linear-scaling solvers for electronic structure calculations using atomic orbitals. The modular implementation of the orbital minimization method, in which linear algebra and parallelization issues are handled via external libraries, is demonstrated in the SIESTA code. The DBCSR and ScaLAPACK libraries are used for algebraic operations with sparse and dense matrices, respectively. The MatrixSwitch and libOMM libraries, recently developed within the Electronic Structure Library, facilitate switching between different matrix formats and implement the energy minimization. We show results comparing the performance of several cubic-scaling algorithms, and also demonstrate the parallel performance of the linear-scaling solvers, and their supremacy over the cubic-scaling solvers for insulating systems with sizes of several hundreds of atoms.

cond-mat.mtrl-sci↗

arXiv2023

Pressure-induced transitions in FePS$_3$: Structural, magnetic and electronic properties

FePS$_3$ is a prototype van der Waals layered antiferromagnet and a Mott insulator under ambient conditions, which has been recently reported to go through a pressure-induced dimensionality crossover and an insulator-to-metal transition. These transitions also lead to the appearance of a novel magnetic metallic state. To further understand these emergent structural and physical properties, we have performed a first-principles study using van der Waals and Hubbard $U$ corrected density functional theory including a random structure search. Our computational study attempts to interpret the experimental coexistence of the low- and intermediate-pressure phases and we predict a novel high-pressure phase with distinctive dimensionality and different possible origins of metallicity.

cond-mat.str-el↗

arXiv2023

Electronic-mediated nuclear stopping power in proton irradiated water ice

Traditionally, it has been assumed that the stopping of a swift ion travelling through matter can be understood in terms of two essentially independent components, i.e. electronic vs. nuclear. Performing extensive Ehrenfest MD simulations of the process of proton irradiation of water ice that accurately describe not only the non-adiabatic dynamics of the electrons but also of the nuclei, we have found a stopping mechanism involving the interplay of the electronic and nuclear subsystems. This effect, which consists in a kinetic energy transfer from the projectile to the target nuclei thanks to the perturbations of the electronic density caused by the irradiation, is fundamentally different from the atomic displacements and collision cascades characteristic of nuclear stopping. Moreover, it shows a marked isotopic effect depending on the composition of the target, being relevant mostly for light water as opposed to heavy water. This result is consistent with long-standing experimental results which remained unexplained so far.

cond-mat.mtrl-sci↗

arXiv2023

On the effect of electronic stopping in molecular dynamics simulations of collision cascades in Gallium Arsenide

Understanding the generation and evolution of defects induced in matter by ion irradiation is of fundamental importance to estimate the degradation of functional properties of materials. Computational approaches used in dierent communities, from space radiation eects to nuclear energy experiments, are based on a number of approximations that, among others, traditionally neglect the coupling between electronic and ionic degrees of freedom in the description of displacements. In this work, we study collision cascades in GaAs, including the electronic stopping power for selfprojectiles in dierent directions obtained via real time Time Dependent Density Functional Theory in Molecular Dynamics simulations of collision cascades, using the recent electron-phonon model and the previously developed two-temperature model. We show that the former can be well applied to describe the eects of electronic stopping in molecular dynamics simulations of collision cascades in a multielement semiconductor and that the number of defects is considerably aected by electronic stopping eects. The results are also discussed in the wider context of the commonly used non-ionizing energy loss model to estimate degradation of materials by cumulative displacements.

physics.comp-ph↗

arXiv2023

Nonlinear electronic stopping of negatively-charged particles in liquid water

We present real-time time-dependent density-functional-theory calculations of the electronic stopping power for negative and positive projectiles (electrons, protons, antiprotons and muons) moving through liquid water. After correction for finite mass effects, the nonlinear stopping power obtained in this work is significantly different from the previously known results from semi-empirical calculations based on the dielectric response formalism. Linear-nonlinear discrepancies are found both in the maximum value of the stopping power and the Bragg peak's position. Our results indicate the importance of the nonlinear description of electronic processes, particularly for electron projectiles, which are modeled here as classical point charges. Our findings also confirm the expectation that the quantum nature of the electron projectile should substantially influence the stopping power around the Bragg peak and below.

physics.chem-ph↗

arXiv2022

Ab initio electronic stationary states for nuclear projectiles in solids

The process by which a nuclear projectile is decelerated by the electrons of the condensed matter it traverses is currently being studied by following the explicit dynamics of projectile and electrons from first principles in a simulation box with a sample of the host matter in periodic boundary conditions. The approach has been quite successful for diverse systems even in the strong-coupling regime of maximal dissipation. This technique is here revisited for periodic solids in the light of the Floquet theory of stopping, a time-periodic scattering framework characterizing the stationary dynamicalsolutions for a constant velocity projectile in an infinite solid. The effect of proton projectiles in diamond is studied under that light, using time-dependent density-functional theory in real time. The Floquet quasi-energy conserving stationary scattering regime, characterized by time-periodic properties such as particle density and the time derivative of energy, is obtained for a converged system size of one thousand atoms. The validity of the customary calculation of electronic stopping power from the average slope of the density-functional total energy is discussed. Quasi-energy conservation, as well as the implied fundamental approximations, are critically reviewed.

cond-mat.other↗

arXiv2022

Coupling between tilts and charge carriers at polar-nonpolar perovskite interfaces

The phenomenological theory for the polar instability giving rise to a two-dimensional electron gas at perovskite interfaces is hereby extended to include the coupling to perovskite tilts. A Landau theory for homogeneous tilts is first explored, setting the scene for the further, more realistic Landau-Ginzburg theory describing varying tilt amplitudes across a thin film. The theory is also generalized to account for the response to an applied electric field normal to the interface, which allows a finer control on phase transitions. The conventionally described physics of a single metal-insulator transition is substantially enriched by the coupling, the model describing various scenarios with one or two transitions, possibly continuous or discontinuous. First-principles calculations permit the estimation of the parameters defining the model, which have been calculated for the interface between lanthanum aluminate and strontium titanate.

cond-mat.mtrl-sci↗