arXiv subjects

Raúl Bombín

Publications and source records attributed to Raúl Bombín.

16 recordsLinked to original sources

arXiv2026

Quantum Dynamical and isotopic effects for Hydrogen isotopes scattering at W(110) surface

We investigate the scattering of hydrogen isotopes at the W(110) surface using both classical and quantum dynamics approaches to elucidate the role of quantum effects in this system. To characterize the scattering process we focus on key observables, including the absorption probability and diffraction channels that we evaluate at the quasi-classical and quantum levels. The quantum dynamics reveal pronounced resonance structures in the absorption curve that we rationalize in terms of diffraction-mediated selective adsorption and focused sticking mechanisms. Diffraction probabilities for reflected trajectories exhibit strong quantum effects at low incident energies, where classical dynamics underestimate the back scattering probability. These effects become less pronounced with increasing isotope mass, from hydrogen to tritium, however discrepancies between the classical and quantum description persist at low incident energies.

physics.chem-ph↗

arXiv2025

Asymmetry and coverage dependence in two-pulse correlation measurements of CO photodesorption from Pd(111): Insights from theory

Two-pulse correlation experiments performed using pulses of different intensities on Pd(111) with different CO coverages showed that the CO photodesorption probability depends on whether the strong or the weak pulse arrives first to the surface, being this difference particularly large for the low-covered surface. Motivated by these experiments, we perform molecular dynamics simulations using a multicoverage potential energy surface that was previously constructed with the embedded atom neural network method. The process is modeled by combining the two-temperature model (2TM)--to describe the laser-excited electrons and phonons--and Langevin dynamics with electronic time-dependent temperature $T_\textrm{e}$--to model the coupling of the nuclei degrees of freedom with the laser-excited electrons. We show that improving the energy balance description in 2TM--by including \textit{ab-initio} $T_\textrm{e}$-dependent electronic heat capacity and electron-phonon coupling constant--is key to reproduce the asymmetry of the photodesorption probability $P_{\rm des}$ between positive and negative time delays. Furthermore, we also explore possible reasons for the usual underestimation of $P_{\rm des}$ at zero delay given by state-of-the-art calculations. In particular, we improve the description of the energy exchange between CO and the metal surface at high $T_\textrm{e}$ by including in the simulations a $T_\textrm{e}$-dependent friction coefficient. The prediction for $P_{\rm des}$ at zero delay in this case, increases by an order of magnitude, reducing its discrepancy with the experimental value. Altogether, our results hint to the importance of accounting for the temperature dependence of the electronic structure and properties in describing the extreme conditions generated in 2PC experiments.

physics.chem-ph↗

arXiv2025

Thermal behavior of Bose-Einstein condensates of polar molecules

We use the finite-temperature extended Gross-Pitaevskii equation (TeGPE) to study a condensate of dipolar NaCs molecules under the conditions of the very recent, breakthrough experiment [Bigagli et.al., Nature 631, 289 (2024)]. We report the condensate fraction of the system, and its density profile after a time-of flight expansion for the coldest experimental case, finding excellent agreement with the experimental measurements. We also report the peak density of the ground state and establish a comparison with the experimental estimates. Our results, derived from the TeGPE formalism, successfully describe the Bose-Einstein condensation of polar molecules at finite temperature.

cond-mat.quant-gas↗

arXiv2025

Creating and melting a supersolid by heating a quantum dipolar system

Recent experiments have shown that rising the temperature of a dipolar gas under certain conditions leads to a transition to a supersolid state. Here, we employ the path integral Monte Carlo method, which exactly accounts for both thermal and correlation effects, to study that phenomenology in a system of $^{162}$Dy atoms in the canonical ensemble. Our microscopic description allows to quantitatively characterize the emergence of spatial order and superfluidity, the two ingredients that define a supersolid state. Our calculations prove that temperature on its own can promote the formation of a supersolid in a dipolar system. Furthermore, we bridge this exotic phenomenology with the more usual melting of the supersolid at a higher temperature. Our results offer insight into the interplay between thermal excitations, the dipole-dipole interaction, quantum statistics and supersolidity.

cond-mat.quant-gas↗

arXiv2024

Scattering of CO from Vacant-MoSe$_2$ with O Adsorbates: Is CO$_2$ Formed?

Using ab initio molecular dynamics (AIMD) simulations, based on density functional theory that also accounts for van der Waals interactions, we study the oxidation of gas phase CO on MoSe$_2$ with a Se vacancy and oxygen coverage of 0.125~ML. In the equilibrium configuration, one of the O atoms is adsorbed on the vacancy and the other one atop one Se atom. Recombination of the CO molecule with the second of these O atoms to form CO$_2$ is a highly exothermic reaction, with an energy gain of around 3~eV. The likeliness of the CO oxidation reaction on this surface is next examined by calculating hundreds of AIMD trajectories for incidence energies that suffice to overcome the energy barriers in the entrance channel of the CO oxidative recombination. In spite of it, no CO$_2$ formation event is obtained. In most of the calculated trajectories the incoming CO molecule is directly reflected and in some cases, mainly at low energies, the molecules remain trapped at the surface but without reacting. As important conclusion, our AIMD simulations show that the recombination of CO molecules with adsorbed O atoms is a very unlikely reaction in this system, despite its large exothermicity.

physics.chem-ph↗

arXiv2024

Dipolar droplets of strongly interacting molecules

We simulate a molecular Bose-Einstein condensate in the strongly dipolar regime, observing the existence of self-bound droplets, as well as their splitting into multiple droplets by confinement-induced frustration. Our quantum Monte Carlo approach goes beyond the limits of the established effective mean-field theories for dipolar quantum gases, revealing small droplets produced by strong dipolar interactions outside known stable regimes. The simulations include realistic molecular interactions and therefore have direct relevance for current and future experiments.

cond-mat.quant-gas↗

arXiv2024

Ring solids and supersolids in spherical shell-shaped dipolar Bose-Einstein condensates

We study the interplay between the anisotropy of the dipole-dipole interaction and confinement in a curved geometry by means of the extended Gross-Pitaevskii equation, which allows us to characterize the ground state of a dipolar Bose gas under the confinement of a bubble trapping potential. We do so in terms of the scattering length a and the number of particles. We observe the emergence of a wide variety of dipolar solids, consisting on arrangements of different number of droplets along a ring over the equator of the spherical shell confinement. We also show that the transition between the different phases of the system can be engineered by varying a, the number of particles or the radius of the trap, parameters which can be experimentally tuned. Finally, we show the importance of working in microgravity conditions as gravity unstabilizes the observed dipolar solids.

cond-mat.quant-gas↗

arXiv2024

A quantum Monte Carlo based density functional for Dysprosium dipolar system

We present a quantum Monte Carlo based density functional to describe droplet formation and supersolidity in dipolar systems. The usual Lee-Huang-Yang term, accounting for quantum correlations in the conventional extended Gross-Pitaievskii equation (eGPE), has been substituted by the correlation energy evaluated with Quantum Monte Carlo. We demonstrate the ability of the new functional to reproduce existing experimental data for the minimum critical number of atoms $N_\mathrm{c}$ required for droplet formation. $N_\mathrm{c}$ is a challenging quantity for theoretical predictions, and the eGPE provides only a qualitative description of it, mainly when it is applied to Dysprosium. We also use the new approach to characterize the BEC-supersolid transition. The quantum Monte Carlo based functional can be easily implemented in any existing eGPE code, improving the description of dipolar systems without increasing the computational cost.

cond-mat.quant-gas↗

arXiv2023

Vibrational dynamics of CO on Pd(111) in and out of thermal equilibrium

Using many-body perturbation theory and density functional perturbation theory, we study the vibrational spectra of the internal stretch (IS) mode of CO on Pd(111) for the bridge and hollow adsorption structures that are experimentally identified at 0.5~ML coverage. Our theoretical treatment allows us to determine the temperature dependence of the IS vibrational spectra under thermal conditions as well as the time evolution of the non-equilibrium transient spectra induced by femtosecond laser pulses. Under thermal conditions (i.e., for equal electronic $T_e$ and phononic $T_l$ temperatures), the calculated lifetimes at 10-150~K are mostly due to nonadiabatic couplings (NC), i.e., first-order electronic excitations. As temperature increases, also the contribution of the second-order electron mediated phonon-phonon couplings (EMPPC) progressively increases from 25\% at low temperatures to 50\% at 300~K. Our calculations for the laser-induced non-equilibrium conditions comprise experimental absorbed fluences of 6-130~J/m$^2$. For fluences for which $T_e>$2000~K, the transient vibrational spectra are characterized by two different regimes that follow the distinct time-evolution of $T_e$ and $T_l$ and are respectively dominated by NC and EMPPC processes. At lower fluences, the initial fast regime becomes progressively negligible as $T_e$ decreases and only the steady second regime remains visible. Qualitatively, all these spectral properties are common to the both adsorption structures studied here.

cond-mat.mtrl-sci↗

arXiv2023

Anomalous transient blueshift in the internal stretch mode of CO/Pd(111)

In time-resolved pump-probe vibrational spectroscopy the internal stretch mode of polar molecules is utilized as a key observable to characterize the ultrafast dynamics of adsorbates on surfaces. The adsorbates non-adiabatic intermode couplings are the commonly accepted mechanisms behind the observed transient frequency shifts. Here, we study the CO/Pd(111) system with a robust theoretical framework that includes electron-hole pair excitations and electron-mediated coupling between the vibrational modes. A mechanism is revealed that screens the electron-phonon interaction and originates a blueshift under ultrafast non-equilibrium conditions. The results are explained in terms of the abrupt change in the density of states around the Fermi level, and are instrumental for understanding dynamics at multi-component surfaces involving localized and standard $s$ or $p$ states.

cond-mat.mtrl-sci↗

arXiv2022

Adsorption and dissociation of diatomic molecules in monolayer $1H$-MoSe$_2$

Two dimensional transition metal dichalcogenides appear as good candidates for gas sensing and catalysis. Here, by means of density functional theory, we characterize the adsorption and dissociation of selected diatomic molecules (CO, H$_2$, O$_2$, and NO) on the MoSe$_2$ monolayer. We consider that these processes occur on the pristine $1H$-MoSe$_2$ monolayer and in the vicinity of an isolated Se vacancy. The presence of Se vacancies both enhances the molecular adsorption and reduces the energy needed for dissociation, making it energetically favorable for the case of O$_2$ and NO molecules. For each case we evaluate the effect that each adsorbate has on the electronic structure of the MoSe$_2$ monolayer and the charge transfer that takes place between the adsorbate and the surface. Remarkably, adsorption of either CO or NO at the Se vacancy induces a finite spin-magnetization in the system that is spatially well localized around the adsorbate and the three closest Mo atoms.

cond-mat.mtrl-sci↗

arXiv2021

Finite-range effects in the two-dimensional repulsive Fermi polaron

We study the repulsive Fermi polaron in a two-component, two-dimensional system of fermionic atoms inspired by the results of a recent experiment with $^{173}$Yb atoms [N. Darkwah Oppong \textit{et al.}, Phys. Rev. Lett. \textbf{122}, 193604 (2019)]. We use the diffusion Monte Carlo method to report properties such as the polaron energy and the quasi-particle residue that have been measured in that experiment. To provide insight on the quasi-particle character of the problem, we also report results for the effective mass. We show that the effective range, together with the scattering length, is needed in order to reproduce the experimental results. Using different model potentials for the interaction between the Fermi sea and the impurity, we show that it is possible to establish a regime of universality, in terms of these two parameters, that includes the whole experimental regime. This illustrates the relevance of quantum fluctuations and beyond mean-field effects to correctly describe the Fermi polaron problem.

cond-mat.quant-gas↗

arXiv2020

Reply to the Comment on "Berezinskii-Kosterlitz-Thouless Transition in Two-Dimensional Dipolar Stripes"

This is a Reply to the Comment from F. Cinti and M. Boninsegni on our recent work on the Berezinskii-Kosterlitz-Thouless (BKT) phase transition in a two-dimensional dipolar system [R.Bombín, F. Mazzanti and J. Boronat, Physical Review A 100, 063614 (2019)]. The main criticism about our work, expressed in that Comment, is that we did not explicitly report the two spatial contributions to the total superfluid fraction. Here, we analyze our results for a point of the phase diagram corresponding to the stripe phase, close to the gas to stripe transition line, and for a temperature below the BKT critical temperature. The scaling with the system size of the contribution to the superfluid fraction, coming from the direction in which spatial order appears, shows that it remains finite in the thermodynamic limit, as we already stated in our original work. This allow us to state that the stripe phase is superfluid at low temperatures. Furthermore, we offer some comments that help to understand where the differences between the results of Cinti and Boninsegni and ours comes from.

cond-mat.quant-gas↗

arXiv2020

Ultracold Bose and Fermi dipolar gases : a quantum Monte Carlo study

The object of study of this thesis are dipolar systems in the quantum degenerate regime. In general, dealing with many-body systems and evaluating their properties requires to deal with the Schrödinger equation. In the present study we employ different Monte Carlo methods, that are stochastic techniques that allow to find numerical solutions to it.

cond-mat.quant-gas↗

arXiv2019

Dilute dipolar quantum droplets beyond the extended Gross-Pitaevskii equation

Dipolar quantum droplets are exotic quantum objects that are self-bound due to the subtle balance of attraction, repulsion and quantum correlations. Here we present a systematic study of the critical atom number of these self-bound droplets, comparing the experimental results with extended mean-field Gross-Pitaevskii equation (eGPE) and quantum Monte-Carlo simulations of the dilute system. The respective theoretical predictions differ, questioning the validity of the current theoretical state-of-the-art description of quantum droplets within the eGPE framework and indicating that correlations in the system are significant. Furthermore, we show that our system can serve as a sensitive testing ground for many-body theories in the near future.

cond-mat.quant-gas↗

arXiv2019

Two-dimensional repulsive Fermi polarons with short and long-range interactions

We study the repulsive polaron problem in a two-component two-dimensional system of fermionic atoms. We use two different interaction models: a short-range (hard-disk) potential and a dipolar potential. In our approach, all the atoms have the same mass and we consider the system to be composed of a uniform bath of a single species and a single atomic impurity. We use the diffusion Monte Carlo method to evaluate polaron properties such as its chemical potential and pair distribution functions, together with a discussion on the deficit of volume induced by the impurity. We also evaluate observables that allow us to determine the validity of the quasi-particle picture: the quasi-particle residue and the effective mass of the polaron. Employing two different potentials allows us to identify the universality regime, where the properties depend only on the gas parameter $n a_s^2$ fixed by the bath density and the two-dimensional scattering length.

cond-mat.quant-gas↗