arXiv subjects

Alexandra Carvalho

Publications and source records attributed to Alexandra Carvalho.

At least 19 recordsLinked to original sources

arXiv2024

Predicting ionic conductivity in solids from the machine-learned potential energy landscape

Discovering new superionic materials is essential for advancing solid-state batteries, which offer improved energy density and safety compared to the traditional lithium-ion batteries with liquid electrolytes. Conventional computational methods for identifying such materials are resource-intensive and not easily scalable. Recently, universal interatomic potential models have been developed using equivariant graph neural networks. These models are trained on extensive datasets of first-principles force and energy calculations. One can achieve significant computational advantages by leveraging them as the foundation for traditional methods of assessing the ionic conductivity, such as molecular dynamics or nudged elastic band techniques. However, the generalization error from model inference on diverse atomic structures arising in such calculations can compromise the reliability of the results. In this work, we propose an approach for the quick and reliable screening of ionic conductors through the analysis of a universal interatomic potential. Our method incorporates a set of heuristic structure descriptors that effectively employ the rich knowledge of the underlying model while requiring minimal generalization capabilities. Using our descriptors, we rank lithium-containing materials in the Materials Project database according to their expected ionic conductivity. Eight out of the ten highest-ranked materials are confirmed to be superionic at room temperature in first-principles calculations. Notably, our method achieves a speed-up factor of approximately 50 compared to molecular dynamics driven by a machine-learning potential, and is at least 3,000 times faster compared to first-principles molecular dynamics.

cond-mat.mtrl-sci↗

arXiv2024

High capacity NbS2-based anodes for Li-ion batteries

We have investigated the lithium capacity of the 2H phase of niobium sulphide (NbS2) using density functional theory calculations and experiments. Theoretically, this material is found to allow the intercalation of a double layer of Li in between each NbS2 layer when in equilibrium with metal Li. The resulting specific capacity (340.8 mAh/g for the pristine material, 681.6 mAh/g for oxidized material) can reach more than double the specific capacity of graphite anodes. The presence of various defects leads to an even higher capacity with a partially reversible conversion of the material, indicating that the performance of the anodes is robust with respect to the presence of defects. Experiments in battery prototypes with NbS2-based anodes find a first specific capacity of about 1,130 mAh/g, exceeding the theoretical predictions.

cond-mat.mtrl-sci↗

arXiv2023

Theory of defect-mediated ionic transport in Li, Na and K beta and beta prime prime aluminas

Alkali metal $\beta$/$\beta^{\prime\prime}$ aluminas are among the fastest ionic conductors, yet little is understood about the role of defects in the ion transport mechanism. Here, we use density functional theory (DFT) to investigate the crystal structures of $\beta$ and $\beta^{\prime\prime}$ phases, and vacancy and interstitial defects in these materials. We find that charge transport is likely to be dominated by alkali metal interstitials in $\beta$-aluminas and by vacancies in $\beta^{\prime\prime}$ aluminas. Lower bounds for the activation energy for diffusion are found by determining the minimum energy paths for defect migration. The resulting migration barriers are lower than the experimental activation energies for conduction in Na $\beta$ and $\beta^{\prime\prime}$ aluminas, suggesting a latent potential for optimization. The lowest activation energy of about 20 meV is predicted for correlated vacancy migration in K $\beta^{\prime\prime}$ alumina.

cond-mat.mtrl-sci↗

arXiv2022

Direct calculation of the ionic mobility in superionic conductors

We describe an approach based on non-equilibrium molecular dynamics (NEMD) simulations to calculate the ionic mobility of solid ion conductors such as solid electrolytes from first-principles. The calculations are carried out in finite slabs of the material, where an electric field is applied and the dynamic response of the mobile ions is measured. We compare our results with those obtained from diffusion calculations, under the non-interacting ion approximation, and with experiment. This method is shown to provide good quantitative estimates for the ionic mobilities of two silver conductors, $α$-AgI and $α$-RbAg$_4$I$_5$. In addition to being convenient and numerically robust, this method accounts for ion-ion correlations at a much lower computational cost than exact approaches.

cond-mat.mtrl-sci↗

arXiv2022

Two-dimensional non-linear hydrodynamics and nanofluidics

A water monolayer squeezed between two solid planes experiences strong out-of-plane confinement effects while expanding freely within the plane. As a consequence, the transport of such two-dimensional water combines hydrodynamic and nanofluidic features, intimately linked with each other. In this paper, we propose and explicitly solve a non-linear hydrodynamic equation describing two-dimensional water flow with viscosity parameters deduced from molecular dynamic simulations. We demonstrate that the very ability of two-dimensional water to flow in short channels is governed by the second (dilatational) viscosity coefficient, leading to flow compression and velocity saturation in the high-pressure limit. The viscosity parameter values depend strongly on whether graphene or hexoganal boron nitride layers are used to confine 2D water that offers an interesting opportunity to obtain various nanofluids out of the same water molecules just by using alternate materials to fabricate the 2D channels.

cond-mat.mtrl-sci↗

arXiv2022

Edge-Driven Phase Transitions in 2D Ice

2D water, confined by atomically flat layered materials, may transit into various crystalline phases even at room temperature. However, to gain full control over the crystalline state, we should not only confine water in the out of plane direction but also restrict its in plane motion, forming 2D water clusters or ribbons. One way to do this is by using an electric field, in particular the intrinsic electric field of an adjacent polar material. We have found that the crystalline phases of 2D water clusters placed between two hexagonal boron nitride hBN nanoribbons are crucially determined by the nanoribbons edges, the resulting polarity of the nanoribbons, and their interlayer distance. We make use of density functional theory with further assistance of molecular dynamics simulations to establish the comprehensive phase diagrams demonstrating transitions between liquid and solid phases and between the states of different crystalline orders. We also show that the crystalline orders are maintained when water flows between hBN channels under external pressure. Our results open a promising pathway towards the control of water structure and its flow by the use of the microscopic electric field of polar materials.

cond-mat.mtrl-sci↗

arXiv2022

Microscopic theory of ionic motion in solids

Drag and diffusion of mobile ions in solids are of interest for both purely theoretical and applied scientific communities. This article proposes a theoretical description of ion drag in solids that can be used to estimate ionic conductivities in crystals, and forms a basis for the rational design of solid electrolyte materials. Starting with a general solid-state Hamiltonian, we employ the non-equilibrium path integral formalism to develop a microscopic theory of ionic transport in solids in the presence of thermal fluctuations. As required by the fluctuation-dissipation theorem, we obtain a relation between the variance of the random force and friction. Because of the crystalline nature of the system, however, the two quantities are tensorial. We use the drag tensor to write down the formula for ionic mobility, determined by the potential profile generated by the crystal's ions.

cond-mat.mes-hall↗

arXiv2021

Microscopic theory of ionic motion in solid electrolytes

We propose a microscopic, first-principles description of the ionic conduction in crystals. This formalism allows us to gain new insights into the ideal characteristics of general ionic conducting materials and, in particular, solid electrolytes. Using \textit{ab initio} calculations, we show that our formalism results in ionic mobilities consistent with experiments for several materials. Our work opens the possibility of developing solid electrolytes based on fundamental physical principles rather than empirical descriptions of the underlying processes.

cond-mat.mtrl-sci↗

arXiv2021

Collective Excitations in 2D Materials

Research on 2D materials has been one of the fastest-growing fields in condensed matter physics and materials science in the past 10 years. The low dimensionality and strong correlations of 2D systems give rise to electronic and structural properties, in the form of collective excitations, that do not have counterparts in ordinary 3D materials used in modern technology. These 2D materials present extraordinary opportunities for new technologies, such as in flexible electronics. In this Review, we focus on plasmons, excitons, phonons and magnons in 2D materials. We discuss the theoretical formalism of these collective excitations and elucidate how they differ from their 3D counterparts.

cond-mat.mes-hall↗

arXiv2020

Tunable van Hove Singularities and Correlated States in Twisted Trilayer Graphene

Understanding and tuning correlated states is of great interest and significance to modern condensed matter physics. The recent discovery of unconventional superconductivity and Mott-like insulating states in magic-angle twisted bilayer graphene (tBLG) presents a unique platform to study correlation phenomena, in which the Coulomb energy dominates over the quenched kinetic energy as a result of hybridized flat bands. Extending this approach to the case of twisted multilayer graphene would allow even higher control over the band structure because of the reduced symmetry of the system. Here, we study electronic transport properties in twisted trilayer graphene (tTLG, bilayer on top of monolayer graphene heterostructure). We observed the formation of van Hove singularities which are highly tunable by twist angle and displacement field and can cause strong correlation effects under optimum conditions, including superconducting states. We provide basic theoretical interpretation of the observed electronic structure.

cond-mat.mes-hall↗

arXiv2019

Next-to-leading-order predictions for single vector-like quark production at the LHC

We propose simulation strategies for single production of third generation vector-like quarks at the LHC, implementing next-to-leading-order corrections in QCD and studying in detail their effect on cross sections and differential distributions. We also investigate the differences and the relative incertitudes induced by the use of the Four-Flavour Number Scheme ${\it versus}$ the Five-Flavour Number Scheme. As a phenomenological illustration, we concentrate on the production of vector-like quarks coupling to the third generation of the Standard Model in association with a jet and assuming standard couplings to gauge and Higgs bosons.

hep-ph↗

arXiv2018

Single production of vector-like quarks with large width at the Large Hadron Collider

Vector-Like Quarks (VLQs) are predicted by several theoretical scenarios of new physics and, having colour quantum numbers, can copiously be produced at the Large Hadron Collider (LHC), so long that their mass is in the testable kinematic regime of such a machine. While it would be convenient to assume that such objects are narrow and can be treated in the so-called Narrow Width Approximation (NWA), this is not always possible, owing to the fact that couplings and particle content of such new physics scenarios are not generally constrained, so that a large value of the former and/or a large variety of VLQ decay channels into the latter can contribute to generate a large decay width for such extra quarks. We have addressed here the issue of how best to tackle in LHC analysis the presence of large (and model-dependent) interference effects between different VLQ production and decay channels as well as between these and the corresponding irreducible background. We have confined ourselves to the case of single production of VLQs, which is rapidly becoming a channel of choice in experimental searches owing to the ever increasing limits on their mass, in turn depleting the yield of the historically well-established double production channel. Indeed, this poses a further challenge, as the former is model-dependent while the latter is essentially not. Despite these conditions, we show here that an efficient approach is possible, which retains to a large extent a degree of model independence in phenomenological studies of such VLQ dynamics at the LHC.

hep-ph↗

arXiv2018

Gravity particles from Warped Extra Dimensions, predictions for LHC

Warped Extra Dimension scenarios are a rich playground for phenomenology of heavy resonances at LHC. The Radion and the KK-graviton are inevitable signatures of this class of models. On face of the latest LHC experimental results on the direct searches for Beyond Standard Model physics we update the phenomenological predictions for production and decay of such resonances in its main production modes. We also highlight the phenomenology results relevant to collider searches in individual channels, and provide tools for interpretation of current and future experimental analyses using two specific benchmarks as example.

hep-ph↗

arXiv2017

Two-dimensional Square Buckled Rashba Lead Chalcogenides

We propose the lead sulphide (PbS) monolayer as a 2D semiconductor with a large Rashba-like spin-orbit effect controlled by the out-of-plane buckling. The buckled PbS conduction band is found to possess Rashba-like dispersion and spin texture at the $M$ and $Γ$ points, with large effective Rashba parameters of $λ\sim5~$eV$Å~$ and $λ\sim1~$eV$~Å$, respectively. Using a tight-binding formalism, we show that the Rashba effect originates from the very large spin-orbit interaction and the hopping term that mixes the in-plane and out-of-plane $p$ orbitals of Pb and S atoms. The latter, which depends on the buckling angle, can be controlled by applying strain to vary the spin texture as well as the Rashba parameter at $Γ$ and $M$. Our density functional theory results together with tight-binding formalism provide a unifying framework for designing Rashba monolayers and for manipulating their spin properties.

cond-mat.mtrl-sci↗

arXiv2017

On the reinterpretation of non-resonant searches for Higgs boson pairs

The detection of production of a pair of Higgs bosons before the end of LHC operation would be clear evidence of New Physics (NP). As searches for non-resonant production of Higgs pairs are being designed it is of particular importance to be able to conveniently present current experimental results in terms of limits in the most 'model-independent' fashion possible. In this article we provide an analytic parametrization of the {\it differential} Higgs-pair production at the LHC in the effective field theory (EFT) extension of the SM. It results from a fit to the theory prediction for the $gg \to hh$ cross section at the 13\,TeV at the LHC. Subsequently the resulting formula is used for a reweighing technique that allows to recast exclusion bounds from ATLAS and CMS HH$\toγγ\,b\bar{b}$ searches to any point of the considered EFT parameter space. We demonstrate with a fast simulation of the LHC detectors that with this approach it is possible to cover the continuously of the EFT parameter space, taking correctly into account the efficiencies of signal selections, without the necessity of rerunning a large number of full detector simulations. Finally, the resulting exclusion bounds are confronted to several explicit models such as setups with additional scalars, including 2HDM, vector-like fermions, and minimal composite Higgs models, mapped to the EFT.

hep-ph↗

arXiv2017

Oxygen passivation mediated tunability of trion and excitons in MoS$_2$

Using wide spectral range in situ spectroscopic ellipsometry with systematic ultra high vacuum annealing and in situ exposure to oxygen, we report the complex dielectric function of MoS$_2$ isolating the environmental effects and revealing the crucial role of unpassivated and passivated sulphur vacancies. The spectral weights of the A ($1.92$ eV) and B ($2.02$ eV) exciton peaks in the dielectric function reduce significantly upon annealing, accompanied by spectral weight transfer in a broad energy range. Interestingly, the original spectral weights are recovered upon controlled oxygen exposure. This tunability of the excitonic effects is likely due to passivation and reemergence of the gap states in the bandstructure during oxygen adsorption and desorption, respectively, as indicated by ab initio density functional theory calculation results. This work unravels and emphasizes the important role of adsorbed oxygen in the optical spectra and many-body interactions of MoS$_2$.

cond-mat.mes-hall↗

arXiv2017

Probing vector-like quark models with Higgs-boson pair production

We investigate Higgs-boson pair production at the LHC when the final state system arises from decays of vector-like quarks coupling to the Higgs boson and the Standard Model quarks. Our phenomenological study includes next-to-leading-order QCD corrections, which are important to guarantee accurate predictions, and focuses on a detailed analysis of a di-Higgs signal in the four $b$-jet channel. Whereas existing Run II CMS and ATLAS analyses are not specifically designed for probing non-resonant, vector-like-quark induced, di-Higgs production, we show that they nevertheless offer some potential for these modes. We then investigate the possibility of distinguishing between the various di-Higgs production mechanisms by exploiting the kinematic properties of the signal.

hep-ph↗

arXiv2017

Spin-Orbit Dirac Fermions in 2D Systems

We propose a novel model for including spin-orbit interactions in buckled two dimensional systems. Our results show that in such systems, intrinsic spin-orbit coupling leads to a formation of Dirac cones, similar to Rashba model. We explore the microscopic origins of this behaviour and confirm our results using DFT calculations.

cond-mat.mes-hall↗