arXiv subjects

Jaime Ferrer

Publications and source records attributed to Jaime Ferrer.

At least 19 recordsLinked to original sources

arXiv2026

Magnetic ground states of CrPS$_4$ and NiPS$_3$ monolayers from long-range exchange interactions

We investigate the magnetic properties of monolayer CrPS$_4$ and NiPS$_3$ by combining first-principles calculations, second-principles spin models, and Monte Carlo simulations. Unlike conventional approaches that truncate exchange interactions after only a few shells and determine them by fitting total energies, we extract the magnetic exchange tensors directly from density functional theory using the LKAG formalism and include interactions until numerical convergence is achieved. We show that long-range exchange interactions qualitatively modify the magnetic behavior of both materials. In CrPS$_4$, they destabilize the previously predicted ferromagnetic ground state and stabilize a spin-spiral phase, reducing the critical temperature to about 21\,K, in agreement with available experiments. The resulting magnetic phase diagram contains multiple collinear and non-collinear phases that can be tuned by temperature and external magnetic fields. In NiPS$_3$, the experimentally observed zigzag antiferromagnetic order only emerges when exchange interactions up to the fifth shell are included. These results demonstrate that quantitatively predictive spin models for thiophosphate monolayers require long-range exchange interactions and provide a predictive framework for accurately describing two-dimensional van der Waals magnets.

cond-mat.mtrl-sci↗

arXiv2026

Proximity-Induced Spin Reorientation in Monolayer CrI$_3$ on Hexagonal WTe$_2$

Magnetic anisotropy controls the orientation and thermal stability of two-dimensional magnetic order. Predicting proximity-induced changes in anisotropy requires linking the electronic structure to microscopic magnetic interactions and finite-temperature behavior. Here we study monolayer CrI$_3$ on hexagonal WTe$_2$ using a first-principles-to-finite-temperature workflow centered on relativistic spin-Hamiltonian mapping. We find that WTe$_2$ reorients the CrI$_3$ magnetization from out-of-plane to in-plane and substantially enhances the magnetic ordering scale within the extracted spin models. Analysis of the extracted spin Hamiltonians shows that the reorientation is driven by a substrate-induced change in the balance between symmetric anisotropic exchange and onsite anisotropy. We establish a transferable workflow for proximity-controlled magnetism in two-dimensional van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2026

Strain induced magnetic phase transitions in Fe3GeTe2 monolayer

We investigate the magnetic properties of a monolayer of Fe3GeTe2 as a function of the lattice constant by combining first-principles calculations with atomistic spin dynamics simulations. The calculated magnetic exchange interactions reveal a competition between ferromagnetic and antiferromagnetic couplings, with the latter being significantly strengthened under compressive strain. Stochastic Landau-Lifshitz-Gilbert simulations reveal a substantial decrease in the Curie temperature with decreasing lattice constant, and predict a transition of the magnetic ground state from a ferromagnetic configuration to a conical spin-spiral state. We introduce a simple spin-model which explains the stabilization of the spiral phase due to competing exchange interactions. We found multiple magnetic phase transitions involving ferromagnetic, conical spin-spiral, and planar Neel states, depending on both the lattice constant and the temperature. The absence of Dzyaloshinskii-Moriya interactions is found to significantly reduce the Neel temperature, while leaving the Curie temperature largely unaffected. Our findings reveal the importance of lattice distortions in controlling complex magnetic phases and their evolution with temperature.

cond-mat.mtrl-sci↗

arXiv2025

Graphene-based quantum heterospin graphs

We investigate from first principles a variety of low-dimensional open quantum spin systems based on magnetic nanographene structures that contain spin-1/2 and spin-1 triangulenes and/or olympicenes. These graphene nanostructures behave as localized spins and can be effectively described by a quantum bilinear-biquadratic Heisenberg Hamiltonian, for which we will compute the energy spectrum and the quantum numbers associated with the low-energy eigenstates. We propose the experimental realization of antiferromagnetic alternating spin chains using these graphene nanostructures, which result in ferrimagnetic systems whose ground state spin and degeneracy depend on the length of the chain. We identify a double degeneracy in the total spin quantum number $S$ of the first excited state in three-leg spin graphs (3-LSGs) and other heterospin nanostructures, which depends on both the number of sites and the spin species, and originates from the swapping transformation symmetry of the Hamiltonian. Numerical simulations indicate that this degeneracy remains largely robust for $N=7$ spin-1 3-LSGs under realistic perturbations present in experimental conditions.

cond-mat.mes-hall↗

arXiv2025

Reference lattice, sound, stiffness, and magnetic transitions of Ising monolayers

A reference lattice, away from which elastic distortions induced by the spin texturing of 2D magnets take hold, is motivated from a picture of pairwise Biot-Savart interactions among identical solenoids that either elongate or compress a (``zero-current'') spring lattice. Applied to a paradigmatic CrSiTe$_3$ monolayer (ML), the reference is given by the average between the atomic positions of FM and N\'eel AFM lattices; such an atomic disposition permits understanding structural distortions and elastic energies due to magnetism readily. Furthermore, the anisotropic speed of sound in the magnetic ground state explains an observed anisotropy of vibrational frequencies on similar magnets. Elastic stiffness constants are reported, too. Magnetic energies in four Ising structural configurations were calculated, and the strain needed for those 2D magnets to undergo an AFM to FM quantum phase transition was determined as well.

cond-mat.mtrl-sci↗

arXiv2025

Spin Wave Dispersion of the van der Waals Antiferromagnet NiPS$_3$

We calculate the magnon dispersion spectra of the two-dimensional zigzag van der Waals antiferromagnet NiPS$_3$ for monolayer, bilayer, and bulk systems as a function of an external magnetic field. We calculate the exchange and anisotropy constants in our spin model by first principles. We can accurately explain the transition from a collinear to a canted ground state for a magnetic field applied normal to the (in-plane) easy-axis, and a spin-flop transition when the field is parallel to it. A topologically protected Dirac nodal line is present and robust with respect to both external and anisotropy fields.

cond-mat.mes-hall↗

arXiv2024

Programmable Magnetic Hysteresis in Orthogonally-Twisted Two-Dimensional CrSBr Magnets via Stacking Engineering

Twisting two-dimensional van der Waals magnets allows the formation and control of different spin-textures, as skyrmions or magnetic domains. Beyond the rotation angle, different spin reversal processes can be engineered by increasing the number of magnetic layers forming the twisted van der Waals heterostructure. Here, we consider pristine monolayers and bilayers of the A-type antiferromagnet CrSBr as building blocks. By rotating 90 degrees these units, we fabricate symmetric (monolayer/monolayer and bilayer/bilayer) and asymmetric (monolayer/bilayer) heterostructures. The magneto-transport properties reveal the appearance of magnetic hysteresis, which is highly dependent upon the magnitude and direction of the applied magnetic field and is determined not only by the twist-angle but also by the number of layers forming the stack. This high tunability allows switching between volatile and non-volatile magnetic memory at zero-field and controlling the appearance of abrupt magnetic reversal processes at either negative or positive field values on demand. The phenomenology is rationalized based on the different spin-switching processes occurring in the layers, as supported by micromagnetic simulations. Our results highlight the combination between twist-angle and number of layers as key elements for engineering spin-switching reversals in twisted magnets, of interest towards the miniaturization of spintronic devices and realizing novel spin textures.

cond-mat.mes-hall↗

arXiv2024

Tuning magnetic exchange interactions in 2D magnets: the case of CrGeX$_3$ (X = Se, Te) and Janus Cr$_2$Ge$_2$(Se,Te)$_3$ monolayers

We present a computational study to explore the potential of different experimental approaches to tune the magnetic interactions in two-dimensional van der Waals magnets. We selected CrGeSe$_3$, CrGeTe$_3$, and Janus Cr$_2$Ge$_2$(Se,Te)$_3$ monolayers as case studies and calculated the full exchange tensors among all relevant atomic pairs and analyze their dependence on different external parameters, such as biaxial and uniaxial strain, as well as gate voltage. We pay special attention to interactions that emerge or vanish due to changes of the symmetry of the system. We find that biaxial and uniaxial strains significantly modify isotropic exchange couplings, which can lead to a transition from a ferromagnetic to an antiferromagnetic phase, while a gate voltage induces Dzyaloshinskii-Moriya interactions, forming a vortex pattern whose chirality is determined by the sign of the electric field. The electric dipole moment of the Janus material is large, raising the possibility of multiferroic behaviour. The polarizability is similar for the three compounds.

cond-mat.mes-hall↗

arXiv2024

Stacking-engineered ferroelectricity and multiferroic order in van der Waals magnets

Two-dimensional (2D) materials that exhibit spontaneous magnetization, polarization or strain (referred to as ferroics) have the potential to revolutionize nanotechnology by enhancing the multifunctionality of nanoscale devices. However, multiferroic order is difficult to achieve, requiring complicated coupling between electron and spin degrees of freedom. We propose a universal method to engineer multiferroics from van der Waals magnets by taking advantage of the fact that changing the stacking between 2D layers can break inversion symmetry, resulting in ferroelectricity and possibly magnetoelectric coupling. We illustrate this concept using first-principles calculations in bilayer NiI$_2$, which can be made ferroelectric upon rotating two adjacent layers by $180^{\circ}$ with respect to the bulk stacking. Furthermore, we discover a novel multiferroic order induced by interlayer charge transfer which couples the interlayer spin order and electronic polarization. Our approach is not only general but also systematic, and can enable the discovery of a wide variety of 2D multiferroics.

cond-mat.mtrl-sci↗

arXiv2024

Solution of the mean-field Hubbard model of graphene rectangulenes

We present a complete analytical solution of the mean-field Hubbard model of undoped and doped graphene rectangulenes. These are non-chiral ribbons of arbitrary length and width, whose dimensions range from simple short acene molecules all the way up to the bulk limit. We rewrite the Hubbard model in the basis of bulk and edge non-interacting eigen-states, and provide explicit expressions for the Coulomb matrix elements. We present a general mean-field decoupling of the Hamiltonian, and discuss in detail the paramagnetic, ferromagnetic and antiferromagnetic mean-field solutions. We calculate the eigen-energies, occupations, spin densities and addition energies of rectangulenes with lengths and widths ranging from a nanometer to several hundreds of them. We rewrite the exact mean-field tight-binding Hamiltonian back in the site-occupation basis, that can be used to model electronic, thermo-electric, transport and optical properties of experimental-size graphene flakes.

cond-mat.str-el↗

arXiv2023

Relativistic magnetic interactions from non-orthogonal basis sets

We propose a method to determine the magnetic exchange interaction and on-site anisotropy tensors of extended Heisenberg spin models from density functional theory including relativistic effects. The method is based on the Liechtenstein-Katsnelson-Antropov-Gubanov torque formalism, whereby energy variations upon infinitesimal rotations are performed. We assume that the Kohn-Sham Hamiltonian is expanded in a non-orthogonal basis set of pseudo-atomic orbitals. We define local operators that are both hermitian and satisfy relevant sum rules. We demonstrate that in the presence of spin-orbit coupling a correct mapping from the density functional total energy to a spin model that relies on the rotation of the exchange field part of the Hamiltonian can not be accounted for by transforming the full Hamiltonian. We derive a set of sum rules that pose stringent validity tests on any specific calculation. We showcase the flexibility and accuracy of the method by computing the exchange and anisotropy tensors of both well-studied magnetic nanostructures and of recently synthesized two-dimensional magnets. Specifically, we benchmark our approach against the established Korringa-Kohn-Rostoker Green's function method and show that they agree well. Finally, we demonstrate how the application of biaxial strain on the two-dimensional magnet T-CrTe2 can trigger a magnetic phase transition.

cond-mat.mtrl-sci↗

arXiv2022

Relevance of Shockley states on the electrical and thermoelectric response of gold-based single-molecule junctions

Noble metals break preferably exposing (111)-oriented surfaces, that host Shockley type surface states (SSs). Nevertheless, the relevance of SSs on the electrical properties of gold-based molecular junctions has not been explored in detail yet. Here, we present ab initio simulations that show how the gold (111) SS, that lies approximately 0.5 eV below the Fermi energy, is key to determining correctly the electrical and thermoelectric response of the above junctions. We show how the ability to shift in a controlled way the energy position of gold SS enables us to tune the electrical and thermoelectric response of gold molecular junctions. We also show that gold's SS appears in our simulations only if the 5d orbitals are included explicitly in the valence shell. To illustrate this behaviour, we discuss in detail Benzenediamine (BDA) and Benzenedicarbonitrile (BDCN) gold (111) junctions.

cond-mat.mes-hall↗

arXiv2022

Electrically driven singlet-triplet transition in triangulene spin-1 chains

Recently, graphene triangulene chains have been synthesized and their magnetic response has been analyzed by STM methods by Mishra and coworkers (Nature 598, 287 (2021)). Motivated by this study, we determine the exchange bilinear and biquadratic constants of the triangulene chains by calculating two-spin rotations in the spirit of the magnetic force theorem. We then analyze open-ended, odd-numbered chains, whose edge states pair up forming a triplet ground state. We propose three experimental approaches that enable us to trigger and control a singlet-triplet spin transition. Two of these methods are based on applying a mechanical distortion to the chain. We finally show that the transition can be controlled efficiently by the application of an electric field.

cond-mat.mes-hall↗

arXiv2020

SIESTA: recent developments and applications

A review of the present status, recent enhancements, and applicability of the SIESTA program is presented. Since its debut in the mid-nineties, SIESTA's flexibility, efficiency and free distribution has given advanced materials simulation capabilities to many groups worldwide. The core methodological scheme of SIESTA combines finite-support pseudo-atomic orbitals as basis sets, norm-conserving pseudopotentials, and a real-space grid for the representation of charge density and potentials and the computation of their associated matrix elements. Here we describe the more recent implementations on top of that core scheme, which include: full spin-orbit interaction, non-repeated and multiple-contact ballistic electron transport, DFT+U and hybrid functionals, time-dependent DFT, novel reduced-scaling solvers, density-functional perturbation theory, efficient Van der Waals non-local density functionals, and enhanced molecular-dynamics options. In addition, a substantial effort has been made in enhancing interoperability and interfacing with other codes and utilities, such as Wannier90 and the second-principles modelling it can be used for, an AiiDA plugin for workflow automatization, interface to Lua for steering SIESTA runs, and various postprocessing utilities. SIESTA has also been engaged in the Electronic Structure Library effort from its inception, which has allowed the sharing of various low level libraries, as well as data standards and support for them, in particular the PSML definition and library for transferable pseudopotentials, and the interface to the ELSI library of solvers. Code sharing is made easier by the new open-source licensing model of the program. This review also presents examples of application of the capabilities of the code, as well as a view of on-going and future developments.

physics.comp-ph↗

arXiv2020

A Mechanically Tunable Quantum Dot in a Graphene Break Junction

Graphene quantum dots (QDs) are intensively studied as platforms for the next generation of quantum electronic devices. Fine tuning of the transport properties in monolayer graphene QDs, in particular with respect to the independent modulation of the tunnel barrier transparencies, remains challenging and is typically addressed using electrostatic gating. We investigate charge transport in back-gated graphene mechanical break junctions and reveal Coulomb blockade physics characteristic of a single, high-quality QD when a nanogap is opened in a graphene constriction. By mechanically controlling the distance across the newly-formed graphene nanogap, we achieve reversible tunability of the tunnel coupling to the drain electrode by five orders of magnitude, while keeping the source-QD tunnel coupling constant. These findings indicate that the tunnel coupling asymmetry can be significantly modulated with a mechanical tuning knob and has important implications for the development of future graphene-based devices, including energy converters and quantum calorimeters.

cond-mat.mes-hall↗

arXiv2018

Exchange interactions from a nonorthogonal basis set: from bulk ferromagnets to the magnetism in low-dimensional graphene systems

We present a computational method to determine the exchange constants in isotropic spin models. The method uses the Hamiltonian and overlap matrices computed from density functional schemes that are based on nonorthogonal basis sets. We demonstrate that the new method as implemented in the SIESTA code reproduces the Heisenberg interactions of simple metallic bulk ferromagnets as obtained from former well--established computational approaches. Then we address $sp$ magnetism in graphene nanostructures. For fluorinated graphene we obtain exchange interactions in fairly good agreement with previous calculations using maximally localized Wannier functions and we confirm the theoretical prediction of a 120$^\circ$ N\'eel state. Associated with the magnetic edge-states of a zigzag graphene nanoribbon we find rapidly decaying exchange interactions, however, with an unconventional distance dependence of $\exp(-\sqrt{r/\delta})$. We show that the stiffness constant derived from the exchange interactions is consistent with previous estimate based on total energy differences of twisted spin configurations. We highlight that our method is an efficient tool for the analysis of novel hybrid nano-structures where metallic and organic components are integrated to form exotic magnetic patterns.

cond-mat.mes-hall↗

arXiv2018

Spin-State dependent Conductance Switching in Single Molecule-Graphene Junctions

Spin-crossover (SCO) molecules are versatile magnetic switches with applications in molecular electronics and spintronics. Downscaling devices to the single-molecule level remains, however, a challenging task since the switching mechanism in bulk is mediated by cooperative intermolecular interactions. Here, we report on electron transport through individual Fe-SCO molecules coupled to few-layer graphene electrodes \textit{via} $\pi - \pi$ stacking. We observe a distinct bistability in the conductance of the molecule and a careful comparison with density functional theory (DFT) calculations allows to associate the bistability with a SCO-induced orbital reconfiguration of the molecule. We find long spin-state lifetimes that are caused by the specific coordination of the magnetic core and the absence of intermolecular interactions according to our calculations. In contrast with bulk samples, the SCO transition is not triggered by temperature but induced by small perturbations in the molecule at any temperature. We propose plausible mechanisms that could trigger the SCO at the single-molecule level.

cond-mat.mes-hall↗

arXiv2018

Mechanically Controlled Quantum Interference in Graphene Break Junctions

The ability to detect and distinguish quantum interference signatures is important for both fundamental research and for the realization of devices including electron resonators, interferometers and interference-based spin filters. Consistent with the principles of subwavelength optics, the wave nature of electrons can give rise to various types of interference effects, such as Fabry-P\'erot resonances, Fano resonances and the Aharonov-Bohm effect. Quantum-interference conductance oscillations have indeed been predicted for multiwall carbon nanotube shuttles and telescopes, and arise from atomic-scale displacements between the inner and outer tubes. Previous theoretical work on graphene bilayers indicates that these systems may display similar interference features as a function of the relative position of the two sheets. Experimental verification is, however, still lacking. Graphene nanoconstrictions represent an ideal model system to study quantum transport phenomena due to the electronic coherence and the transverse confinement of the carriers. Here, we demonstrate the fabrication of bowtie-shaped nanoconstrictions with mechanically controlled break junctions (MCBJs) made from a single layer of graphene. We find that their electrical conductance displays pronounced oscillations at room temperature, with amplitudes that modulate over an order of magnitude as a function of sub-nanometer displacements. Surprisingly, the oscillations exhibit a period larger than the graphene lattice constant. Charge-transport calculations show that the periodicity originates from a combination of quantum-interference and lattice-commensuration effects of two graphene layers that slide across each other. Our results provide direct experimental observation of Fabry-P\'erot-like interference of electron waves that are partially reflected/transmitted at the edges of the graphene bilayer overlap region.

cond-mat.mes-hall↗