arXiv subjects

Flaviano José dos Santos

Publications and source records attributed to Flaviano José dos Santos.

13 recordsLinked to original sources

arXiv2026

Probing the real-space density of spin-entangled electrons

On the textbook example of an isolated antiferromagnetic Heisenberg dimer, we demonstrate that the magnetic form factor and the magnetic electron density distribution can be extracted from the momentum-dependence of the inelastic neutron scattering (INS) intensity of a magnetic excitation. We measure the three-dimensional (3D) magnetic structure factor of the singlet-to-triplet excitation in Cu(II) acetate monohydrate with INS. Using a minimal parametrization of the magnetic electron density, we deduce the real-space density of the spin-entangled electrons and the transfer of magnetic electron density between metal and ligand atoms from the experimental data. Density functional theory (DFT) calculations reproduce the measured structure factor quantitatively, providing a direct validation of DFT broken-symmetry spin densities against full 3D INS data. The quantitative agreement between experiment, parametrization, and theory establishes a robust framework for determining magnetic form factors and the magnetic electron density in a broad range of magnetic materials and demonstrates INS as a probe of the envelope of spatial electronic wavefunctions.

cond-mat.str-el↗

arXiv2026

Spin fluctuations steer the electronic behavior in the FeSb$_{3}$ skutterudite

Skutterudites are promising materials for thermoelectric and spintronics applications. Here we explore spin fluctuations in the FeSb$_{3}$ skutterudite and their effect on its electronic structure using Hubbard-corrected density-functional theory calculations. We identify multiple magnetic and charge-disproportionated configurations, with an antiferromagnetic metallic ground state. Paramagnetic fluctuations modeled through a special quasirandom spin structure open a 61 meV gap, consistent with experiments. This state features non-degenerate spin channels and band-avoided crossings, resembling a Luttinger-compensated ferrimagnet. Mapping the electronic structure to a Heisenberg Hamiltonian fails to explain the low Néel temperature ($\lesssim$10 K), suggesting that factors such as stoichiometry and magnetic exchange frustration may play an important role, calling for more detailed experimental investigations.

cond-mat.mtrl-sci↗

arXiv2026

Comparative study of magnetic exchange parameters and magnon dispersions in NiO and MnO from first principles

Spin-wave excitations are fundamental to understanding the behavior of magnetic materials and hold promise for future information and communication technologies. Yet, modeling these accurately in transition-metal compounds remains challenging, starting from the self-interaction errors affecting localized and partially filled $d$-orbitals in density-functional theory (DFT) with (semi-)local functionals. In this work, we compare three advanced first-principles approaches for computing magnetic exchange parameters and magnon dispersions in NiO and MnO, all based on a common DFT+$U$ ground state with ab initio Hubbard $U$ values obtained from density-functional perturbation theory. Two methods extract exchange parameters directly: one via total-energy differences using the four-state mapping ($ΔE$), and the other via the magnetic force theorem (MFT) using infinitesimal spin rotations. Magnon dispersions are then obtained from a Heisenberg Hamiltonian through linear spin-wave theory (LSWT). The third approach, time-dependent density-functional perturbation theory with $U$ (TDDFPT+$U$), yields magnon dispersions directly from the dynamical spin susceptibility, with exchange parameters fitted a posteriori, for comparison, via LSWT. Our results show that TDDFPT+$U$ and the Heisenberg model based on $ΔE$-derived parameters align well with experimental neutron scattering data, whereas the MFT-based approach shows larger discrepancies, possibly due to some inherent approximations and limitations of the particular implementation used. This study benchmarks the accuracy of state-of-the-art first-principles techniques for spin-wave modeling and contributes to advancing reliable computational tools for the study and design of magnetic materials.

cond-mat.mtrl-sci↗

arXiv2025

Accurate and efficient protocols for high-throughput first-principles materials simulations

Advancements in theoretical and algorithmic approaches, workflow engines, and an ever-increasing computational power have enabled a novel paradigm for materials discovery through first-principles high-throughput simulations. A major challenge in these efforts is to automate the selection of parameters used by simulation codes to deliver numerical precision and computational efficiency. Here, we propose a rigorous methodology to assess the quality of self-consistent DFT calculations with respect to smearing and $k$-point sampling across a wide range of crystalline materials. For this goal, we develop criteria to reliably estimate average errors on total energies, forces, and other properties as a function of the desired computational efficiency, while consistently controlling $k$-point sampling errors. The present results provide automated protocols (named standard solid-state protocols or SSSP) for selecting optimized parameters based on different choices of precision and efficiency tradeoffs. These are available through open-source tools that range from interactive input generators for DFT codes to high-throughput workflows.

cond-mat.mtrl-sci↗

arXiv2025

Optical signatures of spin symmetries in unconventional magnets

The concept of spin symmetries has gained renewed interest as a valuable tool for classifying unconventional magnetic phases, including altermagnets and recently identified p-wave magnets. In this work, we show that in compounds with weak spin-orbit coupling, the dominant spin and charge photoresponse is determined by spin group rather than the conventional magnetic group symmetry. As a concrete realization we consider the nonlinear shift photocurrent in Mn$_5$Si$_3$, a material that features the two possible classes of unconventional p-wave magnetism in the form of two competing spin structures, a coplanar and non-coplanar one. While both are predicted to generate shift currents based on magnetic symmetry considerations, only the non-coplanar configuration survives the spin symmetry requirements. This is numerically confirmed by our $\textit{ab-initio}$ calculations, providing a protocol to experimentally identify the spin configuration of this promising material in photogalvanic or transport measurements.

cond-mat.mes-hall↗

arXiv2023

Fermi energy determination for advanced smearing techniques

Smearing techniques are widely used in first-principles calculations of metallic and magnetic materials, where they improve the accuracy of Brillouin zone sampling and lessen the impact of level-crossing instabilities. Smearing introduces a fictitious electronic temperature that smooths the discontinuities of the integrands; consequently, a corresponding fictitious entropic term arises, and needs to be considered in the total free energy functional. Advanced smearing techniques -- such as Methfessel-Paxton and cold smearing -- have been introduced to guarantee that the system's total free energy remains independent of the smearing temperature at least up to the second order. In doing so, they give rise to non-monotonic occupation functions (and, for Methfessel-Paxton, non-positive definite), which can result in the chemical potential not being uniquely defined. We explore this shortcoming in detail and introduce a numerical protocol utilizing Newton's minimization method that is able to identify the desired Fermi energy. We validate the method by calculating the Fermi energy of $\sim$20,000 materials and comparing it with the results of standard bisection approaches. In passing, we also highlight how traditional approaches, based on Fermi-Dirac or Gaussian smearing, are actually equivalent for all practical purposes, provided the smearing width is appropriately renormalized by a factor $\sim$2.565.

cond-mat.mtrl-sci↗

arXiv2021

Topological magnon insulators in two-dimensional van der Waals ferromagnets CrSiTe$_3$ and CrGeTe$_3$: towards intrinsic gap-tunability

The bosonic analogues of topological insulators have been proposed in numerous theoretical works, but their experimental realization is still very rare, especially for spin systems. Recently, two-dimensional (2D) honeycomb van der Waals (vdW) ferromagnets have emerged as a new platform for topological spin excitations. Here, via a comprehensive inelastic neutron scattering study and theoretical analysis of the spin-wave excitations, we report the realization of topological magnon insulators in CrXTe$_3$ (X=Si, Ge) compounds. The nontrivial nature and intrinsic tunability of the gap opening at the magnon band-crossing Dirac points are confirmed, while the emergence of the corresponding in-gap topological edge states is demonstrated theoretically. The realization of topological magnon insulators with intrinsic gap-tunability in this class of remarkable 2D materials will undoubtedly lead to new and fascinating technological applications in the domain of magnonics and topological spintronics.

cond-mat.str-el↗

arXiv2021

Complex magnetism of the two-dimensional antiferromagnetic Ge2F: from a Néel spin-texture to a potential antiferromagnetic skyrmion

Based on density functional theory combined with low-energy models, we explore the magnetic properties of a hybrid atomic-thick two-dimensional (2D) material made of Germanene doped with fluorine atoms in a half-fluorinated configuration (Ge2F). The Fluorine atoms are highly electronegative, which induce magnetism and break inversion symmetry, triggering thereby a finite and strong Dzyaloshinskii-Moriya interaction (DMI). The magnetic exchange interactions is of antiferromagnetic nature among the first, second and third neighbors, which leads to magnetic frustration. The Néel state is found to be the most stable state, with magnetic moments lying in the surface plane. This results from the out-of-plane component of the DMI vector, which seems to induce an effective in-plane magnetic anisotropy. Upon application of a magnetic field, spin-spirals and antiferromagnetic skyrmions can be stabilized. We conjecture that this can be realized via magnetic exchange fields induced by a magnetic substrate. To complete our characterization, we computed the spin-wave excitations and the resulting spectra, which could be probed via electron energy loss spectroscopy, magneto-Raman spectroscopy or scanning tunneling spectroscopy.

cond-mat.mtrl-sci↗

arXiv2020

The interplay of Dzyaloshinskii-Moriya and Kitaev interactions for magnonic properties of Heisenberg-Kitaev honeycomb ferromagnets

The properties of Kitaev materials are attracting ever increasing attention owing to their exotic properties. In realistic two-dimensional materials, Kitaev interaction is often accompanied by the Dzyloshinskii-Moriya interaction, which poses a challenge of distinguishing their magnitude separately. In this work, we demonstrate that it can be done by accessing magnonic transport properties. By studying honeycomb ferromagnets exhibiting Dzyaloshinskii-Moriya and Kitaev interactions simultaneously, we reveal non-trivial magnonic topological properties accompanied by intricate magnonic transport characteristics as given by thermal Hall and magnon Nernst effects. We also investigate the effect of a magnetic field, showing that it does not only break the symmetry of the system but also brings drastic modifications to magnonic topological transport properties, which serve as hallmarks of the relative strength of anisotropic exchange interactions. Based on our findings, we suggest strategies to estimate the importance of Kitaev interactions in real materials.

cond-mat.str-el↗

arXiv2020

Modelling spin waves in noncollinear antiferromagnets: spin-flop states, spin spirals, skyrmions and antiskyrmions

Spin waves in antiferromagnetic materials have great potential for next-generation magnonic technologies. However, their properties and their dependence on the type of ground-state antiferromagnetic structure are still open questions. Here, we investigate theoretically spin waves in one- and two-dimensional model systems with a focus on noncollinear antiferromagnetic textures such as spin spirals and skyrmions of opposite topological charges. We address in particular the nonreciprocal spin excitations recently measured in bulk antiferromagnet $α$--$\text{Cu}_2\text{V}_2\text{O}_7$ utilizing inelastic neutron scattering experiments [Phys.\ Rev.\ Lett.\ \textbf{119}, 047201 (2017)], where we help to characterize the nature of the detected spin-wave modes. Furthermore, we discuss how the Dzyaloshinskii-Moriya interaction can lift the degeneracy of the spin-wave modes in antiferromagnets, resembling the electronic Rashba splitting. We consider the spin-wave excitations in antiferromagnetic spin-spiral and skyrmion systems and discuss the features of their inelastic scattering spectra. We demonstrate that antiskyrmions can be obtained with an isotropic Dzyaloshinskii-Moriya interaction in certain antiferromagnets.

cond-mat.mes-hall↗

arXiv2020

Nonreciprocity of spin waves in noncollinear magnets due to the Dzyaloshinskii-Moriya interaction

Broken inversion symmetry in combination with the spin-orbit interaction generates a finite Dzyaloshinskii-Moriya interaction (DMI), which can induce noncollinear spin textures of chiral nature. The DMI is characterized by an interaction vector whose magnitude, direction and symmetries are crucial to determine the stability of various spin textures, such as skyrmions and spin spirals. The DMI can be measured from the nonreciprocity of spin waves in ferromagnets, which can be probed via inelastic scattering experiments. In a ferromagnet, the DMI can modify the spin-wave dispersion, moving its minimum away from the $Γ$ point. Spin waves propagating with opposite wavevectors are then characterized by different group velocities, energies and lifetimes, defining their nonreciprocity. Here, we address the case of complex spin textures, where the manifestation of DMI-induced chiral asymmetries remains to be explored. We discuss such nonreciprocal effects and propose ways of accessing the magnitude and direction of the DMI vectors in the context of spin-polarized or spin-resolved inelastic scattering experiments. We show that only when a periodic magnetic system has finite net magnetization, that is, when the vector sum of all magnetic moments is nonzero, can it present a total nonreciprocal spin-wave spectrum. However, even zero-net-magnetization systems, such as collinear antiferromagnets and cycloidal spin spirals, can have spin-wave modes that are individually nonreciprocal, while the total spectrum remains reciprocal.

cond-mat.mes-hall↗

arXiv2018

Spin-resolved inelastic electron scattering by spin waves in noncollinear magnets

Topological non-collinear magnetic phases of matter are at the heart of many proposals for future information nanotechnology, with novel device concepts based on ultra-thin films and nanowires. Their operation requires understanding and control of the underlying dynamics, including excitations such as spin-waves. So far, no experimental technique has attempted to probe large wave-vector spin-waves in non-collinear low-dimensional systems. In this work, we explain how inelastic electron scattering, being suitable for investigations of surfaces and thin films, can detect the collective spin-excitation spectra of non-collinear magnets. To reveal the particularities of spin-waves in such non-collinear samples, we propose the usage of spin-polarized electron-energy-loss spectroscopy augmented with a spin-analyzer. With the spin-analyzer detecting the polarization of the scattered electrons, four spin-dependent scattering channels are defined, which allow to filter and select specific spin-wave modes. We take as examples a topological non-trivial skyrmion lattice, a spin-spiral phase and the conventional ferromagnet. Then we demonstrate that, counter-intuitively and in contrast to the ferromagnetic case, even non spin-flip processes can generate spin-waves in non-collinear substrates. The measured dispersion and lifetime of the excitation modes permit to fingerprint the magnetic nature of the substrate.

cond-mat.mes-hall↗

arXiv2017

First-principles investigation of spin wave dispersions in surface-reconstructed Co thin films on W(110)

We computed spin wave dispersions of surface-reconstructed Co films on the W(110) surface in the adiabatic approximation. The magnetic exchange interactions are obtained via first-principles electronic structure calculations using the Korringa-Kohn-Rostoker Green function method. We analyze the strength and oscillatory behavior of the intralayer and interlayer magnetic interactions and investigate the resulting spin wave dispersions as a function of the thickness of Co films. In particular, we highlight and explain the strong impact of hybridization of the electronic states at the Co-W interface on the magnetic exchange interactions and on the spin wave dispersions. We compare our results to recent measurements based on electron energy loss spectroscopy [E. Michel, H. Ibach, and C.M. Schneider, Phys. Rev. B 92, 024407 (2015)]. Good overall agreement with experimental findings can be obtained by considering the possible overestimation of the spin splitting, stemming from the local spin density approximation, and adopting an appropriate correction.

cond-mat.mes-hall↗