arXiv subjects

D. Legut

Publications and source records attributed to D. Legut.

At least 19 recordsLinked to original sources

arXiv2026

Complex Magnetic Behavior of the Ce sawtooth chains in CeRhSn$_2$

Conflicting reports exist on the ground state of the intermetallic compound CeRhSn$_2$. This can be rooted in the sawtooth-like arrangement of two inequivalent Ce sites in the unit cell, which suggests potential geometric magnetic frustration. To resolve, we conducted a comprehensive study on high-quality single crystals of CeRhSn$_2$ by means of magnetization ($M$), specific heat ($C_p/T$), and resistivity ($\rho$). The system exhibits strong magnetic anisotropy, confirming the $b$-axis as the easy magnetic axis. We establish three successive transitions, an AFM order at $T_{N} = 3.65$K, a first-order FM order at $T_{C} = 1.7$K and final transition, at $T = 1.5$K. The transition temperatures are highly field-directional dependent: in a magnetic field, the lowest transition is immediately suppressed while $\mathbf{H} \parallel b$ rapidly merges $T_{C}$ and $T_{N}$ into a single second-order transition. Conversely, $\mathbf{H}\parallel c$ suppresses the FM order and reduces $T_{N}$. Additional ab initio calculations affirm the FM ground state of CeRhSn$_2$. The observation of an enhancement of the Sommerfeld coefficient ($\gamma = 76.5$mJ/mol$\cdot$K$^2$) may arise from geometric frustration, but it is most consistently attributed to weak Kondo hybridization as frustration cannot be conclusively established through our data.

cond-mat.str-el↗

arXiv2025

Stability of graphene hyperbolic pseudospheres under harsh conditions

We demonstrate the high stability of simulated graphene hyperbolic pseudospheres under large externally imposed deformations and high temperature annealing. Hyperbolic pseudospheres are produced in a two-step Molecular Dynamics simulation process. First, carbon atoms are forced down a thin three-dimensional volume of a chosen shape. During this extrusion process the carbon atoms form a precursor to graphene that is unrealistically less stable than graphite or diamond. Then the unstable carbon structure is annealed inside the thin volume at high temperature, turning the carbon into realistic polycrystalline, curved graphene. Point defects naturally appear in numbers and places that stabilize the graphene in the desired shape, without high residual stresses. We applied this new methodology to the creation of graphene hyperbolic pseudosphere surfaces, which reproduce analogs to some aspects of classical or quantum gravity. The free edges of the pseudosphere cause bending of the graphene. When these free edges are removed from the simulations by attaching periodic flat graphene sheets to the pseudosphere edges, the carbon atoms assume positions just some tenths of \r{A} from the mathematical hyperbolic pseudosphere surface. In demanding tests of their stability, the hyperbolic pseudospheres proved stable against $20^\circ$ shearing or $20\%$ elongation and then being released, which eventually raised their temperatures by $\sim 300 \ \text{K}$. Our methodology is relatively easy to use and offers a practical way to create simulated curved graphene surfaces of almost any shape. It allows for thorough testing in advance of the stability of graphene shapes that are to be produced experimentally.

cond-mat.mes-hall↗

arXiv2025

Intermediate-valence behavior in U2Rh2Sb

Intermediate-valence behavior is sometimes observed in lanthanide-based materials containing Ce, Yb, Sm or Eu. However, the number of actinide-based systems that exhibit this type of behavior is rather limited. In this work, we present the discovery and characterization of a uranium compound U2Rh2Sb, which turns out to be a candidate for the intermediate-valencebehavior. The material shows a characteristic feature in the magnetic susceptibility around T = 50 K, which can be described within the interconfiguration-fluctuation model of intermediate valence systems. We find the energy difference between the 5f3(U3+) and 5f2(U4+) states to be $\delta$Eex/kB $\approx$ 400 K and the corresponding valence fluctuation temperature to be Tvf $\approx$ 140 K. The value of the electronic specific heat coefficient $\gamma$ = 50 mJ mol-1 U K-2 signals a modest electron effective mass enhancement. The electrical resistivity indicates metallic behavior, albeit with a small residual resistivity ratio. Measurements of thermoelectric properties indicate a change of sign in the Seebeck coefficient around T = 100 K, with a minimum achieved at T = 50 K, which coincides with the broad peak observed in magnetic susceptibility. The experimental results are compared with the theoretical analysis, based on the first-principles calculations, including lattice dynamics.

cond-mat.str-el↗

arXiv2024

VelCrys: Interactive web-based application to compute acoustic wave velocity in crystals and its magnetic corrections

We present VelCrys, a web-based interactive tool, that allows to perform further post-processing of the elastic tensor in order to compute and plot the group velocity of the acoustic waves for any crystal symmetry. We also implemented the calculation of effective magnetic corrections to the elastic tensor and corresponding fractional change in group velocity under a magnetic field. We apply it to dry sandstone, cubic CoPt and hcp Co to show some of the program features. In the analysis of magnetic corrections, we find complex landscapes of fractional change in group velocity as a function of ray direction, as well as a field dependence consistent with Simon effect.

cond-mat.mtrl-sci↗

arXiv2024

Long-range magnetic order in CePdAl$_3$ enabled by orthorhombic deformation

We investigate the effect of structural deformation on the magnetic properties of orthorhombic CePdAl$_3$ in relation to its tetragonal polymorph. Utilizing x-ray and neutron diffraction we establish that the crystal structure has the $Cmcm$ space group symmetry and exhibits pseudo-tetragonal twinning. According to density-functional calculations the tetragonal-orthorhombic deformation mechanism has its grounds in relatively small free enthalpy difference between the polymorphs, allowing either phase to be quenched and fully accounts for the twinned microstructure of the orthorhombic phase. Neutron diffraction measurements show that orthorhombic CePdAl$_3$ establishes long-range magnetic order below $T_\mathrm{N}$=5.29 (5) K characterized by a collinear, antiferromagnetic arrangement of magnetic moments. Magnetic anisotropies of orthorhombic CePdAl$_3$ arise from strong spin-orbit coupling as evidenced by the crystal-field splitting of the $4f$ multiplet, fully characterised with neutron spectroscopy. We discuss the potential mechanism of frustration posed by antiferromagnetic interactions between nearest neighbours in the tetragonal phase, which hinders the formation of long-range magnetic order in tetragonal CePdAl$_3$. We propose that orthorhombic deformation releases the frustration and allows for long-range magnetic order.

cond-mat.str-el↗

arXiv2022

Automated calculations of exchange magnetostriction

We present a methodology based on deformations of the unit cell that allows to compute the isotropic magnetoelastic constants, isotropic magnetostrictive coefficients and spontaneous volume magnetostriction associated to the exchange magnetostriction. This method is implemented in the python package MAELAS (v3.0), so that it can be used to obtain these quantities by first-principles calculations and classical spin-lattice models in an automated way. We show that the required reference state to obtain the spontaneous volume magnetostriction combines the equilibrium volume of the paramagnetic state and magnetic order of the ground state. We identify an error in the theoretical expression of the isotropic magnetostrictive coefficient $\lambda^{\alpha 1,0}$ for uniaxial crystals given in previous publications, which is corrected in this work. The presented computational tool may be helpful to provide a better understanding and characterization of the relationship between the exchange interaction and magnetoelasticity.

cond-mat.mtrl-sci↗

arXiv2022

First-principles calculations of the spontaneous volume magnetostriction based on the magnetoelastic energy

We present a simple methodology to compute the spontaneous volume magnetostriction with first-principles calculations on the basis of the magnetoelastic energy. This method makes use of deformations of the unit cell only at the ferromagnetic state. Hence, it does not require the difficult first-principles calculation of the equilibrium volume at the paramagnetic state. To validate this methodology, we apply it to body-centered cubic Fe and face-centered cubic Ni single crystals, finding consistent results with experiment and previous first-principles calculations. The simplicity and reliability of this approach could be exploited in the high-throughput screening of spontaneous volume magnetostriction, as well as associated quantities like isotropic magnetoelastic constants and isotropic magnetostrictive coefficients.

cond-mat.mtrl-sci↗

arXiv2022

Atomistic simulations of magnetoelastic effects on sound velocity

In this work, we leverage atomistic spin-lattice simulations to examine how magnetic interactions impact the propagation of sound waves through a ferromagnetic material. To achieve this, we characterize the sound wave velocity in BCC iron, a prototypical ferromagnetic material, using three different approaches that are based on the oscillations of kinetic energy, finite-displacement derived forces, and corrections to the elastic constants, respectively. Successfully applying these methods within the spin-lattice framework, we find good agreement with the Simon effect including high order terms. In analogy to experiments, morphic coefficients associated with the transverse and longitudinal waves propagating along the [001] direction are extracted from fits to the fractional change in velocity data. The present efforts represent an advancement in magnetoelastic modelling capabilities which can expedite the design of future magneto-acoustic devices.

cond-mat.mtrl-sci↗

arXiv2021

Optical control of 4f orbital state in rare-earth metals

A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth (RE) elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved X-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4f-electronic excitations out of the ground state multiplet occur after optical pumping. These excitations are driven by inelastic 5d-4f-electron scattering, alter the 4f-orbital state and consequently the MCA with important implications for magnetization dynamics in 4f-metals, and more general for the excitation of localized electronic states in correlated materials.

cond-mat.mtrl-sci↗

arXiv2021

MAELAS 2.0: A new version of a computer program for the calculation of magneto-elastic properties

MAELAS is a computer program for the calculation of magnetocrystalline anisotropy energy, anisotropic magnetostrictive coefficients and magnetoelastic constants in an automated way. The method originally implemented in version 1.0 of MAELAS was based on the length optimization of the unit cell, proposed by Wu and Freeman, to calculate the anisotropic magnetostrictive coefficients. We present here a revised and updated version (v2.0) of MAELAS, where we added a new methodology to compute anisotropic magnetoelastic constants from a linear fitting of the energy versus applied strain. We analyze and compare the accuracy of both methods showing that the new approach is more reliable and robust than the one implemented in version 1.0, especially for non-cubic crystal symmetries. This analysis also help us to find that the accuracy of the method implemented in version 1.0 could be improved by using deformation gradients derived from the equilibrium magnetoelastic strain tensor, as well as potential future alternative methods like the strain optimization method. Additionally, we clarify the role of the demagnetized state in the fractional change in length, and derive the expression for saturation magnetostriction for polycrystals with trigonal, tetragonal and orthorhombic crystal symmetry. In this new version, we also fix some issues related to trigonal crystal symmetry found in version 1.0.

cond-mat.mtrl-sci↗

arXiv2021

Influence of grain morphology and orientation on saturation magnetostriction of polycrystalline Terfenol-D

In this work we computationally study the effect of microstructure on saturation magnetostriction of Terfenol-D (Tb$_{0.27}$Dy$_{0.73}$Fe$_{2}$) by means of Finite Element Method. The model is based on the equilibrium magnetoelastic strain tensor at magnetic saturation, and shows that the crystal orientation might play a more significant role on saturation magnetostriction than the morphology of the grains. We also calculate the dependence of saturation magnetostriction on the dispersion angle of the distribution of grains in the oriented growth crystal directions $<011>$ and $<111>$, finding that not highly oriented grain distributions reduce saturation magnetostriction significantly. This result evinces the importance of high-quality control of grain orientation in the synthesis of grain-aligned polycrystalline Terfenol-D, and provides a quantitative estimation for the range of acceptable values for the dispersion angle of the distribution of the oriented grains.

cond-mat.mtrl-sci↗

arXiv2021

Photoemission signature of momentum-dependent hybridization in CeCoIn$_5$

Hybridization between $f$ electrons and conduction bands ($c$-$f$ hybridization) is a driving force for many unusual phenomena. To provide insight into it, systematic studies of CeCoIn$_5$ heavy fermion superconductor have been performed by angle-resolved photoemission spectroscopy (ARPES) in a large angular range at temperature of $T=6$ K. The used photon energy of 122 eV corresponds to Ce $4d$-$4f$ resonance. Calculations carried out with relativistic multiple scattering Korringa-Kohn-Rostoker method and one-step model of photoemission yielded realistic simulation of the ARPES spectra indicating that Ce-In surface termination prevails. Surface states, which have been identified in the calculations, contribute significantly to the spectra. Effects of the hybridization strongly depend on wave vector. They include a dispersion of heavy electrons and bands gaining $f$-electron character when approaching Fermi energy. We have also observed a considerable variation of $f$-electron spectral weight at $E_F$, which is normally determined by both matrix element effects and wave vector dependent $c$-$f$ hybridization. Fermi surface scans covering a few Brillouin zones revealed large matrix element effects. A symmetrization of experimental Fermi surface, which reduces matrix element contribution, yielded a specific variation of $4f$-electron enhanced spectral intensity at $E_F$ around $\bar{\Gamma}$ and $\bar{M}$ points. Tight-binding approximation calculations for Ce-In plane provided the same universal distribution of $4f$-electron density for a range of values of the parameters used in the model.

cond-mat.str-el↗

arXiv2020

Spin-lattice model for cubic crystals

We present a methodology based on the N\'{e}el model to build a classical spin-lattice Hamiltonian for cubic crystals capable of describing magnetic properties induced by the spin-orbit coupling like magnetocrystalline anisotropy and anisotropic magnetostriction, as well as exchange magnetostriction. Taking advantage of the analytical solutions of the N\'{e}el model, we derive theoretical expressions for the parameterization of the exchange integrals and N\'{e}el dipole and quadrupole terms that link them to the magnetic properties of the material. This approach allows to build accurate spin-lattice models with the desire magnetoelastic properties. We also explore a possible way to model the volume dependence of magnetic moment based on the Landau energy. This new feature can allow to consider the effects of hydrostatic pressure on the saturation magnetization. We apply this method to develop a spin-lattice model for BCC Fe and FCC Ni, and we show that it accurately reproduces the experimental elastic tensor, magnetocrystalline anisotropy under pressure, anisotropic magnetostrictive coefficients, volume magnetostriction and saturation magnetization under pressure at zero-temperature. This work could constitute a step towards large-scale modeling of magnetoelastic phenomena.

cond-mat.mtrl-sci↗

arXiv2020

Trimeron-phonon coupling in magnetite

Using density functional theory, we study the lattice dynamical properties of magnetite (Fe$_3$O$_4$) in the high-temperature cubic and low-temperature monoclinic phases. The calculated phonon dispersion curves and phonon density of states are compared with the available experimental data obtained by inelastic neutron, inelastic x-ray, and nuclear inelastic scattering. We find a very good agreement between the theoretical and experimental results for the monoclinic $Cc$ structure revealing the strong coupling between charge-orbital (trimeron) order and specific phonon modes. For the cubic phase, clear discrepancies arise which, remarkably, can be understood assuming that the strong trimeron-phonon coupling can be extended above the Verwey transition, with lattice dynamics influenced by the short-range trimeron order instead of the average cubic structure. Our results establish the validity of trimerons (and trimeron-phonon coupling) in explaining the physics of magnetite much beyond their original formulation.

cond-mat.str-el↗

arXiv2020

MAELAS: MAgneto-ELAStic properties calculation via computational high-throughput approach

In this work, we present the program MAELAS to calculate magnetocrystalline anisotropy energy, anisotropic magnetostrictive coefficients and magnetoelastic constants in an automated way by Density Functional Theory calculations. The program is based on the length optimization of the unit cell proposed by Wu and Freeman to calculate the magnetostrictive coefficients for cubic crystals. In addition to cubic crystals, this method is also implemented and generalized for other types of crystals that may be of interest in the study of magnetostrictive materials. As a benchmark, some tests are shown for well-known magnetic materials.

cond-mat.mtrl-sci↗

arXiv2020

M\"ossbauer studies of spin- and charge-modulations in BaFe2(As1-xPx)2

The BaFe2(As1-xPx)2 compounds with x = 0 (parent), x = 0.10 (under-doped), x = 0.31, 0.33, 0.53 (superconductors with Tc = 27.3 K, 27.6 K, 13.9 K, respectively) and x = 0.70, 0.77 (over-doped) have been investigated versus temperature using 57Fe M\"ossbauer spectroscopy. Special attention was paid to regions of the spin-density-wave (SDW) antiferromagnetic order, spin-nematic phase, and superconducting transition. The BaFe2(As0.90P0.10)2 compound exhibits a reduced amplitude of SDW as compared to the parent compound and preserved universality class of two-dimensional magnetic planes with one-dimensional spins. The spin-nematic phase region for x = 0.10 is characterized by an incoherent magnetic order. BaFe2(As0.69P0.31)2 shows coexistence of a weak magnetic order and superconductivity due to the vicinity of the quantum critical point. The charge density modulations in the BaFe2(As0.67P0.33)2 and BaFe2(As0.47P0.53)2 superconductors are perturbed near Tc. Pronounced hump of the average quadrupole splitting across superconducting transition is observed for the system with x = 0.33. The phosphorus substitution increases the Debye temperature of the BaFe2(As1-xPx)2 compound. Moreover, experimental electron charge densities at Fe nuclei in this material conclusively show that it should be recognized as a hole-doped system. The measured M\"ossbauer spectral shift and spectral area are not affected by transition to the superconducting state. This indicates that neither the average electron density at Fe nuclei nor the dynamical properties of the Fe-sublattice in BaFe2(As1-xPx)2 are sensitive to the superconducting transition. Theoretical calculations of hyperfine parameters determining the patterns of M\"ossbauer spectra of BaFe2(As1-xPx)2 with x = 0, 0.31, 0.5, and 1.0 are performed within the framework of the density functional theory.

cond-mat.supr-con↗

arXiv2018

PNADIS: An automated Peierls-Nabarro Analyzer for DISlocation core structure and slip resistance

Dislocation is one of the most critical and fundamental crystal defects that dominate the mechanical behavior of crystalline solids, however, a quantitative determination of its character and property in experiments is quite challenging and limited so far. In this paper, a fully automated Peierls-Nabarro (P-N) analyzer named PNADIS is presented; a complete set of the character and property of dislocation can be automatically derived, including the dislocation core structure, Peierls energy and stress, pressure field around dislocation core, solute/dislocation interaction energy, as well as the energy barrier and yield stress at 0K for solid solution strengthening. Furthermore, both one-dimensional (1D) and two-dimensional (2D) P-N models are implemented to meet the demand to analyze the character and property of dislocation for not only simple FCC and HCP structures but also complex crystals. The implementation of this code has been critically validated by a lot of evaluations and tests including 1D P-N model for complex crystals, 2D P-N model for FCC and HCP metals, pressure field around dislocation core, and solid solution strengthening for alloys. We expect that the automated feature of this code would provide a high-efficiency solution for determining the character and property of dislocation.

cond-mat.mtrl-sci↗

arXiv2014

Lattice dynamics of the heavy fermion compound URu$_2$Si$_2$

We report a comprehensive investigation of the lattice dynamics of URu$_2$Si$_2$ as a function of temperature using Raman scattering, optical conductivity and inelastic neutron scattering measurements as well as theoretical {\it ab initio} calculations. The main effects on the optical phonon modes are related to Kondo physics. The B$_{1g}$ ($\Gamma_3$ symmetry) phonon mode slightly softens below $\sim$100~K, in connection with the previously reported softening of the elastic constant, $C_{11}-C_{12}$, of the same symmetry, both observations suggesting a B$_{1g}$ symmetry-breaking instability in the Kondo regime. Through optical conductivity, we detect clear signatures of strong electron-phonon coupling, with temperature dependent spectral weight and Fano line shape of some phonon modes. Surprisingly, the line shapes of two phonon modes, E$_u$(1) and A$_{2u}$(2), show opposite temperature dependencies. The A$_{2u}$(2) mode loses its Fano shape below 150 K, whereas the E$_u$(1) mode acquires it below 100~K, in the Kondo cross-over regime. This may point out to momentum-dependent Kondo physics. By inelastic neutron scattering measurements, we have drawn the full dispersion of the phonon modes between 300~K and 2~K. No remarkable temperature dependence has been obtained including through the hidden order transition. {\it Ab initio} calculations with the spin-orbit coupling are in good agreement with the data except for a few low energy branches with propagation in the (a,b) plane.

cond-mat.str-el↗