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Dominik Legut

Publications and source records attributed to Dominik Legut.

At least 19 recordsLinked to original sources

Ultralow-Field Triplon Condensation in a Spin-Ladder Magnet

We realise the first ultralow-field Bose-Einstein condensation of triplons in a spin-ladder magnet, uncovering a quantum critical point at only $\mu_0 H_{c1}=0.17$ T in Henmilite ($\mathrm{Ca_2Cu(OH)_4[B(OH)_4]_2}$). Unlike dimer magnets, a ladder retains extended one-dimensional correlations in its gapped parent state, making this limit strongly fluctuation dominated. Thermodynamic, magnetoelastic, $\mu$SR, and neutron-diffraction measurements overturn the previous assignment of zero-field antiferromagnetic order, establishing a quantum-disordered coupled-ladder parent state with persistent low-energy dynamics. The weak low-temperature anomaly instead marks a gap-controlled crossover from the correlated ladder regime into the activated quantum-disordered state. These measurements further reveal an exceptionally asymmetric ordered dome extending to $\mu_0 H_{c2}\simeq 8.2$ T. Quantum Monte Carlo simulations for the relevant spin Hamiltonian place Henmilite just on the gapped side of the zero-field ladder-ordering instability, naturally accounting for the strong separation between the exchange and residual-gap scales and the tiny critical field. Our findings extend ultralow-field triplon condensation beyond the dimer paradigm and establish Henmilite as a platform for controlled tuning across quantum criticality in a fluctuation-dominated spin ladder.

cond-mat.str-el

Room-temperature magnon-phonon transduction in high-damping Co/Pt structures

Quantum communication and information processing strongly benefit from the coupling between different quasi-particles, offering complementary advantages. Magnetoelastic materials inherently allow for direct coupling between magnetization dynamics and quantized lattice vibrations, called phonons. Near the ferromagnetic resonances, phonons may thus trade energy and angular momentum with uniformly precessing magnetization, called magnons, and enable transduction of information from magnetic to phononic modes, thereby paving the way for long-range transport of magnetic information without the need of magnetic material. Here, we employ tailored magnetic-nonmagnetic heterostructures, which simultaneously act as cavities for standing shear waves, to bring selective phonons and magnons into resonance. These Co films with Pt seed layers show extended linewidth and reduced amplitude of the phonon-resonant FMR lines, providing a hallmark of energy and angular momentum exchange. Complementarily, by theoretical modeling and ultra-fast coherent phonon spectroscopy, we identify the responsible transverse acoustic phonons as standing shear waves in the combined Co and Pt structure. We find a high crystal quality in conjunction with a large magnetoelastic coupling constant as a prerequisite for efficient magnon-phonon coupling of this type. Such resonant enhancement of magnon-phonon coupling in CMOS-compatible material provides an ideal material platform for future quantum transducers.

cond-mat.mtrl-sci

Spin-lattice model simulations of tetragonal FePt system

Magnetic materials play a key role in the contemporary industry, providing unique features with a wide application potential. To study physical phenomena and design new materials, it is important to possess an appropriate tool, a model allowing simulation of desired behavior. Spin-lattice model simulations can be used to investigate spacious systems containing thousands of atoms, while complex phenomena arising from the interplay of lattice and spin dynamics can be modeled. One of the important phenomena that can be modeled in the spin lattice simulation is magnetoelastic behavior, offering direct conversion between the mechanical and magnetic energy. However, so far, only models for systems with cubic symmetry have been introduced. Therefore, here, a spin-lattice model for a system with tetragonal symmetry is proposed, where its strength is manifested by simulation of magnetoelastic properties of a characteristic representative L1$_{0}$ FePt system.

cond-mat.mtrl-sci

Higher order magnetoelasticity energy corrections in bcc and fcc systems

Magnetoelastic properties play a vital role in industrial applications. Despite being hidden behind either purely magnetic or elastic behavior, magnetoelasticity takes place in a wide range of devices as transducers, acoustic actuators, or fast response sensors. In this work, we inspect the impact of higher-order terms on the anisotropic magnetostriction behavior. Regarding ab-initio calculations, the anisotropic magnetostriction can be related to the strain dependence of the magnetocrystaline energy. Commonly, the description is restricted to a linear strain dependence in the magnetoelastic energy. Here, we derive higher-order terms in strain for bcc and fcc crystal structures. Using a simple parametrization, we show that the influence of the higher-order strain terms is negligible for the studied cubic systems.

cond-mat.mtrl-sci

Development of a magnetic interatomic potential for cubic anti-ferromagnets: the case of NiO

Interatomic potentials are essential for molecular dynamics simulations of magnetic materials, yet incorporating magnetic features into potentials for complex antiferromagnets remains challenging. Nickel oxide (NiO), a prototypical cubic antiferromagnet, exemplifies this difficulty. Here we develop a methodology to integrate magnetic properties into interatomic potentials for cubic antiferromagnets by adding a magnetic Hamiltonian which includes both the Heisenberg exchange and N\'eel model. We apply this approach to NiO by constructing two potentials: one based on the Born model of ionic solids and another using a reference-free modified embedded atom method. Both potentials include magnetoelastic interactions and are validated against Density Functional Theory calculations, showing excellent agreement in mechanical and magnetic properties at zero temperature. These models enable large-scale simulations of magnetoelastic phenomena in antiferromagnets and open avenues for molecular dynamics studies involving coupled electric and magnetic fields in metal oxides.

cond-mat.mtrl-sci

Thermoelectric power factors of defective scandium nitride nanostructures from first principles

The thermoelectric properties of scandium nitride are strongly influenced by structural and electronic factors arising from defects and impurities. Nevertheless, the mechanisms by which these microscopic features affect transport are not yet fully understood. Experiments show a large variability in the electronic transport properties, with a strong dependence on the experimental conditions, and attempts to improve thermoelectric efficiency often lead to conflicting effects. In this work, we employ the Landauer approach to analyze the effects of different kinds of structural defects and impurities on electronic transport in scandium nitride. This approach allows us to relate the transport mechanisms to the structural and electronic modifications introduced in the lattice, with atomistic resolution. In light of these new insights, we propose a rationale relating part of the experimental variability to its microscopic origin.

cond-mat.mtrl-sci

Ambient and high pressure studies of structural, electronic and magnetic properties of EuZn$_2$P$_2$ single crystal

A thorough study of EuZn$_2$P$_2$ single crystals, which were grown from Sn flux, was performed using both bulk (heat capacity, ac susceptibility, dc magnetization, electrical resistivitivity, magnetoresistance) and microscopic (M\"ossbauer spectroscopy) techniques. Electrical resistance and magnetic susceptibility were measured also under high pressure conditions (up to 19 GPa and 9.5 GPa, respectively). Further insight into electronic properties and phonons is provided by ab initio calculations. The results indicate that EuZn$_2$P$_2$ is an antiferromagnet with strong Eu-Eu exchange coupling of ferromagnetic type within the basal plane and weaker antiferromagnetic interaction along the c axis. The Eu magnetic moments are tilted from the basal plane. Hydrostatic pressure strongly affects both magnetic (increase of the N\'eel temperature) and electronic (suppression of the band gap and semi metallic behavior) properties, indicating a strong interplay of structure with magnetic and electronic degrees of freedom.

cond-mat.mtrl-sci

Ab initio investigation of electronic and lattice properties of Fe$_4$(P$_2$O$_7$)$_3$

In this research, we examine the electronic, magnetic, and lattice properties of the Fe$_4$(P$_2$O$_7$)$_3$ compound using the first principles calculations based on the density functional theory. The crystal lattice has a monoclinic structure, belonging to the P$2_1/n$ space group. The optimized lattice parameters are a=7.406 \AA, b=21.425 \AA, c=9.529 \AA, and agree very well with the experimental data, thanks to the local Coulomb interactions and van der Waals forces included in the calculations. The investigation considers several magnetic orderings. The lowest total energy was found for the antiferromagnetic configuration with the magnetic moment of $\sim4.6~\mu_{\text{B}}$ per Fe atom. The electronic structure calculation shows the Mott insulating state with the energy gap $E_g=2.87$~eV. For the relaxed crystal structure, the elastic properties were obtained and analyzed. The phonon dispersion relations and density of states were calculated within the temperature-dependent effective potential methodusing atomic multidisplacements obtained by high efficiency configuration space sampling.

cond-mat.mtrl-sci

Magneto-Raman effect in van der Waals layered two-dimensional CrSBr antiferromagnet

Magneto-Raman spectroscopy is applied to study spin-phonon coupling in the layered two-dimensional (2D) van der Waals antiferromagnet CrSBr. We report on the effects of temperature and external magnetic field on Raman-active phonons of $A_g$ symmetry in bulk and one-to-six-layer forms of CrSBr that are reflected by the Raman spectral patterns measured at different configurations of circularly polarized laser beam. The results of experimental investigations reveal that spin-spin and spin-phonon interactions play a significant role below the N\'{e}el temperature and are notably stronger in CrSBr monolayer than in bulk material. Spin-phonon coupling leads to the emergence of \textit{ new} phonon peaks at very low temperatures. Such effect is solely observed in one-to-six-layer CrSBr and is absent in its bulk form. Our experimental research is accompanied by \textit{ab initio} simulations of the Raman spectra of bulk and monolayer CrSBr that uncover correlations between intensities of Raman-active phonons and the arrangement of spin magnetic moments on Cr atoms. Comparative analysis of simulated and experimental Raman spectra suggests the most favored spin orientation in the CrSBr antiferromagnetic system.

cond-mat.mtrl-sci

Magnetoelasticity - magnetic structure interrelation - tetragonal MnPt system study

Magnetic materials represent an essential ingredient for the contemporary industry. Apart from common material parameters such as magnetocrystalline anisotropy, coercivity, or saturation magnetization, magnetoelastic behavior is vital for applications serving in various devices, e.g., in acoustic actuators, transducers, or sensors providing a desirable fast response and high efficiency with respect to applied magnetic field. Magnetoelastic properties have been studied for ferromagnetic 3d elements, or especially in high symmetry systems containing rare-earth elements to achieve higher values. Since, unlike for rare earth Laves phases, in the transition metals or alloys, these effects are very weak. Here, in contrast, we analyze the magnetoelastic behavior of antiferromagnetic tetragonal system MnPt, explaining the experimentally measured data based on the theoretical calculations and discussing the influence of the magnetic structure. Particularly, we inspect the origin of magnetocrystalline anisotropy energy, as well as the size and source of the isotropic and anisotropic parts of magnetoelastic (magnetostriction) coefficients.

cond-mat.mtrl-sci

Effect of interface on magnetic exchange coupling in Co/Ru/Co trilayer: from ab-initio simulations to micromagnetics

Interfaces play a substantial role for the functional properties of structured magnetic materials and magnetic multilayers. Modeling the functional behavior of magnetic materials requires the treatment of the relevant phenomena at the device level. Properties predicted from the electronic structure and spin dynamics at the atomistic level have to be properly transferred into a continuum level treatment. In this work we show how Co/Ru/Co three layers can be simulated with the continuum theory of micromagnetism, with interface coupling energies and bulk intrinsic properties properly derived from the results of \emph{ab initio} and spin dynamics simulations at different temperatures.

cond-mat.mtrl-sci

OstravaJ: a tool for calculating magnetic exchange interactions via DFT

OstravaJ is a Python package for high-throughput calculation of exchange interaction terms in the Heisenberg model for magnetic materials. It uses the total energy difference method, where calculations are based on the total energy of the system in different magnetic configurations, calculated by means of density functional theory. OstravaJ can propose a suitable set of magnetic configurations, generate VASP configuration files in cooperation with the user, and read VASP calculation results, which minimizes necessary human interaction. It can also calculate other relevant properties (e. g. MFA and RPA critical temperature, spin-wave stiffness) and provide input for various atomistic spin dynamics codes. We present results for a number of materials from various classes (metals, transition metal oxides), compared to other methods. They show that the total energy difference method is a useful method for exchange interaction calculation from first principles.

cond-mat.mtrl-sci

Modeling and theoretical design of next-generation lithium metal batteries

Rechargeable lithium metal batteries (LMBs) with an ultrahigh theoretical energy density have attracted more and more attentions for their crucial applications of portable electronic devices, electric vehicles, and smart grids. However, the implementation of LMBs in practice is still facing numerous challenges, such as low Coulombic e ciency, poor cycling performance, and complicated interfacial reactions. First-principles calculations have become a powerful technique in lithium battery research eld, in terms of modeling the structures and properties of speci c electrode materials, understanding the charge/discharge mechanisms at the atomic scale, and delivering rational design strategies for electrode materials as well as electrolytes. In this review, theoretical studies on sulfur cathodes, oxygen cathodes, lithium metal anodes, and solid-state electrolytes (SSEs) of LMBs are summarized. A brief introduction of simulation methods is o ered at rst. The next two chapters mainly focus on issues concerning cathodes of LMBs. Then the theoretical researches on the Li metal anode and SSEs are particularly reviewed. The current challenges and potential research directions in each field of LMBs are prospected from a theoretical viewpoint.

cond-mat.mtrl-sci

Hydrostatic pressure control of the spin-orbit proximity effect, spin relaxation, and thermoelectricity in a phosphorene-WSe$_2$ heterostructure

Effective control of interlayer interactions is a key element in modifying the properties of van der Waals heterostructures and the next step toward their practical applications. Focusing on the phosphorene-WSe$_2$ heterostructure, we demonstrate, using first-principles calculations, proximity-induced amplification of the spin-orbit coupling in phosphorene by applying vertical pressure. We simulate external pressure by changing the interlayer distance between bilayer constituents and show that it is possible to tune the spin-orbit field of phosphorene holes in a controllable way. By fitting effective electronic states of the proposed Hamiltonian to the first principles data, we reveal that the spin-orbit coupling in phosphorene hole bands is enhanced more than two times for experimentally accessible pressures up to 17 kbar. Correspondingly, we find that the pressure-enhanced spin-orbit coupling boosts the Dyakonov-Perel spin relaxation mechanism, reducing the spin lifetime of phosphorene holes by factor 4. We further explore the role of the lateral shift on the spin-orbit field and reveal that the spin-orbit strength of phosphorene holes can be sizably modulated when strong pressure is applied. We also found that the thermopower is governed mainly by the phosphorene and pressure reduces the overall thermoelectric efficiency of the heterostructure.

cond-mat.mes-hall

Anharmonicity and structural phase transition in the Mott insulator Cu$_2$P$_2$O$_7$

Ab initio investigations of structural, electronic, and dynamical properties of the high-temperature $\beta$ phase of copper pyrophosphate were performed using density functional theory. The electronic band structure shows the Mott insulating state due to electron correlations in copper ions. By calculating phonon dispersion relations, the soft mode at the A point of the Brillouin zone was revealed, showing the dynamical instability of the $\beta$ phase at low temperatures. The double-well potential connected with the soft mode is derived and the mechanism of the structural phase transition to the $\alpha$ phase is discussed. The self-consistent phonon calculations based on the temperature-dependent effective potential show the stabilization of the $\beta$ phase at high temperatures, due to the anharmonic effects. The pronounced temperature dependence and the large line width of the soft mode indicate an essential role of anharmonicity in the structural phase transition.

cond-mat.mtrl-sci

Control of the phonon band gap with isotopes in hexagonal boron nitride

The isotopic mass of constituent elements of materials has a well-known effect on the energy of vibrational modes. By means of monochromated scanning transmission electron microscopy we have experimentally studied the phonon bandstructure of hexagonal BN, where a phonon band gap appears between in-plane optical phonon modes and the lower energy part of the phonon spectrum. The size of the phonon band gap can be manipulated by the isotopic mass of the boron. While in $^{11}$BN the phonon band gap is about 7 meV wide, in $^{10}$BN the gap nearly closes, being an order of magnitude smaller (below 0.5 meV). This opens exciting options for manipulating terahertz wave propagation through isotopically structured devices having otherwise no interfaces between chemically distinct components.

cond-mat.mtrl-sci

On the miscibility gap in tungsten-based alloys

In this work we establish an approach to model miscibility gaps of alloys using statistical physics, lattice dynamics from first-principles calculations. We carefully calculate the entropy to include all processes introducing disorder to the system, i.e., combining the electronic, phononic, and configuration entropies. Furthermore we present our algorithm for generating Special Quasirandom Structures (SQS). We model the miscibility gap in tungsten - chromium and tungsten - molybdenum systems, obtaining the agreement with the experimental data. Furthermore, we propose an enhancement for the tungsten-chromium W$_{70}$Cr$_{30}$ alloy with tantalum and hafnium, leading to the modified stabilization temperatures $T_S$, where the solid solution is miscible.

cond-mat.mtrl-sci

Inhibition of steel corrosion with imidazolium-based compounds -- experimental and theoretical study

This work aims to investigate the corrosion inhibition of the mild steel in the 1 M HCl solution by 1-octyl-3-methylimidazolium hydrogen sulphate 1-butyl-3-methylimidazolium hydrogen sulphate, and 1-octyl-3-methylimidazolium chloride, using electrochemical, weight loss, and surface analysis methods as well as the full quantum-mechanical treatment. Polarization measurements prove that studied compounds are mixed-type inhibitors with a predominantly anodic reaction. The inhibition efficiency obtained from the polarization curves is about 80-92% for all of the 1-octyl-3-methylimidazolium salts with a concentration higher than 0.005 mol/l, while it is much lower for 1-butyl-3-methylimidazolium hydrogen sulphate. The values measured in the weight loss experiments (after seven days) are to some extent higher (reaching up to 98% efficiency). Furthermore, we have shown that the influence of the alkyl chain length on the inhibition efficiency is much larger than that of the anion type. Furthermore, we obtain a realistic model of a single molecule on iron surface Fe(110) by applying the Density Functional Theory calculations. We use the state-of-the-art computational approach, including the meta-GGA strongly-constrained and appropriately normed semilocal density functional to model the electronic structure properties of both free and bounded-to-surface molecules of 1-butyl-, 1-hexyl-, and 1-octyl-3-methylimizadolium bromide, chloride, and hydrogen sulphate. From the calculations we extract, the HOMO/LUMO gap, hardness, electronegativity, and charge transfer of electrons from/to molecules-in-question. It supports the experimental findings and explains the influence of the alkyl chain length and the functional group on the inhibition process.

physics.chem-ph