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N. N. Kovaleva

Publications and source records attributed to N. N. Kovaleva.

At least 19 recordsLinked to original sources
arXiv2025

Electronic localization on the structural inhomogeneities formed due to Bi and Te deficiency in the MBE grown films of AFM topological insulator MnBi2Te4: Evidence from spectroscopic ellipsometry and infrared studies

The intrinsic substitutional and antisite defects cause unintentional doping and shift of the E_F position above the conduction band minimum in the AFM topological insulator (TI) MnBi2Te4. This prevents measurements of the quantum anomalous Hall effect (QAH) and investigation of the topological Dirac states. In the present study, the Mn-Bi-Te films grown by the MBE technique onto Si(111) substrates with decreasing Bi and Te contents and increasing Mn content were investigated by 0.5-6.5 eV spectroscopic ellipsometry. In addition, the 0.004-0.9 eV infrared (IR) transmittance spectra were examined. An effective medium model was used to reproduce the measured ellipsometric angles, Psi(omega) and Delta(omega), of the Mn-Bi-Te films in terms of the constructed model, including film thickness, surface roughness, and volume fractions of two (MnTe and Bi2Te3) or three constituents, the latter being associated with the structural inhomogeneities contribution. The results obtained for the inhomogeneous Mn-Bi-Te films using the three-phase EMA model indicate that the defect-associated optical response systematically shifts to higher photon energies from ~1.95 to ~2.43 eV with decreasing Te and Bi contents and increasing Mn content, pointing out that the electrons become more deeply localized in the formed structural inhomogeneities. The obtained results indicate that the structure of the non-stoichiometric Mn-Bi-Te films is not continuous but represented by regions of nearly stoichiometric MnBi2Te4 phase, which includes hollows or quantum anti-dots (QADs). The measured FIR transmittance spectra for the non-stoichiometric Mn-Bi-Te films show substantially reduced (or absent) contribution(s) from free charge carriers, which supports the relevance of localization effects.

cond-mat.str-el↗
arXiv2023

Fingerprints of the Jahn-Teller and superexchange physics in optical spectra of manganites

Transition metal oxides incorporating Jahn-Teller (JT) ions Mn3+ (3d4) in manganites and Cu2+ (3d9) in cuprates exhibit outstanding magnetic and electronic properties, including colossal magnetoresistance (CMR) and high-temperature superconductivity (HTSC). The physics of these compounds is associated with the orbitally-degenerate electronic states of JT ions, leading to the linear electron-lattice interaction, complemented by the entirely electronic superexchange (SE) interaction. Here, we discuss the fingerprints of the JT and SE physics in the temperature-dependent complex dielectric function spectra and multi-order Raman scattering spectra measured in a detwinned LaMnO3 crystal, which is a famous compound exhibiting cooperative JT effect, being also a progenitor of magnetic materials exhibiting CMR effect. In accordance with the obtained experimental evidence, the associated effective parameters characterizing the JT and SE physics in manganites are presented.

cond-mat.str-el↗
arXiv2023

Fingerprints of Mott-Hubbard physics in optical spectra of antiferromagnetic LaTiO3

Magnetic properties of Mott-Hubbard insulators are determined by superexchange interactions mediated by the high-spin (HS) and low-spin (LS) intersite d-d charge excitations, which can be associated with the HS- and LS-Hubbard subbands in optical experiments. To explore the Mott-Hubbard physics in orthorhombic LaTiO_3 crystal exhibiting the G-type antiferromagnetic order at the Neel temperature T_N = 146 K, we present a comprehensive spectroscopic ellipsometry study in the spectral range 0.5-5.6 eV at temperatures 10 K < T < 300 K. We found that the complex dielectric function spectra of LaTiO_3 crystal are almost featureless, nearly isotropic, and weakly temperature dependent in the range of d-d optical transitions. Nonetheless, analyzing the difference spectra below the T_N, we have identified the LS-state d^1d^1 - d^2d^0 excitations at ~3.7 and ~5.15 eV and estimated values of the on-site Coulomb repulsion U ~4.2 eV and Hund's exchange constant J_H ~0.5 eV, which define the energy of the HS-state d^1d^1 - d^2d^0 excitation at ~2.7 eV. In addition, we discovered that the pronounced lowest-energy 1.3 eV optical band displays the critical intensity behavior and anomalous broadening with decreasing temperature below the T_N. The discovered properties indicate that the 1.3 eV band in LaTiO_3 can be associated with a Mott-Hubbard exciton.

cond-mat.str-el↗
arXiv2023

Bismuth layer properties in the ultrathin Bi-FeNi multilayer films probed by spectroscopic ellipsometry

Using wide-band (0.5-6.5 eV) spectroscopic ellipsometry we study ultrathin [Bi(0.6-2.5 nm)-FeNi(0.8,1.2 nm)]N multilayer films grown by rf sputtering deposition, where the FeNi layer has a nanoisland structure and its morphology and magnetic properties change with decreasing the nominal layer thickness. From the multilayer model simulations of the ellipsometric angles, Psi(omega) and Delta(omega), the complex (pseudo)dielectric function spectra of the Bi layer were extracted. The obtained results demonstrate that the Bi layer can possess the surface metallic conductivity, which is strongly affected by the morphology and magnetic properties of the nanoisland FeNi layer in the GMR-type Bi-FeNi multilayer structures.

cond-mat.mtrl-sci↗
arXiv2022

Raman scattering study and lattice-dynamics calculations in YTiO3: Precursor of the magnetic phase transition in the phonon anomalies

The origin of the low-temperature ferromagnetic instability in YTiO3 driven by the interplay between lattice, orbital, spin, and charge degrees of freedom is on the background of lattice dynamics. We present a comprehensive study of temperature-dependent polarized Raman scattering in a nearly stoichiometric orthorhombic YTiO3 single crystal. The lattice-dynamics calculations authenticate the assignment for the observed Ag- and B2g-symmetry modes in terms of the atoms vibrational patterns. The obtained results suggest that trigonal GdFeO3-type distortions become unstable against tetragonal Jahn-Teller distortions, leading to the consequent orbital structure refinement and ferromagnetic ground state in YTiO3.

cond-mat.str-el↗
arXiv2021

Localization effects in the disordered Ta interlayer of multilayer Ta-FeNi films: Evidence from dc transport and spectroscopic ellipsometry study

Using dc transport and wide-band spectroscopic ellipsometry techniques, we study localization effects in the disordered metallic Ta interlayer of different thickness in the multilayer films (MLFs) (Ta - FeNi)_N grown by rf sputtering deposition. In the grown MLFs, the FeNi layer was 0.52 nm thick, while the Ta layer thickness varied between 1.2 and 4.6 nm. The Ta layer dielectric function was extracted from the Drude-Lorentz simulation. The dc transport study of the MLFs implies non-metallic (dr/dT<0) behavior, with negative temperature coefficient of resistivity (TCR). The TCR absolute value increases upon increasing the Ta interlayer thickness, indicating enhanced electron localization. With that, the free charge carrier Drude response decreases. Moreover, the pronounced changes occur at the extended spectral range, involving the higher-energy Lorentz bands. The Drude dc conductivity drops below the weak localization limit for the thick Ta layer. The global band structure reconstruction may indicate the formation of a nearly localized many-body electron state.

cond-mat.str-el↗
arXiv2020

Control of Mooij correlations at the nanoscale in the disordered metallic Ta - nanoisland FeNi multilayers

Localisation phenomena in highly disordered metals close to the extreme conditions determined by the Mott-Ioffe-Regel (MIR) limit when the electron mean free path is approximately equal to the interatomic distance is a challenging problem. Here, to shed light on these localisation phenomena, we studied the dc transport and optical conductivity properties of nanoscaled multilayered films composed of disordered metallic Ta and magnetic FeNi nanoisland layers, where ferromagnetic FeNi nanoislands have giant magnetic moments of 10^3-10^5 Bohr magnetons (μ_B). In these multilayered structures, FeNi nanoisland giant magnetic moments are interacting due to the indirect exchange forces acting via the Ta electron subsystem. We discovered that the localisation phenomena in the disordered Ta layer lead to a decrease in the Drude contribution of free charge carriers and the appearance of the low-energy electronic excitations in the 1-2 eV spectral range characteristic of electronic correlations, which may accompany the formation of electronic inhomogeneities. From the consistent results of the dc transport and optical studies we found that with an increase in the FeNi layer thickness across the percolation threshold evolution from the superferromagnetic to ferromagnetic behaviour within the FeNi layer leads to the delocalisation of Ta electrons from the associated localised electronic states. On the contrary, we discovered that when the FeNi layer is discontinuous and represented by randomly distributed superparamagnetic FeNi nanoislands, the Ta layer normalized dc conductivity falls down below the MIR limit by about 60%. The discovered effect leading to the dc conductivity fall below the MIR limit can be associated with non-ergodicity and purely quantum (many-body) localisation phenomena, which need to be challenged further.

cond-mat.str-el↗
arXiv2018

Collective magnetic response of inhomogeneous nanoisland FeNi films around the percolation transition

By using superconducting quantum interference device (SQUID) magnetometry we investigated anisotropic high-field (H < 7 T) low-temperature (10 K) magnetization response of inhomogeneous nanoisland FeNi films grown by rf sputtering deposition on Sitall (TiO2) glass substrates. In the grown FeNi films, the FeNi layer nominal thickness varied from 0.6 to 2.5 nm, across the percolation transition at the d_c=1.8 nm. We discovered that, beyond conventional spin-magnetism of Fe21Ni79 permalloy, the extracted out-of-plane magnetization response of the nanoisland FeNi films is not saturated in the range of investigated magnetic fields and exhibits paramagnetic-like behavior. We found that the anomalous out-of-plane magnetization response exhibits an escalating slope with increase in the nominal film thickness from 0.6 to 1.1 nm, however, it decreases with further increase in the film thickness, and then practically vanishes on approaching the FeNi film percolation threshold. At the same time, the in-plane response demonstrates saturation behavior above 1.5-2 T, competing with anomalously large diamagnetic-like response, which becomes pronounced at high magnetic fields. It is possible that the supported-metal interaction leads to the creation of a thin charge-transfer (CT) layer and a Schottky barrier at the FeNi film/Sitall (TiO2) interface. Then, in the system with nanoscale circular domains, the observed anomalous paramagnetic-like magnetization response can be associated with a large orbital moment of the localized electrons. The observed magnetization response is determined by the interplay between the paramagnetic- and diamagnetic-like contributions.

cond-mat.str-el↗
arXiv2014

Optical evidence of quantum rotor orbital excitations in orthorhombic manganites

In magnetic compounds with Jahn-Teller (JT) ions (such as Mn3+ or Cu2+), the ordering of the electron or hole orbitals is associated with cooperative lattice distortions. There the role of JT effect, although widely recognised, is still elusive in the ground state properties. We suggest that, in these materials, there exist elementary excitations whose energy spectrum is described in terms of the total angular momentum eigenstates and is quantised as in quantum rotors found in JT centers. We observed features originating from these excitations in the optical spectra of a model compound LaMnO3 using ellipsometry technique. They appear clearly as narrow sidebands accompanying the electron transition between the JT split orbitals on neighbouring Mn3+ ions, strongly influenced by anisotropic spin correlations. We present these results together with new experimental data on photoluminescence and its kinetics found in LaMnO3, which lend additional support to the ellipsometry implying the existence of the quantum rotor orbital excitations. We note that the discovered elementary excitations of quantum rotors may play an important role in many unusual properties observed in these materials upon doping, such as high-temperature superconductivity and colossal magnetoresistance.

cond-mat.str-el↗
arXiv2014

Anomalous multi-order Raman scattering in LaMnO_3: a signature of a quantum lattice effect in a Jahn-Teller crystal

The multi-order Raman scattering is studied up to a fourth order for a detwinned LaMnO_3 crystal. Based on a comprehensive data analysis of the polarisation-dependent Raman spectra, we show that the anomalous features in the multi-order scattering could be the sidebands on the low-energy mode at about 25 cm-1. We suggest that this low-energy mode stems from the tunneling transition between the potential energy minima arising near the Jahn-Teller Mn3+ ion due to the lattice anharmonicity, and the multi-order scattering is activated by this low-energy electronic motion. The sidebands are dominated by the oxygen contribution to the phonon density-of-states, however, there is an admixture of an additional component, which may arise from coupling between the low-energy electronic motion and the vibrational modes.

cond-mat.str-el↗
arXiv2013

Formation of metallic magnetic clusters in a Kondo-lattice metal: Evidence from an optical study

Magnetic materials are usually divided into two classes: those with localised magnetic moments, and those with itinerant charge carriers. We present a comprehensive experimental (spectroscopic ellipsomerty) and theoretical study to demonstrate that these two types of magnetism do not only coexist but complement each other in the Kondo-lattice metal, Tb2PdSi3. In this material the itinerant charge carriers interact with large localised magnetic moments of Tb(4f) states, forming complex magnetic lattices at low temperatures, which we associate with self-organisation of magnetic clusters. The formation of magnetic clusters results in low-energy optical spectral weight shifts, which correspond to opening of the pseudogap in the conduction band of the itinerant charge carriers and development of the low- and high-spin intersite electronic transitions. This phenomenon, driven by self-trapping of electrons by magnetic fluctuations, could be common in correlated metals, including besides Kondo-lattice metals, Fe-based and cuprate superconductors.

cond-mat.str-el↗
arXiv2009

Low-energy Mott-Hubbard excitations in LaMnO_3 probed by optical ellipsometry

We present a comprehensive ellipsometric study of an untwinned, nearly stoichiometric LaMnO_3 crystal in the spectral range 1.2-6.0 eV at temperatures 20 K < T < 300 K. The complex dielectric response along the b and c axes of the Pbnm orthorhombic unit cell, ε^b(ν) and ε^c(ν), is highly anisotropic over the spectral range covered in the experiment. The difference between ε^b(ν) and ε^c(ν) increases with decreasing temperature, and the gradual evolution observed in the paramagnetic state is strongly enhanced by the onset of A-type antiferromagnetic long-range order at T_N = 139.6 K. In addition to the temperature changes in the lowest-energy gap excitation at 2 eV, there are opposite changes observed at higher energy at 4 - 5 eV, appearing on a broad-band background due to the strongly dipole-allowed O 2p -- Mn 3d transition around the charge-transfer energy 4.7 eV. Based on the observation of a pronounced spectral-weight transfer between low- and high-energy features upon magnetic ordering, they are assigned to high-spin and low-spin intersite d^4d^4 - d^3d^5 transitions by Mn electrons. The anisotropy of the lowest-energy optical band and the spectral weight shifts induced by antiferromagnetic spin correlations are quantitatively described by an effective spin-orbital superexchange model. An analysis of the multiplet structure of the intersite transitions by Mn e_g electrons allowed us to estimate the effective intra-atomic Coulomb interaction, the Hund exchange coupling, and the Jahn-Teller splitting energy between e_g orbitals in LaMnO_3. This study identifies the lowest-energy optical transition at 2 eV as an intersite d-d transition, whose energy is substantially reduced compared to that obtained from the bare intra-atomic Coulomb interaction.

cond-mat.str-el↗
arXiv2009

Electron-phonon interaction and spectral weight transfer in Fe$_{1-x}$Co$_{x}$Si

A comprehensive ellipsometric study was performed on Fe$_{1-x}$Co$_{x}$Si single crystals in the spectral range from 0.01 eV to 6.2 eV. Direct and indirect band gaps of 73 meV and 10 meV, respectively, were observed in FeSi at 7 K. One of four infrared-active phonons that is energetically close to the direct absorption edge is coupled both to the electrons and to the low-energy phonon. This is evident from asymmetry in the phonon line shape and a reduction of its frequency when the absorption edge shifts across the phonon energy due to the temperature dependence of the direct band gap. As the temperature increases, the indirect gap changes sign, which manifests as a transition from a semiconductor to a semimetal. The corresponding gain of the spectral weight at low energies was recovered within an energy range of several eV. The present findings strongly support the model indicating that Fe$_{1-x}$Co$_{x}$Si can be well described in an itinerant picture, taking into account self-energy corrections.

cond-mat.mtrl-sci↗
arXiv2008

Ferromagnetism and Lattice Distortions in the Perovskite YTiO$_3$

The thermodynamic properties of the ferromagnetic perovskite YTiO$_3$ are investigated by thermal expansion, magnetostriction, specific heat, and magnetization measurements. The low-temperature spin-wave contribution to the specific heat, as well as an Arrott plot of the magnetization in the vicinity of the Curie temperature $T_C\simeq27$ K, are consistent with a three-dimensional Heisenberg model of ferromagnetism. However, a magnetic contribution to the thermal expansion persists well above $T_C$, which contrasts with typical three-dimensional Heisenberg ferromagnets, as shown by a comparison with the corresponding model system EuS. The pressure dependences of $T_C$ and of the spontaneous moment $M_s$ are extracted using thermodynamic relationships. They indicate that ferromagnetism is strengthened by uniaxial pressures $\mathbf{p}\parallel \mathbf{a}$ and is weakened by uniaxial pressures $\mathbf{p}\parallel \mathbf{b},\mathbf{c}$ and hydrostatic pressure. Our results show that the distortion along the $a$- and $b$-axes is further increased by the magnetic transition, confirming that ferromagnetism is favored by a large GdFeO$_3$-type distortion. The c-axis results however do not fit into this simple picture, which may be explained by an additional magnetoelastic effect, possibly related to a Jahn-Teller distortion.

cond-mat.str-el↗
arXiv2008

Dipole-active optical phonons in YTiO_3: ellipsometry study and lattice-dynamics calculations

The anisotropic complex dielectric response was accurately extracted from spectroscopic ellipsometry measurements at phonon frequencies for the three principal crystallographic directions of an orthorhombic (Pbnm) YTiO_3 single crystal. We identify all twenty five infrared-active phonon modes allowed by symmetry, 7B_1u, 9B_2u, and 9B_3u, polarized along the c-, b-, and a-axis, respectively. From a classical dispersion analysis of the complex dielectric functions \tildeε(ω) and their inverses -1/\tildeε(ω) we define the resonant frequencies, widths, and oscillator strengths of the transverse (TO) and longitudinal (LO) phonon modes. We calculate eigenfrequencies and eigenvectors of B_1u, B_2u, and B_3u normal modes and suggest assignments of the TO phonon modes observed in our ellipsometry spectra by comparing their frequencies and oscillator strengths with those resulting from the present lattice-dynamics study. Based on these assignments, we estimate dynamical effective charges of the atoms in the YTiO_3 lattice. We find that, in general, the dynamical effective charges in YTiO_3 lattice are typical for a family of perovskite oxides. By contrast to a ferroelectric BaTiO_3, the dynamical effective charge of oxygen related to a displacement along the c-axis does not show the anomalously large value. At the same time, the dynamical effective charges of Y and ab-plane oxygen exhibit anisotropy, indicating strong hybridization along the a-axis.

cond-mat.str-el↗
arXiv2008

Signatures of Electronic Correlations in Optical Properties of LaFeAsO$_{1-x}$F$_x$

Spectroscopic ellipsometry is used to determine the dielectric function of the superconducting LaFeAsO$_{0.9}$F$_{0.1}$ ($T_c$ = 27 K) and undoped LaFeAsO polycrystalline samples in the wide range 0.01-6.5 eV at temperatures 10 $\leq T \leq$ 350 K. The free charge carrier response in both samples is heavily damped with the effective carrier density as low as 0.040$\pm$0.005 electrons per unit cell. The spectral weight transfer in the undoped LaFeAsO associated with opening of the pseudogap at about 0.65 eV is restricted at energies below 2 eV. The spectra of superconducting LaFeAsO$_{0.9}$F$_{0.1}$ reveal a significant transfer of the spectral weight to a broad optical band above 4 eV with increasing temperature. Our data may imply that the electronic states near the Fermi surface are strongly renormalized due to electron-phonon and/or electron-electron interactions.

cond-mat.supr-con↗
arXiv2007

Optical response of ferromagnetic YTiO_3 studied by spectral ellipsometry

We have studied the temperature dependence of spectroscopic ellipsometry spectra of an electrically insulating, nearly stoichiometric YTiO_3 single crystal with ferromagnetic Curie temperature T_C = 30 K. The optical response exhibits a weak but noticeable anisotropy. Using a classical dispersion analysis, we identify three low-energy optical bands at 2.0, 2.9, and 3.7 eV. Although the optical conductivity spectra are only weakly temperature dependent below 300 K, we are able to distinguish high- and low-temperature regimes with a distinct crossover point around 100 K. The low-temperature regime in the optical response coincides with the temperature range in which significant deviations from Curie-Weiss mean field behavior are observed in the magnetization. Using an analysis based on a simple superexchange model, the spectral weight rearrangement can be attributed to intersite d_i^1d_j^1 \longrightarrow d_i^2d_j^0 optical transitions. In particular, Kramers-Kronig consistent changes in optical spectra around 2.9 eV can be associated with the high-spin-state (^3T_1) optical transition. This indicates that other mechanisms, such as weakly dipole-allowed p-d transitions and/or exciton-polaron excitations, can contribute significantly to the optical band at 2 eV. The recorded optical spectral weight gain of 2.9 eV optical band is significantly suppressed and anisotropic, which we associate with complex spin-orbit-lattice phenomena near ferromagnetic ordering temperature in YTiO_3.

cond-mat.str-el↗