arXiv subjects

S. Kamba

Publications and source records attributed to S. Kamba.

At least 19 recordsLinked to original sources

arXiv2026

THz-induced phonomagnetism in diamagnetic quantum paraelectric KTaO$_3$

The current efforts striving to develop new ways of data manipulation are aimed at ultrafast control of magnetization in magnetic materials, as well as at inducing magnetic moments in diamagnetics. We demonstrate that in the diamagnetic quantum paraelectric KTaO$_3$, the electric field of circularly polarized THz pulses with an amplitude of $\sim 300\,$kV/cm induces a transient magnetic-like response by resonantly exciting its degenerate soft polar phonon. This phonon-mediated response was measured using the THz pump---optical probe technique via the time-resolved magneto-optic Faraday effect. Our detection scheme was set up to cancel out the major part of the electro-optic Kerr effect which also usually significantly contributes to the transient response. The Kerr-effect-related signal was further suppressed by subtracting the experimental data related to oppositely circularly polarized THz radiation. Thus, we were able to unambiguously identify a temperature-dependent magnetic-like behavior of the KTaO$_3$ crystal manifested by the extracted Faraday rotation. We developed a theoretical model describing well quantitatively the measured curves of the transient Faraday effect signal. However, their amplitudes exhibit an unexpected temperature dependence, which might be a key to a deeper understanding of the observed phonomagnetic effect.

cond-mat.mtrl-sci↗

arXiv2026

Giant dielectric permittivity in Nb-doped rutile crystals

Dielectric properties of Nb-doped (~1.5 at%) rutile single crystals were studied in the 10-300 K temperature range (at frequencies below the MHz range down to 0.3 K) in a broad frequency range, up to terahertz and infrared range, to understand the origin of its giant permittivity. The results were fitted, modelled and compared with those of the undoped rutile crystal measured in the terahertz and infrared ranges. The primary effect originates from the near-electrode depletion layer of lower conductivity compared to the bulk (surface barrier-layer capacitor effect), which causes a strong thermally activated relaxation in the MHz dielectric spectra. In the higher frequency range, the main difference between doped and undoped crystals is the presence of an overdamped microwave excitation (central mode) in the doped crystal for both polarizations, persisting down to 10 K and not thermally activated. This accounts for the previously reported permittivity increase, even at 2 K - where all lower-frequency relaxations are frozen - compared to undoped crystals. It also explains why our low-frequency permittivity at 0.3K exceeds the THz value. The origin of this excitation remains unclear and requires further investigations. Doping affects polar phonons only by slightly increasing their damping.

cond-mat.mtrl-sci↗

arXiv2025

High-Frequency and Microwave Magnetic Properties of Ni$_{0.5}$Zn$_{0.5}$Fe$_2$O$_4$ Spinel Ferrite Ceramics

Magnetic properties of the Ni$_{0.5}$Zn$_{0.5}$Fe$_2$O$_4$ (NZF) spinel ferrite ceramics were studied over a broad frequency range (1 MHz - 50 GHz). Between 10 MHz and 2 GHz, strong temperature-dependent resonance-like magnetic permeability dispersion was observed and attributed to the magnetic domain-wall dynamics. It is responsible for the high magnetic losses, absorption and shielding ability of NZF, and provides high nonlinearity and tunability of the permeability under a weak magnetic field. The attenuation constant of NZF is comparable to those of dielectric-conductor composites and giant permittivity materials. In the microwave range (2-50 GHz), three magnetic excitations dependent on a weak magnetic field were revealed and related to magnons. The lowest-frequency magnon (<10 GHz) is attributed to the natural ferromagnetic resonance, two others are excited between 28 and 44 GHz. Interaction of the magnons and magneto-dielectric resonance modes with electromagnetic waves provides high absorption and shielding efficiency in the GHz range, including 5G and 6G communication frequencies.

cond-mat.mtrl-sci↗

arXiv2025

Suppression of ferromagnetism in van der Waals insulator due to pressure-induced layer stacking variation

Ferromagnetism in van der Waals insulators like CrBr3 is highly sensitive to structural modifications. We explore the pressure-driven structural and magnetic transformations of the van der Waals magnet CrBr3, establishing it as a model platform for phenomena emerging in layered vdW systems. Single-crystal X-ray diffraction revealed intrinsic trimorphism with two known phases (monoclinic and rhombohedral) and a so-far unreported trigonal phase. The paracrystal model well captures the coexistence of the rhombohedral and trigonal phases at ambient conditions. Increasing pressure drives the growth of the AA-stacked trigonal phase at the expense of the rhombohedral phase, which becomes undetectable above 8.4 GPa. Magnetization measurements provided the first direct evidence of a collapse of ferromagnetism above 5.8 GPa. This behavior is attributed to the increasing number of AFM-coupled Cr moments in AA stackings. Ab initio DFT calculations of electronic structure and atomistic simulations of finite-temperature magnetism corroborate the scenario.

cond-mat.mtrl-sci↗

arXiv2024

A frustrated antipolar phase analogous to classical spin liquids

The study of magnetic frustration in classical spin systems was motivated by the prediction and discovery of classical spin liquid states. These uncommon magnetic phases are characterized by a massive degeneracy of their ground state implying a finite magnetic entropy at zero temperature. While the classical spin liquid state was originally predicted in the Ising triangular lattice antiferromagnet in 1950, this state has never been experimentally observed in any triangular magnets. We report here the discovery of an electric analogue of classical spin liquids on a triangular lattice of uniaxial electric dipoles in EuAl12O19 . This new type of frustrated antipolar phase is characterized by a highly degenerate state at low temperature implying an absence of long-range antiferroelectric order, despite short-range antipolar correlations. Its dynamics are governed by a thermally activated process, slowing down upon cooling towards a complete freezing at zero temperature.

cond-mat.str-el↗

arXiv2024

Microwave magnetic excitations in U-type hexaferrite Sr$_4$CoZnFe$_{36}$O$_{60}$ ceramics

Microwave (MW) transmission, absorption, and reflection loss spectra of the ferrimagnetic U-type hexaferrite Sr$_4$CoZnFe$_{36}$O$_{60}$ ceramics were studied from 100 MHz to 35 GHz at temperatures between 10 and 390 K. 9 MW magnetic excitations with anomalous behavior near the ferrimagnetic phase transitions were revealed. They also change under the application of weak bias magnetic field (0 - 700 Oe) at room temperature. 6 pure magnetic modes are assigned to dynamics of the magnetic domain walls and inhomogeneous magnetic structure of the ceramics, to the natural ferromagnetic resonance (FMR) and to the higher-frequency magnons. Three modes are considered as the magnetodielectric ones with dominating influence of the magnetic properties on their temperature and field dependences. Presence of the natural FMR in all ferrimagnetic phases proves existence of the non-zero internal magnetization and magnetocrystalline anisotropy. Splitting of the FMR into the two components without magnetic bias was observed in the collinear phase and is attributed to a change of the magnetocrystalline anisotropy during the phase transition. The high-frequency FMR component critically slows down to the phase transition. At room temperature, the FMR splitting and essential suppression of the higher-frequency modes was revealed under the weak bias field (300 - 700 Oe). The highly nonlinear MW response and the FMR splitting are caused by the gradual evolution of the polydomain magnetic structure to a monodomain one. The high number of magnetic excitations observed in the MW region confirms the suitability of using hexaferrite Sr$_4$CoZnFe$_{36}$O$_{60}$ ceramics as MW absorbers, shielding materials and highly tunable filters.

cond-mat.mtrl-sci↗

arXiv2024

Two Displacive Ferroelectric Phase Transitions in Multiferroic Quadruple Perovskite $BiMn_{7}O_{12}$

We report on the microwave, terahertz (THz), infrared and Raman spectroscopic studies of $BiMn_{7}O_{12}$ ceramics, shedding more light into the nature of two structural phase transitions and their possible relation with ferroelectricity in this compound. We observed a softening of one polar phonon in the THz range on cooling towards 460 and 300 K, i.e., temperatures at which $BiMn_{7}O_{12}$ undergoes subsequent structural phase transitions from monoclinic $\textit{I2/m}$ to polar monoclinic $\textit{Im}$ and triclinic $\textit{P1}$ phases. The soft phonon causes dielectric anomalies typical for displacive ferroelectric phase transitions. Microwave measurements performed at 5.8 GHz up to 400 K qualitatively confirmed not only the dielectric anomaly at 300 K, but also revealed two other weak dielectric anomalies near the magnetic phase transitions at 60 K and 28 K. This evidences the multiferroic nature of the low-temperature phases, although the relatively high conductivity in the kHz and Hz spectral range prevented us from directly measuring the permittivity and ferroelectric polarization. Some Raman modes sense the magnetic phase transitions occurring near 60 and 25 K, showing that spin-phonon coupling is relevant in this compound and in this temperature range. The deviation of the Mn-O stretching mode frequency from the anharmonic temperature behavior was successfully explained by the spin correlation function calculated from the magnetic contribution to the specific heat.

cond-mat.mtrl-sci↗

arXiv2024

Strong impact of low-level substitution of Mn by Fe on the magnetoelectric coupling in $TbMnO_{3}$

The correlation between static magnetoelectric coupling and magnetic structure was investigated in $TbMn_{0.98}Fe_{0.02}O_{3}$ with magnetic field up to 8 T and down to 2 K. Single-crystal neutron diffraction experiments reveal a substantial increase in the temperature dependence of the incommensurate modulation wave vector of the antiferromagnetic phase as the magnetic field strength increases. Magnetic field-dependent pyroelectric current measurements revealed significantly higher magnetoelectric coupling at magnetic fields below 4 T than in pure TbMnO3. This is due to the higher sensitivity of the incommensurably modulated cycloid structure to weak magnetic fields. Detailed analysis of our data confirmed that the ferroelectric polarization is induced by inverse Dzyaloshinskii-Moriya interaction for magnetic field strength up to 4 T, but at higher fields a departure from theoretical predictions is ascertained, giving evidence for an additional, as yet misunderstood, contribution to magnetoelectric coupling. It shows that a small 2% substitution of Mn3+ by Fe3+ has a strong impact on the magnetic structure, promoting the destabilization of the incommensurably modulated magnetic cycloidal structure of $TbMnO_{3}$ in a magnetic field above 5 T. We demonstrate that the magnetoelectric coupling magnitude can be tuned through suitable substitutional elements, even at low level, inducing local lattice distortions with different electronic and magnetic properties.

cond-mat.mtrl-sci↗

arXiv2023

Modifying the magnetoelectric coupling in TbMnO$_3$ by low-level Fe$^{3+}$ substitution

We report a comprehensive study of the low-level substitution of Mn$^{3+}$ by Fe$^{3+}$ effect on the static and dynamic magnetoelectric coupling in TbMn$_{1-x}$Fe$_x$O$_3$ ($x=0$, 0.02 and 0.04). The cationic substitution has a large impact on the balance between competitive magnetic interactions and, as a result, on the stabilization of the magnetic structures and ferroelectric phase at low temperatures. Low-lying electromagnon excitation is activated in the cycloidal modulated antiferromagnetic and ferroelectric phase in TbMnO$_3$, while it is observed up to TN in the Fe-substituted compounds, pointing for different mechanisms for static and dynamic magnetoelectric coupling. A second electrically active excitation near 40 cm$^{-1}$ is explained by means of Tb3+ crystal-field effects. This excitation is observed up to room temperature, and exhibits a remarkable 15 cm$^{-1}$ downshift on cooling in Fe-substituted compounds. Both electromagnon and crystal-field excitations are found to be coupled to the polar phonons with frequencies up to 250 cm$^{-1}$. Raman spectroscopy reveals a spin-phonon coupling below TN in pure TbMnO$_3$, but the temperature where the coupling start to be relevant increases with Fe concentration and reaches 100 K in TbMn$_{0.96}$Fe$_{0.04}$O$_3$. The anomalies in the T-dependence of magnetic susceptibility above TN are well accounted by spin-phonon coupling and crystal-field excitation, coupled to oxygen motions.

cond-mat.mtrl-sci↗

arXiv2017

Infrared, terahertz, and microwave spectroscopy of the soft and central modes in Pb(Mg1/3Nb2/3)O3

From the new infrared (IR) reflectivity and time-domain terahertz (THz) spectra combined with available high-frequency dielectric data above the MHz range in a broad temperature range of 10-900 K, a full picture of the soft and central mode behavior in the classical relaxor ferroelectric Pb(Mg1/3Nb2/3)O3 (PMN) is suggested. A detailed comparison is given with the recent hyper-Raman spectroscopy data (Phys. Rev. Lett. 117, 155501 (2016)), and also with other available experiments based on inelastic light and neutron scattering. The closest agreement is with the hyper-Raman data, both techniques yield the same number of soft-mode components and the same high-temperature softening towards the temperature T* ~ 400 K. In addition to evaluation of the IR-THz data using fitting with standard factorized form of the dielectric function, we performed a successful fitting of the same data using the effective medium approach (EMA), originally based on the assumption that the mesoscopic structure of PMN consists of randomly oriented uniaxially anisotropic polar nanodomains (PNDs) with somewhat harder TO polar modes in the direction along the local PND dipole (Phys. Rev. Lett. 96, 027601 (2006)). Evaluation using the Bruggeman EMA modelling has been successfully applied in the entire investigated temperature range. These results suggest that the response perpendicular to the local dipole moment, at high temperatures induced by random fields rather than PNDs, undergoes a classical softening from high temperatures with permittivity obeying the Curie-Weiss law, eps_per = C/(T-Tc), C = 1.7 x 10^5 K and Tc = 380 K. Below the Burns temperature ~620 K, a GHz relaxation ascribed to flipping of the PNDs emerges from the soft mode response, slows down and broadens, remaining quite strong towards the cryogenic temperatures, where it can be assigned to fluctuations of the PND boundaries.

cond-mat.mtrl-sci↗

arXiv2016

Magnetic resonance study of bulk and thin film EuTiO3

Magnetic resonance spectra of EuTiO3 in both bulk and thin film form were taken at temperatures from 3-350 K and microwave frequencies from 9.2-9.8 and 34 GHz. In the paramagnetic phase, magnetic resonance spectra are determined by magnetic dipole and exchange interactions between Eu2+ spins. In the film, a large contribution arises from the demagnetization field. From detailed analysis of the linewidth and its temperature dependence, the parameters of spin-spin interactions were determined: the exchange frequency is 15-15.5 GHz and the estimated critical exponent of the spin correlation length is ~ 0.5. In the bulk samples, the spectra exhibited a distinct minimum in the linewidth at the N\'eel temperature, T_N = 5.5 K, while the resonance field practically does not change even on cooling below T_N. This is indicative of a small magnetic anisotropy ~ 320 G in the antiferromagnetic phase. In the film, the magnetic resonance spectrum is split below T_N into several components due to excitation of the magnetostatic modes, corresponding to a non-uniform precession of magnetization. Moreover, the film was observed to degrade over two years. This was manifested by an increase of defects and a change in the domain structure. The saturated magnetization in the film, estimated from the magnetic resonance spectrum, was about 900 emu/cm3 or 5.5 mu_B/unit cell at T = 3.5 K.

cond-mat.mtrl-sci↗

arXiv2016

Broad-band dielectric response of BTZ-BCT piezoceramics: soft and central mode behaviour

Dielectric properties of BTZ-BCT ceramics were probed in the frequency range from 10 Hz to 100 THz in a broad temperature range (10-900 K). Polar soft phonon observed in infrared spectra softens with cooling, however below 500 K its frequency becomes temperature independent. Simultaneously, a central mode activates in terahertz and microwave spectra; and it actually drives the ferroelectric phase transitions. Consequently, the phase transition strongly resemble a crossover between the dispacive and order-disorder type. The central mode vanishes below 200 K. The dielectric relaxation in the radiofrequency and microwave range anomalously broadens on cooling below T$_{C1}$ resulting in the nearly frequency independent dielectric loss bleow 200 K. This broadening comes from a broad frequency distribution of ferroelectric domain wall vibrations. Raman spectra reveal new phonons below 400 K, i.e. already 15 K above T$_{C1}$. Several weak modes are detected in the paraelectric phase up to 500 K in the Raman spectra. Activation of these modes is ascribed to the presence of polar nanoclusters in the material.

cond-mat.mtrl-sci↗

arXiv2015

Spin and lattice excitations of a BiFeO3 thin film and ceramics

We present a comprehensive study of polar and magnetic excitations in BiFeO3 ceramics and a thin film epitaxially grown on an orthorhombic (110) TbScO3 substrate. Infrared reflectivity spectroscopy was performed at temperatures from 5 to 900 K for the ceramics and below room temperature for the thin film. All 13 polar phonons allowed by the factor-group analysis were observed in theceramic samples. The thin-film spectra revealed 12 phonon modes only and an additional weak excitation, probably of spin origin. On heating towards the ferroelectric phase transition near 1100 K, some phonons soften, leading to an increase in the static permittivity. In the ceramics, terahertz transmission spectra show five low-energy magnetic excitations including two which were not previously known to be infrared active; at 5 K, their frequencies are 53 and 56 cm-1. Heating induces softening of all magnetic modes. At a temperature of 5 K, applying an external magnetic field of up to 7 T irreversibly alters the intensities of some of these modes. The frequencies of the observed spin excitations provide support for the recently developed complex model of magnetic interactions in BiFeO3 (R.S. Fishman, Phys. Rev. B 87, 224419 (2013)). The simultaneous infrared and Raman activity of the spin excitations is consistent with their assignment to electromagnons.

cond-mat.mtrl-sci↗

arXiv2014

Strong spin-phonon coupling in infrared and Raman spectra of SrMnO3

Infrared reflectivity spectra of cubic SrMnO$_{3}$ ceramics reveal 18 % stiffening of the lowest-frequency phonon below the antiferromagnetic phase transition occurring at T$_{N}$ = 233 K. Such a large temperature change of the polar phonon frequency is extraordinary and we attribute it to an exceptionally strong spin-phonon coupling in this material. This is consistent with our prediction from first principles calculations. Moreover, polar phonons become Raman active below T$_{N}$, although their activation is forbidden by symmetry in $Pm\bar{3}m$ space group. This gives evidence that the cubic $Pm\bar{3}m$ symmetry is locally broken below T$_{N}$ due to a strong magnetoelectric coupling. Multiphonon and multimagnon scattering is also observed in Raman spectra. Microwave and THz permittivity is strongly influenced by hopping electronic conductivity, which is caused by small non-stoichiometry of the sample. Thermoelectric measurements show room-temperature concentration of free carriers $n_{e}=$3.6 10$^{20}$ cm$^{-3}$ and the sample composition Sr$^{2+}$Mn$_{0.98}^{4+}$Mn$_{0.02}^{3+}$O$_{2.99}^{2-}$. The conductivity exhibits very unusual temperature behavior: THz conductivity increases on cooling, while the static conductivity markedly decreases on cooling. We attribute this to different conductivity of the ceramic grains and grain boundaries.

cond-mat.mtrl-sci↗

arXiv2013

Lattice instabilities in bulk EuTiO3

The phase purity and the lattice dynamics in bulk EuTiO3 were investigated both microscopically, using X-ray and neutron diffraction, 151-Eu-Mössbauer spectroscopy, and 151-Eu nuclear inelastic scattering, and macroscopically using calorimetry, resonant ultrasound spectroscopy, and magnetometry. Furthermore, our investigations were corroborated by ab initio theoretical studies. The perovskite symmetry, Pm-3m, is unstable at the M- and R- points of the Brillouin zone. The lattice instabilities are lifted when the structure relaxes in one of the symmetries: I4/mcm, Imma, R-3c with relative relaxation energy around -25 meV. Intimate phase analysis confirmed phase purity of our ceramics. A prominent peak in the Eu specific density of phonon states at 11.5 meV can be modelled in all candidate symmetries. A stiffening on heating around room temperature is indicative of a phase transition similar to the one observed in SrTiO3, however, although previous studies reported the structural phase transition to tetragonal I4/mcm phase our detailed sample purity analysis and thorough structural studies using complementary techniques did not confirm a direct phase transition. Instead, in the same temperature range, Eu delocalization is observed which might explain the lattice dynamical instabilities.

cond-mat.str-el↗

arXiv2012

Absence of ferroelectricity in BiMnO3 ceramics

We performed factor-group analysis of all phonons in possible monoclinic C2/c and C2 structures of BiMnO3 and compared it with our experimental infrared and Raman spectra. We conclude that the crystal structure is centrosymmetric C2/c in the whole investigated temperature range from 10 to 550 K, therefore BiMnO3 cannot be ferroelectric. We revealed a dielectric relaxation in THz spectra above the structural phase transition taking place at T_C1=475 K giving evidence in strong lattice anharmonicity and a large dynamical disorder of Bi cations above T_C1. Step-like dielectric anomaly observed at T_C1 in THz permittivity reminds antiferroelectric phase transition. Nevertheless, the low-temperature dielectric studies did not reveal any antiferroelectric or ferroelectric hysteresis loop. Our experimental results support theoretical paper of P. Baettig et al. (J. Am. Chem. Soc. 129, 9854 (2007)) claiming that BiMnO3 is not multiferroic, but only antipolar ferromagnet.

cond-mat.mtrl-sci↗

arXiv2012

Antiferrodistortive phase transition in EuTiO3

X-ray diffraction, dynamical mechanical analysis and infrared reflectivity studies revealed an antiferrodistortive phase transition in EuTiO3 ceramics. Near 300K the perovskite structure changes from cubic Pm-3m to tetragonal I4/mcm due to antiphase tilting of oxygen octahedra along the c axis (a0a0c- in Glazer notation). The phase transition is analogous to SrTiO3. However, some ceramics as well as single crystals of EuTiO3 show different infrared reflectivity spectra bringing evidence of a different crystal structure. In such samples electron diffraction revealed an incommensurate tetragonal structure with modulation wavevector q ~ 0.38 a*. Extra phonons in samples with modulated structure are activated in the IR spectra due to folding of the Brillouin zone. We propose that defects like Eu3+ and oxygen vacancies strongly influence the temperature of the phase transition to antiferrodistortive phase as well as the tendency to incommensurate modulation in EuTiO3.

cond-mat.mtrl-sci↗

arXiv2012

Optical Response of DyN

We report measurements of the optical response of polycrystalline DyN thin films. The frequency-dependent complex refractive index in the near IR-visible-near UV was determined by fitting reflection/transmission spectra. In conjunction with resistivity measurements these identify DyN as a semiconductor with 1.2 eV optical gap. When doped by nitrogen vacancies it shows free carrier absorption and a blue-shifted gap associated with the Moss-Burstein effect. The refractive index of 2.0+/-0.1 depends only weakly on energy. Far infrared reflectivity data show a polar phonon of frequency 280 cm-1 and dielectric strength delta epsilon= 20.

cond-mat.mtrl-sci↗