arXiv subjects

M. N. Popova

Publications and source records attributed to M. N. Popova.

At least 19 recordsLinked to original sources

arXiv2026

The ground ytterbium doublet in h-YbMnO3 and the related low-temperature peculiarities of the compound

We have performed detailed temperature-dependent study of optical f-f transitions of the Yb3+ ions in h-YbMnO3 by means of Fourier-transform spectroscopy. The splitting of the ground Kramers doublet as a function of temperature, D0(T), for the Yb3+ ion at 4b site was determined. The D0(T) function follows the dynamics of the manganese magnetic moment below TN = 87 K, indicating, that the ytterbium subsystem is magnetized by the magnetic field generated by an ordered manganese subsystem, which is consistent with the results of previous studies. Excitation of the upper component of the split ground doublet plays a significant role in low-temperature dynamics of the h-YbMnO3 crystal. Using the D0(T) function we calculated the temperature behavior of the of the Yb(4b) magnetic moment: it is in clear agreement with the neutron data [Phys. Rev. B 98, 134413, 2018]. The calculated contribution of Yb(4b) to heat capacity definitely explains the origin of the Schottky anomaly in the CP(T) dependence. A scenario for phase transitions in h-YbMnO3 is proposed in which the energy gain in the ytterbium system plays a key role.

cond-mat.str-el↗

arXiv2026

In-plane and out-of-plane electric dipoles and phase transitions in 2D-layered TlGaS2

Out-of-plane and in-plane electric polarization, which rarely coexist in a two-dimensional (2D) ferroelectric material, offer different advantages in ferroelectricity-based devices. Here, we report the coexistence of in-plane and out-of-plane electric dipoles, along with various phase transitions, in 2D van der Waals layered TlGaS2 single crystal. Quantum paraelectricity was observed along both in-plane and out-of-plane directions of the TlGaS2 crystal. Detailed investigation of the quantum paraelectric soft-mode behavior reveals a close correlation between the electric dipoles and the off-center displacement of Tl1+ ions with 6s2 lone pairs in TlGaS2. Anomalies near temperatures of about 120 K and 60-75 K in dielectric and/or infrared spectra indicate the existence of local or weak long-range structural transitions in TlGaS2. Our results provide important experimental evidence for elucidating the phase transitions and coexistence of in-plane and out-of-plane electric dipoles in 2D layered TlGaS2.

cond-mat.mtrl-sci↗

arXiv2026

High-resolution spectroscopy of Pr3+ions in YAl3(BO3)4:Pr3+. Crystal-field, hyperfine,and electron-deformation interactions

Optical transmission spectra of YAl3(BO3)4 crystals doped with the Pr3+ ions in concentrations 1 and 2.5 at. % were studied by high-resolution (up to 0.05 cm-1) Fourier spectroscopy, including in magnetic field parallel to the trigonal c axis of the crystal. The g factors of several crystal-field doublets of Pr3+ were determined. The crystal-field calculations performed using the exchange-charge model and high-resolution spectroscopy data allowed us to obtain a physically reasonable set of crystal-field parameters. The observed splitting of a number of doublets in zero magnetic field is explained by the presence of random lattice deformations. Simulation of the profiles of observed deformational doublets was carried out taking into account both hyperfine and electron-deformation interactions. The width of the distribution function of random strains was estimated. The main sources of random strains in YAl3(BO3)4:Pr3+ crystals are discussed.

physics.optics↗

arXiv2025

High-resolution luminescence spectroscopy of CaWO$_4$:Ho$^{3+}$: Sensitive detection of internal strains, temperature, and magnetic field

We carried out high-resolution (0.02 cm-1) measurements of the photoluminescence (PL) spectra of CaWO4:Ho3+, including in magnetic field, and performed spectra modeling. Well-resolved hyperfine structure was observed in the luminescence spectra of CaWO4:Ho3+ for the first time. Energies of several crystal-field levels were specified, g-factors were determined. Variations of a magnetic field as small as several tenths of mT can be detected from the PL spectra. We show that the PL spectra are much more sensitive to lattice strains in CaWO4:Ho3+ than the absorption spectra. The spectra were simulated using refined crystal-field parameters and taking into account both hyperfine and deformation interactions. Here, we used the previously obtained distribution function of random strains induced by point lattice defects in an elastically anisotropic CaWO4 crystal. A luminescence thermometer for temperatures around 20 K based on CaWO4:Ho3+ is suggested.

physics.optics↗

arXiv2017

Lattice dynamics and electronic transitions in a structurally-complex layered copper borate Cu$_3$(BO$_3$)$_2$

Copper borate Cu$_3$(BO$_3$)$_2$ is a complex compound with a layered crystallographic structure in which the Jahn-Teller active and magnetic copper Cu$^{2+}$ ions occupy sixteen nonequivalent positions in the unit cell displaying controversial magnetic behavior. In this paper, we report on the infrared and Raman spectroscopic studies of the lattice dynamics and the electronic structure of 3$d^9$ copper states below the fundamental absorption band. The lattice dynamics is characterized by a large number of phonons due to a low $P\overline{1}$ space group symmetry and a large unit cell with Z=10. Unusually rich set of phonons was found in the low-energy part of the infrared and Raman spectra below 100 cm$^{-1}$, which we tentatively assign to interlayer vibrations activated by a crystal superstructure and/or to weak force constants for modes related to some structural groups. Several phonons show anomalous behavior in the vicinity of the magnetic phase transition at $T_N$=10 K thus evidencing magnetoelastic interaction. No new phonons were found below $T_N$, which excludes the spin-Peierls type of the magnetic transition. In the region of electronic transitions, a strong broad absorption band centered at $\sim$1.8 eV is observed, which we assign to overlapping of transitions between the 3$d^9$ states of Cu$^{2+}$ ions split by the crystal field in nonequivalent positions. The fundamental charge-transfer absorption band edge has a complex structure and is positioned around $\sim$2.8-3.0 eV.

cond-mat.mtrl-sci↗

arXiv2016

Spectroscopy of f-f transitions, crystal-field calculations, and magnetic and quadrupole helix chirality in DyFe$_3$(BO$_3$)$_4$

Recently, quadrupole helix chirality and its domain structure was observed in resonant x-ray diffraction experiments on DyFe$_3$(BO$_3$)$_4$ using circularly polarized x rays [T. Usui et al., Nature Materials 13, 611 (2014)]. We show that this effect can be explained quantitatively by calculating the quadrupole moments of the Dy$^{3+}$ ions induced by the low-symmetry ($C_2$) crystal-field (CF) component. In this work, the CF parameters for the Dy$^{3+}$ ions in the $P3_121$ ($P3_221$) phase of DyFe$_3$(BO$_3$)$_4$ are obtained from CF calculations based on the analysis of high-resolution temperature-dependent optical spectroscopy data. We also consider the helix chirality of the single-site magnetic susceptibility tensors of the Dy$^{3+}$ ions in the paramagnetic $P3_121$ ($P3_221$) phase and suggest a neutron diffraction experiment to reveal it.

cond-mat.mtrl-sci↗

arXiv2016

Probing Dy3+ magnetic moments in multiferroic perovskite DyMnO3 by optical spectroscopy

We present a detailed temperature-dependent spectroscopic study of DyMnO3 single crystals with distorted perovskite structure. Energies of 36 crystal-field levels of Dy3+ in paramagnetic DyMnO3 were determined. The Dy3+ ground Kramers doublet does not split at T_N^Mn = 39 K and splits below Tlock = 18 K. The splitting grows fast at temperatures near T_N^Dy = 6.5 K and reaches Δ0 = 11 cm-1 at 4 K. Using the experimental temperature dependence Δ0(T), we calculate the dysprosium magnetic moment mDy(T) and the dysprosium contribution into specific heat and magnetic susceptibility. Analysing all the experimental data, we conclude that the Dy-Mn interaction is of the Dzyaloshinskii-Moriya type.

cond-mat.str-el↗

arXiv2016

Bifurcations observed in the spectra of coupled electron-phonon modes in multiferroic $PrFe_3(BO_3)_4$ subjected to a magnetic field

We report on bifurcations effect mediated by the electron-phonon coupling in a concentrated rare-earth-containing antiferromagnet, observed in the spectra of coupled $4f$-electron-phonon modes under the influence of an external magnetic field. The effect was observed in the low-temperature far-infrared (terahertz) reflection spectra of a multiferroic easy-axis antiferromagnet $PrFe_3(BO_3)_4$ in magnetic fields $\textbf{B}_{ext}||c$. Both paramagnetic and magnetically ordered phases (including a spin-flop one) were studied in magnetic fields up to 30 T. We show that the field behavior of the coupled modes can be successfully explained and modeled on the base of the equation derived in the frame of the theory of coupled electron-phonon modes, with the same field-independent electron-phonon interaction constant $|W| = 14.8 cm^{-1}$.

cond-mat.mtrl-sci↗

arXiv2016

Lattice dynamics and a magnetic-structural phase transition in the nickel orthoborate $Ni_{3}(BO_{3})_{2}$

Nickel orthoborate $Ni_{3}(BO_{3})_{2}$ having a complex orthorhombic structure $P_{nnm}$ (#58, Z=2) of the kotoite type is known for quite a long time as an antiferromagnetic material below $T_{N}$ = 46 K, but up to now its physical properties including the lattice dynamics have not been explored. Six magnetic nickel $Ni^{2+}$ ions (S=1) in the unit cell are distributed over the 2a and 4f positions in the centers of distorted $[O_{6}]$ octahedra. The $[NiO_{6}]$ units are linked via rigid $[BO_{3}]$ groups and these structural particularities impose restrictions on the lattice dynamics and spin-phonon interactions. We performed the symmetry analysis of the phonon modes at the center of the Brillouin zone. The structural parameters and phonon modes were calculated using Dmol3 program. We report and analyze results of infrared and Raman studies of phonon spectra measured in all required polarizations. Most of the even and odd phonons predicted on the basis of the symmetry analysis and theoretical calculations were reliably identified in the measured spectra. Absorption measurements in the infrared region showed emergence of several very narrow and weak phonons at the magnetic ordering temperature $T_{N}$. This observation proves the existence of a structural phase transition not reported before which is evidently coupled intrinsically with the magnetic dynamics of $Ni_{3}(BO_{3})_{2}$. A clear evidence of spin-phonon interaction was observed for some particular phonons below $T_{N}$.

cond-mat.mtrl-sci↗

arXiv2015

Infrared study of lattice dynamics and spin-phonon and electron-phonon interactions in multiferroic TbFe3(BO3)4 and GdFe3(BO3)4

We present a comparative far-infrared reflection spectroscopy study of phonons, phase transitions, spin-phonon and electron-phonon interactions in isostructural multiferroic iron borates of gadolinium and terbium. The behavior of phonon modes registered in a wide temperature range is consistent with a weak first-order structural phase transition (Ts = 143 for GdFe3(BO3)4 and 200 K for TbFe3(BO3)4) from high-symmetry high-temperature R32 structure into low-symmetry low-temperature P3121 one. The temperature dependences of frequencies, oscillator strengths, and damping constants of some low-frequency modes reveal an appreciable lattice anharmonicity. Peculiarities in the phonon mode behavior in both compounds at the temperature of an antiferromagnetic ordering (TN = 32 K for GdFe3(BO3)4 and 40 K for TbFe3(BO3)4) evidence the spin-phonon interaction. In the energy range of phonons, GdFe3(BO3)4 has no electronic levels but TbFe3(BO3)4 possesses several ones. We observe an onset of new bands in the excitation spectrum of TbFe3(BO3)4, due to a resonance interaction between a lattice phonon and 4f electronic crystal-field excitations of Tb3+. This interaction causes delocalization of the CF excitations, their Davydov splitting, and formation of coupled electron-phonon modes.

cond-mat.str-el↗

arXiv2015

Luminescent Ge-related centre in high-pressure synthesized diamond

We report on the high-pressure synthesis of novel nano- and microcrystalline high-quality diamonds with luminescent Ge-related centers. Observation of the four-line fine structure in luminescence at 2 eV (602 nm) at temperatures below 80 K manifests a high quality of diamonds. We demonstrate germanium and carbon isotope shifts in the fine structure of luminescence at 602 nm and its vibrational sideband which allows us to unambiguously associate the center with the germanium impurity entering into the diamond lattice. We show that there are two ground-state energy levels with the separation of 0.7 meV and two excited-state levels separated by 4.6 meV in the electronic structure of the center and suggest a split-vacancy structure of this center.

cond-mat.mtrl-sci↗

arXiv2014

Antiferromagnetic dichroism and Davydov splitting of 3d-excitons in a complex multisublattice magnetoelectric CuB2O4

The space and time symmetry breaking at magnetic phase transitions in multiferroics results in a number of strongly pronounced optical effects. Our high-resolution spectroscopic study of 3d- excitons in a complex multi-sublattice magnetoelectric CuB2O4 demonstrates that, among those, a large antiferromagnetic linear dichroism is observed which is highly sublattice-sensitive to subtle changes in the spin subsystems. We prove that the discovered linear dichroism is related microscopically to the magnetic Davydov splitting of the exciton states. We announce a novel magnetic phase transition and argue that an elliptical spiral structure rather than a simple circular helix is realized in the incommensurate phase, these findings being overlooked in previous studies by optical and other techniques. We claim that this spectroscopic method can be effectively applied to other materials for revealing hidden features of magnetic structures and phase transitions.

cond-mat.mtrl-sci↗

arXiv2014

Splitting of a nondegenerate phonon mode in PrFe3(BO3)4: 4f crystal-field level between TO and LO phonon frequencies

A new effect originating from the crystal-field-excitation - phonon coupling was observed (in the far infrared spectra of a multiferroic PrFe3(BO3)4). The reststrahlen band corresponding to the A2 symmetry nondegenerate phonon mode near 50 cm-1 (1.5 THz) splits into two bands at about 100 K, well above TN = 32 K. These bands shift and narrow progressively with further lowering the temperature, demonstrating pronounced peculiarities at TN. The observed effects were explained by an interaction of the A2 phonon mode with the 4f crystal-field electronic excitation of Pr3+ whose frequency falls into the TO - LO frequency region of the phonon mode. Inversion of the TO and LO frequencies for the electronic excitation and a formation of coupled electron-phonon modes are discussed. Fitting of the TO frequency vs temperature experimental plots by theoretical curves revealed the value 14.6 cm-1 for the electron-phonon coupling constant.

cond-mat.mtrl-sci↗

arXiv2007

Optical spectra, crystal-field parameters, and magnetic susceptibility of the new multiferroic NdFe3(BO3)4

We report high-resolution optical absorption spectra for NdFe3(BO3)4 trigonal single crystal which is known to exhibit a giant magnetoelectric effect below the temperature of magnetic ordering TN = 33 K. The analysis of the temperature-dependent polarized spectra reveals the energies and, in some cases, symmetries and exchange splittings of Nd3+ 84 Kramers doublets. We perform crystal-field calculations starting from the exchange-charge model, obtain a set of six real crystal-field parameters, and calculate wave functions and magnetic g-factors. In particular, the values g(perpendicular) = 2.385, g(parallel) = 1.376 were found for the Nd3+ ground-state doublet. We obtain Bloc=7.88 T and |JFN|= 0.48 K for the values of the local effective magnetic field at liquid helium temperatures at the Nd3+ site and the Nd - Fe exchange integral, respectively, using the experimentally measured Nd3+ ground-state splitting of 8.8 cm-1. To check reliability of our set of crystal field parameters we model the magnetic susceptibility data from literature. A dimer containing two nearest-neighbor iron ions in the spiral chain is considered to partly account for quasi-one-dimensional properties of iron borates, and then the mean-field approximation is used. The results of calculations with the exchange parameters for Fe3+ ions Jnn = -6.25 K (intra-chain interactions) and Jnnn = -1.92 K (inter-chain interactions) obtained from fitting agree well with the experimental data.

cond-mat.str-el↗

arXiv2001

Lattice vibrations of alpha'-NaV_2O_5 in the low-temperature phase. Magnetic bound states?

We report high resolution polarized infrared studies of the quarter-filled spin ladder compound alpha'-NaV_2O_5 as a function of temperature (5K <= T <= 300K). Numerous new modes were detected below the temperature T_c=34K of the phase transition into a charge ordered nonmagnetic state accompanied by a lattice dimerization. We analyse the Brillouin zone (BZ) folding due to lattice dimerization at T_c and show that some peculiarities of the low-temperature vibrational spectrum come from quadruplets folded from the BZ point (1/2, 1/2, 1/4). We discuss an earlier interpretation of the 70, 107, and 133cm-1 modes as magnetic bound states and propose the alternative interpretation as folded phonon modes strongly interacting with charge and spin excitations.

cond-mat.str-el↗

arXiv2000

High resolution infrared absorption spectra, crystal field, and relaxation processes in CsCdBr_3:Pr^3+

High resolution low-temperature absorption spectra of 0.2% Pr^3+ doped CsCdBr_3 were measured in the spectral region 2000--7000 cm-1. Positions and widths of the crystal field levels within the 3H5, 3H4, 3F2, and 3F3 multiplets of the Pr^3+ main center have been determined. Hyperfine structure of several spectral lines has been found. Crystal field calculations were carried out in the framework of the semiphenomenological exchange charge model (ECM). Parameters of the ECM were determined by fitting to the measured total splittings of the 3H4 and 3H6 multiplets and to the observed in this work hyperfine splittings of the crystal field levels. One- and two-phonon relaxation rates were calculated using the phonon Green's functions of the perfect (CsCdBr_3) and locally perturbed (impurity dimer centers in CsCdBr_3:Pr^3+) crystal lattice. Comparison with the measured linewidths confirmed an essential redistribution of the phonon density of states in CsCdBr_3 crystals doped with rare-earth ions.

cond-mat↗

arXiv1998

High frequency dielectric and magnetic anomaly at the phase transition in NaV2O5

We found anomalies in the temperature dependence of the dielectric and the magnetic susceptibiliy of NaV_2O_5 in the microwave and far infrared frequency ranges. The anomalies occur at the phase transition temperature T_c, at which the spin gap opens. The real parts of the dielectric constants epsilon_a and epsilon_c decrease below T_c. The decrease of epsilon_a (except for the narrow region close to T_c) is proportional to the intensity of the x-ray reflection appearing at T_c. The dielectric constant anomaly can be explained by the zigzag charge ordering in the ab-plane appearing below T_c. The anomaly of the microwave magnetic losses is probably related to the coupling between the spin and charge degrees of freedom in vanadium ladders.

cond-mat.str-el↗

arXiv1998

Lattice vibrations of alpha'-NaV2O5

We have measured far infrared reflectance and transmittance spectra as well as Raman scattering spectra of α'-NaV2O5 single crystals for all the principal polarizations. The temperature range above the phase transition temperature T_c=35 K was investigated, mainly. On the basis of this experimental study and of the lattice dynamics calculations we conclude that the symmetry of NaV2O5 in the high temperature phase is described by the centrosymmetric D_{2h}^{13} space group. The assignment of the observed phonons is given. Values of dielectric constants are obtained from the infrared data. Asymmetric shapes of several infrared lines as well as higher order infrared vibrational spectra are discussed. The crystal field energy levels of the 3d electron localized at the V^{4+} site have been calculated in the framework of the exchange charge model using the values of effective charges obtained from the lattice dynamics calculations. According to the results of these calculations, the earlier observed broad optical bands in the region of 1 eV can be interpreted as phonon assisted d-d transitions.

cond-mat.str-el↗