arXiv subjects

R. V. Pisarev

Publications and source records attributed to R. V. Pisarev.

At least 19 recordsLinked to original sources

arXiv2026

Nonlinear Optical Probing of Ferroic-Octupolar Order Parameter in Collinear Altermagnet

Altermagnetism as a new concept in condensed matter physics is currently being thoroughly investigated. Despite the absence of macroscopic magnetization, altermagnets host a hidden spin order whose direct detection remains a challenge. Here we report on the observation of electric and magnetic dipole forbidden optical second-harmonic generation (SHG) in the altermagnet CoF$_2$ with a centrosymmetric lattice and spin order. We demonstrate that below the Néel temperature $T_N = 38$ K the SHG signal is sensitive to the ferrotype magnetic octupole $\mathbf{\mathcal{O}}^M$ which is the order parameter in the antiferromagnetic phase. By combining polarization-resolved SHG experimental data and a phenomenological symmetry analysis, we show that the altermagnetic spin structure of CoF$_2$ enables a ferroic-octupole-induced electric-quadrupolar nonlinear polarization $\mathbf{P}^{2ω} = \mathrm i\varepsilon_{0}{ }^c\mathbfχ^{(3)}(\mathbf{\mathcal{O}}^M) :\mathbf{E}^ω \nabla \mathbf{E}^ω$. The temperature dependence of SHG reveals a phase transition at $T_N$ confirming the spin origin of the observed signal. The SHG response is resonantly enhanced by a coherent three-photon process caused by the electronic $d$-$d$ transitions of the Co$^{2+}$ ion. Model calculations of SHG polarization rotational anisotropies and temperature dependencies give a reasonable agreement with experimental data, proving the disclosed nonlinear contribution. Our results establish SHG as a novel sensitive tool of ferroic-octupolar spin ordering and highlight the potential of CoF$_2$ and other altermagnets for further nonlinear optical investigations and applications.

cond-mat.str-el↗

arXiv2025

Switching of an antiferromagnet controlled by spin canting in a laser-induced hidden phase

During laser-induced phase transitions, fast transformations of electronic, atomic, and spin configurations often involve emergence of hidden and metastable phases. Being inaccessible under any other stimuli, such phases are indispensable for unveiling mechanisms and controlling the transitions. We experimentally explore spin kinetics during ultrafast first-order 90$^{\circ}$ spin-reorientation (SR) transition in a canted antiferromagnet Fe$_3$BO$_6$, and reveal that the transition is controlled by the canting between the magnetic sublattices. Laser-induced perturbation of the Dzyaloshinskii-Moriya interaction results in a change of the intersublattice canting within first picoseconds, bringing Fe$_3$BO$_6$ to a hidden phase. Once this phase emerges, laser-induced heating activates precessional 90$^\circ$ spin switching. Combination of the spin canting and heating controls the final spin configuration comprising coexisting initial and switched phases. Extended phase coexistence range is in a striking contrast to the narrow SR transition in Fe$_3$BO$_6$ induced by conventional heating.

cond-mat.str-el↗

arXiv2025

Spin and lattice dynamics at the spin-reorientation transitions in the rare-earth orthoferrite Sm$_{0.55}$Tb$_{0.45}$FeO$_{3}$

Linear and non-linear couplings of magnetic and lattice excitations are at the heart of many fascinating magnetophononic phenomena observed in rare-earth orthoferrites, the distinctive feature of which is the tendency to spin-reorientation transitions. Here we report the results of the experimental study of the spin and lattice dynamics in the Brillouin zone center of the rare-earth orthoferrite Sm$_{0.55}$Tb$_{0.45}$FeO$_{3}$ by using polarized infrared reflectivity and Raman scattering spectroscopic techniques. The obtained results were supported by the first-principles calculations, which allowed us to reliably identify the parameters of most infrared- and Raman-active phonons. We reveal the spin-reorientation transitions $Γ_{4}(G_{a}F_{c}) \overset{T_{1}}\longleftrightarrow Γ_{24}(G_{ac}F_{ac}) \overset{T_{2}}\longleftrightarrow Γ_{2}(G_{c}F_{a})$ at $T_{1} \simeq 220$ K and $T_{2} \simeq 130$ K and carefully studied the following evolution of Raman scattering on magnetic excitations at these transitions. Notably, the intermediate magnetic structure $Γ_{24}$ displays an exceptionally broad temperature range $Δ{T} = T_{1} - T_{2} \simeq 90$ K in mixed Sm$_{0.55}$Tb$_{0.45}$FeO$_{3}$ compared to pure rare-earth orthoferrites. We attribute this broadening of the intermediate phase to the modification of the magnetocrystalline anisotropy as a result of the inhomogeneous magnetic structure caused by the random distribution of rare-earth $\mathrm{Sm}^{3+}$ and $\mathrm{Tb}^{3+}$ ions. We found neither change in the parameters of Raman-active $B_{1g}$ phonons nor the appearance of new phonons induced by spin-reorientation transitions, which have been reported in $\mathrm{SmFeO}_{3}$. We assume that our results provide a solid basis for more deeper understanding of magnetophononic phenomena in rare-earth orthoferrites.

cond-mat.mtrl-sci↗

arXiv2025

Antiferromagnetic nonreciprocity of light emission in CuB$_2$O$_4$

Nonreciprocity of light emission, when the radiation intensity differs for two opposite propagation directions, is a rare phenomenon in solids because it requires a violation of the crystal symmetry with respect to time-reversal. Such violation via time-reversal symmetry breaking can occur either due to an applied magnetic field or due to a magnetic ordering. We perform a detailed theoretical and experimental study of the photoluminescence (PL) nonreciprocity in the noncentrosymmetric tetragonal antiferromagnet CuB$_2$O$_4$, where this effect reaches 80\% below the Néel phase transition temperature of $T_N = 20$~K. The effect is observed for three sets of extremely narrow exciton and exciton-magnon PL lines, associated with Frenkel excitons on the Cu$^{2+}$ ions in the magnetic $4b$ subsystem. A strong manifestation of the nonreciprocity of emission is found in certain geometries for the commensurate antiferromagnetic phase, as well as in other phases with incommensurate spin ordering. In accordance with the magnetic symmetry of CuB$_2$O$_4$, the nonreciprocity of emission is observed for light propagation along certain directions within the easy (001) plane. A rigorous quantum-mechanical analysis of the wave functions of the initial and final states of the Cu$^{2+}$ ions responsible for the PL is performed for various experimental geometries of the crystallographic axes and the applied magnetic field. The analysis confirms that the nonreciprocity of emission from Frenkel excitons in CuB$_2$O$_4$ is due to the interference of magnetic-dipole and electric-dipole transitions of antiferromagnetically ordered $4b$ spins of the Cu$^{2+}$ ions, in good agreement with the experimental data.

cond-mat.mtrl-sci↗

arXiv2024

Lattice dynamics and mixing of polar phonons in the rare-earth orthoferrite TbFeO$_{3}$

Rare-earth orthoferrites are a promising platform for antiferromagnetic spintronics with a rich variety of terahertz spin and lattice dynamics phenomena. For instance, it has been experimentally demonstrated that the light-driven optical phonons can coherently manipulate macroscopic magnetic states via nonlinear magnetophononic effects. Here using TbFeO$_{3}$ as an example, we reveal the origin of the mode mixing between the LO and TO phonons, which is important for understanding of nonlinear phononics. We performed a comprehensive study of the lattice dynamics of the TbFeO$_{3}$ single crystal by polarized infrared and Raman scattering spectroscopic techniques, and experimentally obtained and carefully analyzed the spectra of anisotropic complex dielectric functions in the far-infrared spectral range. This allowed us to reliably identify the symmetries and parameters of most infrared- and Raman-active phonons. Next, the experimental studies were supplemented by the lattice dynamics calculations which allowed us to propose the normal mode assignments. We reveal that the relation between LO and TO polar phonons is complex and does not strictly follow the ``LO-TO rule'' due to the strong mode mixing. We further analyze how displacements of different ions contribute to phonon modes and reveal that magnetic Fe ions are not involved in Raman-active phonons, thus shedding light on a lack of spin phonon coupling for such phonons. The obtained results establish a solid basis for further in-depth experimental research in the field of nonlinear phononics and magnetophononics in rare-earth orthoferrites.

cond-mat.mtrl-sci↗

arXiv2024

Polar phonons and magnetic excitations in the antiferromagnet CoF$_2$

The coupling between antiferromagnetic spins and infrared-active phonons in solids is responsible for many intriguing phenomena and is a field of intense research with extensive potential applications in the modern devices based on antiferromagnetic spintronics and phononics. Insulating rutile antiferromagnetic crystal CoF$_2$ is one of the model materials for studying nonlinear magnetophononics due to the strong spin-lattice coupling as a result of the orbitally degenerate ground state of Co$^{2+}$ ions manifested in the plethora of static and induced piezomagnetic effects. Here we report results on the complete infrared spectroscopy study of lattice and magnetic dynamics in CoF$_2$ in a wide temperature range and their careful analysis. We observed that infrared-active phonons demonstrate frequency shifts at the antiferromagnetic ordering. Furthermore, using first-principles calculations, we examined the lattice dynamics and disclosed that these frequency shifts are rather due to the spin-phonon coupling than geometrical lattice effects. Next we found that the low-frequency dielectric permittivity demonstrates distinct changes at the antiferromagnetic ordering due to the spontaneous magnetodielectric effect caused by the behavior of infrared-active phonons. In addition, we have observed magnetic excitations in the infrared spectra and identified their magnetodipole origin. To strengthen our conclusions, we analyze the theoretical phonon-magnon coupling overall phonons at the $Γ$ point. We conclude that the largest effect comes from the $A_{1g}$ and $B_{2g}$ Raman-active modes. As such, our results establish a solid basis for further investigations and more deeper understanding of the coupling of phonons with spins and magnetic excitations in antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2024

Giant intrinsic nonlinear phonon-magnon coupling in the antiferromagnet CoF$_2$

The observation of strongly coupled lattice and spin dynamics in altermagnet CoF$_2$ is reported. On the background of the expected spin-phonon interaction leading to renormalization of all phonons at the Neel temperature an additional strong coupling between one-magnon excitation and the lowest frequency Raman-active phonon of B1g symmetry was observed and manifested an anomaly in its energy, full width, and intensity at temperature T*=23 K precisely where the frequency of the phonon becomes exactly twice the frequency of the magnon. We assigned this effect to unique magnon-phonon coupling in the form of a two-magnons-one-phonon interaction. The consistent experimental data clearly demonstrate that there is an intrinsic coupling that does not require coherent excitation.

cond-mat.mtrl-sci↗

arXiv2023

Coherent THz Spin Dynamics in Antiferromagnets Beyond the Approximation of the Néel vector

Controlled generation of coherent spin waves with highest possible frequencies and the shortest possible wavelengths is a cornerstone of spintronics and magnonics. Here, using the Heisenberg antiferromagnet RbMF$_3$, we demonstrate that laser-induced THz spin dynamics corresponding to pairs of mutually coherent counter propagating spin waves with the wavevectors up to the edge of the Brillouin zone cannot be understood in terms of magnetization and antiferromagnetic (Néel) vectors, conventionally used to describe spin waves. Instead, we propose to model such spin dynamics using the spin correlation function. We derive a quantum-mechanical equation of motion for the latter and emphasize that, unlike the magnetization and antiferromagnetic vectors the spin correlations in antiferromagnets do not exhibit inertia.

cond-mat.str-el↗

arXiv2022

Laser-driven first-order spin reorientation and Verwey phase transitions in the magnetite Fe$_3$O$_4$ beyond the range of thermodynamic equilibrium

Ultrafast photo-induced phase transitions occurring under the impact of femtosecond laser pulses provide versatile opport unities for switching solids between distinctly-different crystalline, electronic, and magnetic states and thus modify their functional properties in a significant way. In this paper, we report on the laser-induced spin reorientation and Verwey phase transitions in a single crystalline ferrimagnetic magnetite Fe$_3$O$_4$. Using femtosecond optical and magneto-optical pump-probe techniques, we define the range of the initial sample temperatures and laser fluences when partialor complete photo-induced phase transitions occur from a monoclinic insulating to a cubic metallic state with concomitant switching of magnetic anisotropy from the uniaxial to the cubic one. We thus reveal a connection between these phase transitions when driven by femtosecond laser pulses.Using transient linear and quadratic magneto-optical effects, we examine magnetization dynamics launched the switching of the magnetic anisotropy axis. We unveil the presence of the domains under going the laser-induced phase transitions even below the established threshold fluence for the transitions, as well as when the material is initially in the cubic phase. This is the manifestation of the first-order of these both laser-induced phase transitions beyond the range of thermodynamic equilibrium.

cond-mat.mtrl-sci↗

arXiv2022

Laser-induced THz magnetism of antiferromagnetic CoF$_2$

Excitation, detection and control of coherent THz magnetic excitation in antiferromagnets are challenging problems that can be addressed using ever shorter laser pulses. We study experimentally excitation of magnetic dynamics at THz frequencies in an antiferromagnetic insulator CoF$_2$ by sub-10 fs laser pulses. Time-resolved pump-probe polarimetric measurements at different temperatures and probe polarizations reveal laser-induced transient circular birefringence oscillating at the frequency of 7.45 THz and present below the Néel temperature. The THz oscillations of circular birefringence are ascribed to oscillations of the magnetic moments of Co$^{2+}$ ions induced by the laser-driven coherent E$_g$ phonon mode via the THz analogue of the transverse piezomagnetic effect. It is also shown that the same pulse launches coherent oscillations of the magnetic linear birefringence at the frequency of 3.4 THz corresponding to the two-magnon mode. Analysis of the probe polarization dependence of the transient magnetic linear birefringence at the frequency of the two-magnon mode enables identifying its symmetry.

cond-mat.str-el↗

arXiv2021

Zeeman and Davydov splitting of Frenkel excitons in the antiferromagnet CuB$_2$O$_4$

The optical spectra of antiferromagnetic copper metaborate CuB$_2$O$_4$ are characterized by an exceptionally rich structure of narrow absorption lines due to electronic transitions within the magnetic Cu$^{2+}$ ions, but their unambiguous identification and behavior in magnetic field remain far from being fully understood. We studied the polarized magneto-absorption spectra of this tetragonal antiferromagnet with a high spectral resolution in the range of $1.4055-1.4065$ eV in magnetic fields up to 9.5 T and temperatures from 1.6 up to $T_N = 20$ K. We observed a set of eight absorption lines at $T=1.6$ K in magnetic fields exceeding 1.4 T which we identified as arising from Frenkel excitons related to the ground and the first excited state of Cu$^{2+}$ ions. The number of these excitons is defined by the presence of the four Cu$^{2+}$ ions with the doubly-degenerate spin state $S = 1/2$ at the 4$b$ positions in the crystallographic unit cell. The energies of these excitons are determined the exchange interaction of 0.5 meV of Cu$^{2+}$ ions in the excited state with surrounding ions and by the Davydov splitting of 0.12 meV. In large magnetic field the observed Zeeman splitting is controlled by the anisotropic $g$-factors of both the ground and excited states. We developed a theoretical model of Frenkel excitons in magnetic field that accounts for specific features of the spin structure and exchange interactions in CuB$_2$O$_4$. The model was used for fitting the experimental data and evaluation of Frenkel exciton parameters, such as the Davydov splitting, the molecular exchange energy, and the $g$-factors of the ground and excited states of the Cu$^{2+}$ ions.

cond-mat.other↗

arXiv2021

Incipient geometric lattice instability of cubic fluoroperovskites

Inorganic metal halide perovskites are promising materials for next-generation technologies due to a plethora of unique physical properties, many of which cannot be observed in the oxide perovskites. On the other hand, the search for ferroelectricity and multiferroicity in lead-free inorganic halide perovskites remains a challenging research topic. Here, we experimentally show that cubic fluoroperovskites exhibit proximity to incipient ferroelectrics, which manifested in the softening of the low-frequency polar phonons in the Brillouin zone center at cooling. Furthermore, we reveal the coupling between harmonic and anharmonic force constants of the softening phonons and their correlation with the perovskite tolerance factor. Next, using first-principles calculations, we examine the lattice dynamics of the cubic fluoroperovskites and disclose the incipient lattice instability at which the harmonic force constants of low-lying phonons tend to decrease with a reduction of tolerance factor at all high-symmetry points of the Brillouin zone. The correlations with the tolerance factor indicate the geometric origin of observed incipient lattice instability in the cubic fluoroperovskites caused by the steric effect due to the volume filling of the unit cell by different radius ions. These results provide insights into the lattice dynamics and potential ferroelectric properties of inorganic lead-free metal halide perovskites, relevant to further design and synthesis of new multifunctional materials.

cond-mat.mtrl-sci↗

arXiv2020

Lattice dynamics and spontaneous magnetodielectric effect in ilmenite CoTiO$_3$

Ilmenite-type crystals find a variety of technological applications due to their intriguing physical properties. We present the results of the lattice dynamics studies of honeycomb antiferromagnetic ilmenite CoTiO$_3$ single crystal by the complementary polarized infrared, Raman, and dielectric spectroscopic techniques that are supplemented by the DFT calculations. The frequencies and symmetries of all predicted infrared and Raman active phonons were uniquely identified. Furthermore, it was found that the dielectric permittivity demonstrates distinct changes below antiferromagnetic ordering temperature in zero magnetic field due to spontaneous magnetodielectric effect. Our results establish the reliable basis for further investigation of the coupling of phonons with spins, magnetic excitations and other physical phenomena of this promising material.

cond-mat.mtrl-sci↗

arXiv2020

Magneto-toroidal nonreciprocity of second harmonic generation

The Lorentz reciprocity principle is a fundamental concept that governs light propagation in any optically linear medium in zero magnetic field. Here, we demonstrate experimentally a novel mechanism of reciprocity breaking in nonlinear optics driven by the toroidal moment. Using high-resolution femtosecond spectroscopy at optical electronic resonances in the magnetoelectric antiferromagnet CuB$_2$O$_4$, we show that by controlling the nonlinear interference of coherent sources of second harmonic generation originating from the toroidal spin order, applied magnetic field, and noncentrosymmetric crystal structure, we induce a huge nonreciprocity approaching 100% for opposite magnetic fields. The experimental results are corroborated by a convincing theoretical analysis based on the magnetic and crystal symmetry. These findings open new degrees of freedom in the nonlinear physics of electronic and magnetic structures and pave the way for future nonreciprocal spin-optronic devices operating on the femtosecond time scale.

cond-mat.mtrl-sci↗

arXiv2019

Laser-driven quantum magnonics and THz dynamics of the order parameter in antiferromagnets

The impulsive generation of two-magnon modes in antiferromagnets by femtosecond optical pulses, so-called femto-nanomagnons, leads to coherent longitudinal oscillations of the antiferromagnetic order parameter that cannot be described by a thermodynamic Landau-Lifshitz approach. We argue that this dynamics is triggered as a result of a laser-induced modification of the exchange interaction. In order to describe the oscillations we have formulated a quantum mechanical description in terms of magnon pair operators and coherent states. Such an approach allowed us to} derive an effective macroscopic equation of motion for the temporal evolution of the antiferromagnetic order parameter. An implication of the latter is that the photo-induced spin dynamics represents a macroscopic entanglement of pairs of magnons with femtosecond period and nanometer wavelength. By performing magneto-optical pump-probe experiments with 10 femtosecond resolution in the cubic KNiF$_3$ and the uniaxial K$_2$NiF$_4$ collinear Heisenberg antiferromagnets, we observed coherent oscillations at the frequency of 22 THz and 16 THz, respectively. The detected frequencies as a function of the temperature ideally fit the two-magnon excitation up to the Néel point. The experimental signals are described as dynamics of magnetic linear dichroism due to longitudinal oscillations of the antiferromagnetic vector.

cond-mat.mes-hall↗

arXiv2019

Lattice and magnetic dynamics in polar chiral incommensurate antiferromagnet Ni$_2$InSbO$_6$

Complex systems with coexisting polarity, chirality and incommensurate magnetism are of great interest because they open new degrees of freedom in interaction between different subsystems and therefore they host a plethora of intriguing physical properties. Here we report on optical properties and lattice and spin dynamics of Ni$_2$InSbO$_6$ single crystals studied with the use of polarized optical microscopy and micro-Raman spectroscopy in the temperature range 10-300 K. Ni$_2$InSbO$_6$ crystallizes in a polar structure described by the noncentrosymmetric space group R3 and two types of structural domains were visualized due to natural optical activity of opposite chirality. Raman tensor elements of most A and E phonons along with their symmetry were determined. The manifestation of LO-TO splitting was observed for the A modes. By tracking the temperature dependencies of phonon frequencies the well pronounced spin-phonon interaction was observed for several modes below and above the Néel transition temperature TN = 76 K. In antiferromagnetic phase a wide excitation centred at 247 cm-1 was detected and assigned to the two-magnon mode and this value was used for estimating exchange parameters through linear spin-wave theory calculations.

cond-mat.mtrl-sci↗

arXiv2018

Third harmonic generation on exciton-polaritons in bulk semiconductors subject to a magnetic field

We report on a comprehensive experimental and theoretical study of optical third harmonic generation (THG) on the exciton-polariton resonances in the zinc-blende semiconductors GaAs, CdTe, and ZnSe subject to an external magnetic field, representing a topic that had remained unexplored so far. In these crystals, crystallographic THG is allowed in the electric-dipole approximation, so that no strong magnetic-field-induced changes of the THG are expected. Therefore, it comes as a total surprise that we observe a drastic enhancement of the THG intensity by a factor of fifty for the $1s$-exciton-polariton in GaAs in magnetic fields up to 10 T. In contrast, the corresponding enhancement is moderate for CdTe and almost neglectful for ZnSe. In order to explain this strong variation, we develop a microscopic theory accounting for the optical harmonics generation on exciton-polaritons and analyze the THG mechanisms induced by the magnetic field. The calculations show that the increase of THG intensity is dominated by the magnetic field enhancement of the exciton oscillator strength which is particularly strong for GaAs in the studied range of field strengths. The much weaker increase of THG intensity in CdTe and ZnSe is explained by the considerably larger exciton binding energies, leading to a weaker modification of their oscillator strengths by the magnetic field.

cond-mat.mtrl-sci↗

arXiv2018

Exciton spectroscopy of semiconductors by the method of optical harmonics generation

Nonlinear optical phenomena are widely used for the study of semiconductor materials. The paper presents an overview of experimental and theoretical studies of excitons by the method of optical second and third harmonics generation in various bulk semiconductors (GaAs, CdTe, ZnSe, ZnO, Cu$_2$O, (Cd,Mn)Te, EuTe, EuSe), and low-dimensional heterostructures ZnSe/BeTe. Particular attention is paid to the role of external electric and magnetic fields that modify the exciton states and induce new mechanisms of optical harmonics generation. Microscopic mechanisms of harmonics generation based on the Stark effect, the spin and orbital Zeeman effects, and on the magneto-Stark effect specific for excitons moving in an external magnetic field are considered. This approach makes it possible to study the properties of excitons and to obtain new information on their energy and spin structure that is not available when the excitons are investigated by linear optical spectroscopy. As a result of these studies, a large amount of information was obtained, which allows us to conclude on the establishing of a new field of research - exciton spectroscopy by the method of optical harmonics generation.

cond-mat.mtrl-sci↗