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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., Comment: 23 pages, 15 figures, 6 tables

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 $\Gamma$ 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., Comment: 17 pages, 11 figures, 5 tables

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.

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 (N\'eel) 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., Comment: Main article contains 7 pages, 3 figures. With Supplementary material

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., Comment: 12 pages, 7 figure

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., Comment: 13 pages, 8 figures

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., Comment: 18 pages, 9 figures, 5 tables

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 N\'eel 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., Comment: Main text: 23 pages, 4 figures Supplementary Materials: 8 pages, 1 figure

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., Comment: 11 pages, 8 figures, 2 tables, 2 tables

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., Comment: 20 pages, 8 figures, 2 tables

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 N\'eel 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., Comment: 10 pages, 7 figures

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., Comment: 16 pages, 13 figures

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., Comment: 35 pages, 13 figures, to be published in Solid State Physics Journal (St. Petersburg, Russia as translation of Fizika Tverdogo Tela)

A time-resolved optical pump-probe technique has been applied for studying the ultrafast dynamics in the magnetic semiconductor EuTe near the absorption band gap. We show that application of external magnetic field up to 6 T results in crossover from the inverse Faraday effect taking place on the femtosecond time scale to the optical orientation phenomenon with an evolution in the picosecond time domain. We propose a model which includes both these processes possessing different spectral and temporal properties. The circularly polarized optical pumping induces the optical electronic transition $4f^75d^0 \rightarrow 4f^65d^1$ forming the absorption band gap in EuTe. The observed crossover is related to a strong magnetic-field shift of the band gap in EuTe at low temperatures. It was found that manipulation of spin states on intrinsic defect levels takes place on a time scale of 19 ps in the applied magnetic field of 6 T., Comment: 11 pages, 4 figures

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., Comment: 11 pages, 8 figures, 2 tables, 68 references

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 N\'eel point. The experimental signals are described as dynamics of magnetic linear dichroism due to longitudinal oscillations of the antiferromagnetic vector., Comment: 25 pages, 10 figures

Terahertz driven magnetization dynamics are explored in the orthoferrite DyFeO3. A high-field, single cycle THz pulse is used to excite magnon modes in the crystal together with other resonances. Both quasi-ferromagnetic and quasi-antiferromagnetic magnon modes are excited and appear in time-resolved measurements of the Faraday rotation. Other modes are also observed in the measurements of the time-resolved linear birefringence. Analysis of the excitation process reveals that despite larger than expected electro-optical susceptibility it is mainly the THz magnetic field that couples to the quasi-ferromagnetic and quasi-antiferromagnetic magnon branches., Comment: 10 pages, 4 figures

Lattice and magnetic dynamics of NiWO$_4$ single crystals were studied with the use of polarized Raman spectroscopy in a wide temperature range of 10-300 K including the antiferromagnetic ordering temperature $T_N$=62 K. Static magnetic measurements were used for characterizing the single crystals. All Raman-active phonons predicted by the group theory were observed and characterized. Magnetic symmetry analysis was used to determine possible magnetic space groups for NiWO$_4$ which can be also applied to any other isostructural crystal with the same magnetic propagation vector k=(1/2,0,0). Though the magnetic structure of NiWO$_4$ is relatively simple, a rich set of narrow and broad magnetic excitations with different polarization properties and temperature behavior in the very broad frequency range of 10-200 cm$^{-1}$ was observed, with some modes surviving at temperatures much higher than $T_N$ up to 220 K. Part of the magnetic excitations was identified as acoustic and optical spin-wave branches which allow us to construct exchange structure and estimate exchange and anisotropy constants with the use of linear spin-wave theory. Since the magnetic structure can be described as exchange-coupled AFM chains of $S=1$ ions, previously unobserved magnetic excitation at 24 cm$^{-1}$ is tentatively assigned to a Haldane gap mode.

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 $T_{N}$., Comment: New version: 29 pages, 10 figures, 73 references

We explore a thermal mechanism of changing the anisotropy by femtosecond laser pulses in dielectric ferrimagnetic garnets by taking a low symmetry (YBiPrLu)3(FeGa)5O12 film grown on the (210)-oriented Gd3Ga5O12 substrate as a model media. We demonstrate by means of spectral magneto-optical pump-probe technique and phenomenological analysis, that the magnetization precession in such a film is triggered by laser-induced changes of the growth-induced magnetic anisotropy along with the well-known ultrafast inverse Faraday effect. The change of magnetic anisotropy is mediated by the lattice heating induced by laser pulses of arbitrary polarization on a picosecond time scale. We show that the orientation of the external magnetic field with respect to the magnetization easy plane noticeably affects the precession excited via the anisotropy change. Importantly, the relative contributions from the ultrafast inverse Faraday effect and the change of different growth-induced anisotropy parameters can be controlled by varying the applied magnetic field strength and direction. As a result, the amplitude and the initial phase of the excited magnetization precession can be gradually tuned., Comment: 16 pages, 10 figures, 2 table

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridge the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter triggered by the impulsive optical generation of spin excitations with the shortest possible nanometer-wavelength and femtosecond-period. Our experiments also disclose a possibility for the coherent control of these femtosecond nanomagnons, which are defined by the exchange energy. These findings open up novel opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and high-temperature superconductivity, since they provide a macroscopic probe of the femtosecond dynamics of sub-nanometer spin-spin correlations and, ultimately, of the exchange energy. With this approach it becomes possible to trace the dynamics of such short-range magnetic correlations for instance during phase transitions. Moreover, our work suggests that nanospintronics and nanomagnonics can employ phase-controllable spin waves with frequencies in the 20 THz domain.

Ultrafast non-thermal manipulation of magnetization by light relies on either indirect coupling of the electric field component of the light with spins via spin-orbit interaction or direct coupling between the magnetic field component and spins. Here we propose a novel scenario for coupling between the electric field of light and spins via optical modification of the exchange interaction, one of the strongest quantum effects, the strength of which can reach 1000 Tesla. We demonstrate that this isotropic opto-magnetic effect, which can be called the inverse magneto-refraction, is allowed in a material of any symmetry. Its existence is corroborated by the experimental observation of THz emission by magnetic-dipole active spin resonances optically excited in a broad class of iron oxides with a canted spin configuration. From its strength we estimate that a sub-picosecond laser pulse with a moderate fluence of ~ 1 mJ/cm^2 acts as a pulsed effective magnetic field of 0.01 Tesla, arising from the optically perturbed balance between the exchange parameters. Our findings are supported by a low-energy theory for the microscopic magnetic interactions between non-equilibrium electrons subjected to an optical field which suggests a possibility to modify the exchange interactions by light over 1 %.

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., Comment: 5 pages, 4 figures

Nonlinear optics of semiconductors is an important field of fundamental and applied research, but surprisingly the role of excitons in the coherent processes leading to harmonics generation has remained essentially unexplored. Here we report results of a comprehensive experimental and theoretical study of the three-photon process of optical second harmonic generation (SHG) involving the exciton resonances of the noncentrosymmetric hexagonal wide-band-gap semiconductor ZnO in the photon energy range of 3.2-3.5 eV. Resonant crystallographic SHG is observed for the 1s(A,B), 2s(A,B), 2p(A,B), and 1s(C) excitons. We show that strong SHG signals at these exciton resonances are induced by the application of a magnetic field when the incident and the SHG light wave vectors are along the crystal z-axis where the crystallographic SHG response vanishes. A microscopic theory of SHG generation through excitons is developed, which shows that the nonlinear interaction of coherent light with excitons has to be considered beyond the electric-dipole approximation. Depending on the particular symmetry of the exciton states SHG can originate from the electric- and magnetic-field-induced perturbations of the excitons due to the Stark effect, the spin as well as orbital Zeeman effects, or the magneto-Stark effect. The importance of each mechanism is analyzed and discussed by confronting experimental data and theoretical results for the dependencies of the SHG signals on photon energy, magnetic field, electric field, crystal temperature, and light polarization. Good agreement is obtained between experiment and theory proving the validity of our approach to the complex problem of nonlinear interaction of light with ZnO excitons. This general approach can be applied also to other semiconductors., Comment: 23 pages, 16 figures

Amplification of the photocurrent in heterostructures of silicon dioxide films containing cobalt nanoparticles grown on gallium arsenide SiO2(Co)/GaAs has been observed in magnetic field in the avalanche regime. While the avalanche process is suppressed by the magnetic field and the current decreases, for photon energy E greater than the GaAs bandgap energy the photocurrent significantly increases. The amplification reaches 9.5 for E = 1.50 eV. The effect of the photocurrent amplification is explained by the spin-dependent recombination process at deep impurity centers in GaAs., Comment: 5 pages, 6 figures

We report on optical studies of the thin films of multiferroic hexagonal (P.G. 6mm) rare-earth orthoferrites RFeO3 (R=Ho, Er, Lu) grown epitaxially on a (111)-surface of ZrO2(Y2O3) substrate. The optical absorption study in the range of 0.6-5.6 eV shows that the films are transparent below 1.9 eV; above this energy four broad intense absorption bands are distinguished. The absorption spectra are analyzed taking into account the unusual fivefold coordination of the Fe(3+) ion. Temperature dependence of the optical absorption at 4.9 eV shows anomaly at 124 K, which we attribute to magnetic ordering of iron sublattices., Comment: 8 pages, 3 figures, 22 references. Copyright (2012) American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in Journal of Applied Physics and may be found at http://link.aip.org/link/?jap/111/056105

Three independent contributions to the magnetically induced spontaneous polarization of multiferroic TbMn2O5 are uniquely separated by optical second harmonic generation and an analysis in terms of Landau theory. Two of them are related to the magnetic Mn3+/4+ order and are independent of applied fields of up to 7 T. The third contribution is related to the long-range antiferromagnetic Tb3+ order. It shows a drastic decrease upon the application of a magnetic field and mediates the change of sign of the spontaneous electric polarization in TbMn2O5. The close relationship between the rare-earth long-range order and the non-linear optical properties points to isotropic Tb-Tb exchange and oxygen spin polarization as mechanism for this rare-earth induced ferroelectricity., Comment: 8 pages, 5 figures

Terahertz and far-infrared electric and magnetic responses of hexagonal piezomagnetic YMnO3 single crystals are investigated. Antiferromagnetic resonance is observed in the spectra of magnetic permeability mu_a [H(omega) oriented within the hexagonal plane] below the Neel temperature T_N. This excitation softens from 41 to 32 cm-1 on heating and finally disappears above T_N. An additional weak and heavily-damped excitation is seen in the spectra of complex dielectric permittivity epsilon_c within the same frequency range. This excitation contributes to the dielectric spectra in both antiferromagnetic and paramagnetic phases. Its oscillator strength significantly increases on heating towards room temperature thus providing evidence of piezomagnetic or higher-order couplings to polar phonons. Other heavily-damped dielectric excitations are detected near 100 cm-1 in the paramagnetic phase in both epsilon_c and epsilon_a spectra and they exhibit similar temperature behavior. These excitations appearing in the frequency range of magnon branches well below polar phonons could remind electromagnons; however, their temperature dependence is quite different. We have used density functional theory for calculating phonon dispersion branches in the whole Brillouin zone. A detailed analysis of these results and of previously published magnon dispersion branches brought us to the conclusion that the observed absorption bands stem from phonon-phonon and phonon- paramagnon differential absorption processes. The latter is enabled by a strong short-range in-plane spin correlations in the paramagnetic phase., Comment: subm. to PRB

Spectroscopy of the centrosymmetric magnetic semiconductors EuTe and EuSe reveals spin-induced optical second harmonic generation (SHG) in the band gap vicinity at 2.1-2.4eV. The magnetic field and temperature dependence demonstrates that the SHG arises from the bulk of the materials due to a novel type of nonlinear optical susceptibility caused by the magnetic dipole contribution combined with spontaneous or induced magnetization. This spin-induced susceptibility opens access to a wide class of centrosymmetric systems by harmonics generation spectroscopy., Comment: 5 pages, 3 figures, submitted to PRL