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M. V. Eremin

Publications and source records attributed to M. V. Eremin.

At least 19 recordsLinked to original sources

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↗

Optical magnetoelectric effect in the polar honeycomb antiferromagnet Fe2Mo3O8

The lack of both time-reversal and spatial inversion symmetry in polar magnets is a prerequisite for the occurrence of optical magnetoelectric effects such as nonreciprocal directional dichroism with the potential for the realization of optical diodes. In particular, antiferromagnetic materials with magnetic excitations in the THz range such as Fe2Mo3O8 are promising candidates for next-generation spintronic applications. In a combined experimental and theoretical effort we investigated the THz excitations of the polar honeycomb antiferromagnet Fe2Mo3O8 in external magnetic fields and their nonreciprocal directional dichroism, together with the temperature dependence of the electronic transitions in the mid- and near-infrared frequency range. Using an advanced single-ion approach for the Fe ions, we are able to describe optical excitations from the THz to the near-infrared frequency range quantitatively and successfully model the observed nonreciprocal directional dichroism in the THz regime.

cond-mat.str-el↗

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↗

Magneto-electric properties and low-energy excitations of multiferroic FeCr2S4

We report on the low-frequency optical excitations in the multiferroic ground state of polycrystalline FeCr2S4 in the frequency range 0.3-3~THz and their changes upon applying external magnetic fields up to 7~T. In the ground state below the orbital-ordering temperature T_OO=9K we observe the appearance of several new modes. By applying the external magnetic field parallel and perpendicular to the propagation direction of the THz radiation, we can identify the strongest absorptions to be of predominantly electric-dipole origin. We discuss these modes as the low-energy electronic excitations of the Fe^{2+} ions (3d^6, S=2) in an tetrahedral environment. The eigenfrequencies and relative intensities of these absorption lines are satisfactorily reproduced by our calculation assuming an effective exchange field of 12.8 cm-1 at the Fe^{2+}-ions sites. The direction of the exchange field is found to be slightly tilted out of the ab-plane. With our approach we can also describe previously reported results from Mössbauer studies and the order of magnitude of the electric polarisation induced by orbital and non-collinear spin ordering.

cond-mat.str-el↗

Sub-gap optical response across the structural phase transition in van der Waals layered α-RuCl$_3$

We report magnetic, thermodynamic, thermal expansion, and on detailed optical experiments on the layered compound $α$-RuCl$_3$ focusing on the THz and sub-gap optical response across the structural phase transition from the monoclinic high-temperature to the rhombohedral low-temperature structure, where the stacking sequence of the molecular layers is changed. This type of phase transition is characteristic for a variety of tri-halides crystallizing in a layered honeycomb-type structure and so far is unique, as the low-temperature phase exhibits the higher symmetry. One motivation is to unravel the microscopic nature of spin-orbital excitations via a study of temperature and symmetry-induced changes. We document a number of highly unusual findings: A characteristic two-step hysteresis of the structural phase transition, accompanied by a dramatic change of the reflectivity. An electronic excitation, which appears in a narrow temperature range just across the structural phase transition, and a complex dielectric loss spectrum in the THz regime, which could indicate remnants of Kitaev physics. Despite significant symmetry changes across the monoclinic to rhombohedral phase transition, phonon eigenfrequencies and the majority of spin-orbital excitations are not strongly influenced. Obviously, the symmetry of the single molecular layers determine the eigenfrequencies of most of these excitations. Finally, from this combined terahertz, far- and mid-infrared study we try to shed some light on the so far unsolved low energy (< 1eV) electronic structure of the ruthenium $4d^5$ electrons in $α$-RuCl$_3$.

cond-mat.str-el↗

Jahn-Teller induced nematic orbital order in tetragonal Sr$_2$VO$_4$

Using high resolution X-Ray diffraction (XRD) on high purity powders, we resolved the structure and $ab$ symmetry of the intriguing compound \svo$ $ from room temperature down to 20 K to an unprecedented level of accuracy. Upon cooling, this new set of data unambiguously reveals a second order phase transition lowering the symmetry from tetragonal to orthorhombic at a temperature $T_{c2}=136$ K. The observation of an orthorhombic distortion of the $ab$-plane is attributed to nematic phase formation supported by local Jahn-Teller (JT) dynamical instability. At $T_{N}=105$ K, spins order and at $T_{c1}=100$ K the tetragonal structure is recovered with an elongated c-axis.

cond-mat.str-el↗

ESR evidence for partial melting of the orbital order in LaMnO$_3$ below the Jahn-Teller transition

We report on high-temperature electron spin resonance studies of a detwinned LaMnO$_3$ single crystal across the Jahn-Teller transition at $T_{\rm JT}$ = 750 K. The anisotropy of the linewidth and g-factor reflects the local Jahn-Teller distortions in the orbitally ordered phase. A clear jump in the linewidth accompanies the Jahn-Teller transition at $T_{\rm JT}$ = 750 K confirming that the transition is of first order. Already at $T^*$ = 550 K a significant decrease of the reduced linewidth is observed. This temperature scale is discussed with respect to the interaction of the $e_g$-electrons of the Mn$^{3+}$-ions and the elastic field of the cooperative distortions. Our results support a partial melting of the orbital order along the antiferromagnetically coupled $b$-axis at $T^*$. The remaining two-dimensional orbital ordering within the ferromagnetically coupled $ac$-plane finally disappears together with the cooperative distortion at $T_{\rm JT}$. Moreover in our discussion we show that elastic strain field interactions can explain the melting of the orbital order and, thus, has to be taken into account to explain the orbital ordering in LaMnO$_3$.

cond-mat.str-el↗

Spin correlations and Dzyaloshinskii-Moriya interaction in Cs$_2$CuCl$_4$

We report on electron spin resonance (ESR) studies of the spin relaxation in Cs$_2$CuCl$_4$. The main source of the ESR linewidth at temperatures $T \leq 150$ K is attributed to the uniform Dzyaloshinskii-Moriya interaction. The vector components of the Dzyaloshinskii-Moriya interaction are determined from the angular dependence of the ESR spectra using a high-temperature approximation. Both the angular and temperature dependence of the ESR linewidth have been analyzed using a self-consistent quantum-mechanical approach. In addition analytical expressions based on a quasi-classical picture for spin fluctuations are derived, which show good agreement with the quantum-approach for temperatures $T \geq 2J/k_{\rm B} \approx 15$ K. A small modulation of the ESR linewidth observed in the $ac$-plane is attributed to the anisotropic Zeeman interaction, which reflects the two magnetically nonequivalent Cu positions.

cond-mat.str-el↗

Electron spin resonance and exchange paths in the orthorhombic dimer system Sr2VO4

We report on magnetization and electron spin resonance (ESR) measurements of Sr$_{2}$VO$_4$ with orthorhombic symmetry. In this dimer system the $V^{4+}$ ions are in tetrahedral environment and are coupled by an antiferromagnetic intra-dimer exchange constant $J/k_B \approx$ 100 K to form a singlet ground state without any phase transitions between room temperature and 2 K. Based on an extended-Hückel-Tight-Binding analysis we identify the strongest exchange interaction to occur between two inequivalent vanadium sites via two intermediate oxygen ions. The ESR absorption spectra can be well described by a single Lorentzian line with an effective g-factor $g$ = 1.89. The temperature dependence of the ESR intensity is well described by a dimer model in agreement with the magnetization data. The temperature dependence of the ESR linewidth can be modeled by a superposition of a linear increase with temperature with a slope $α$ = 1.35 Oe/K and a thermally activated behavior with an activation energy $Δ/k_B$ = 1418 K, both of which point to spin-phonon coupling as the dominant relaxation mechanism in this compound.

cond-mat.str-el↗

Dual Features of Magnetic Susceptibility in Superconducting Cuprates: a comparison to inelastic neutron scattering

Starting from the generalized t-J-G model Hamiltonian, we analyze the spin response in the superconducting cuprates taking into account both local and itinerant spin components which are coupled to each other self-consistently. Derived expression reproduces the basic observations of neutron scattering data in YBa2Cu3O6+y compounds near the optimal doping level.

cond-mat.supr-con↗

Alternating spin-orbital order in tetragonal Sr2VO4

Considering spin-orbit coupling, the tetragonal crystal-field, and all relevant superexchange processes including quantum interference, we derive expressions for the energy levels of the vanadium ions in tetragonal Sr2VO4. The used parameters of the model Hamiltonian allow to describe well the excitation spectra observed in neutron scattering and optical experiments at low temperatures. The free energy exhibits a minimum which corresponds to a novel alternating spin-orbital order with strong thermal fluctuation of the orbital mixing parameter.

cond-mat.str-el↗

Optical study of phonons and electronic excitations in tetragonal Sr$_2$VO$_4$

We report on the optical excitation spectra in Sr$_2$VO$_4$. The phonon modes are assigned and their evolution with temperature is discussed in the frame of the different phase transitions crossed upon cooling. Besides the expected infrared-active phonons we observe two additional excitations at about 290 cm$^{-1}$ and 840 cm$^{-1}$ which could correspond to electronic transitions of the V$^{4+}$ ions. Our experimental results are discussed in the context of recent experimental and theoretical studies of this material with a unique spin-orbital ground state.

cond-mat.str-el↗

Light-matter interaction in antiferromagnets: the exchange-induced magnetic dipole mechanism

We propose a novel mechanism for exchange-induced exciton-magnon absorptions via hopping between two antiferromagnetically coupled sites and a simultaneous magnetic dipole transition to an excited orbital state. The obtained selection rules correspond to ones for magnetic dipole transitions and are in agreement with the exciton-magnon transitions observed in the quasi one-dimensional Heisenberg antiferromagnet KCuF3. The calculated magnon density of states in combination with a structure dependent factor identifies the observed optical magnon sideband to originate from transverse magnon modes.

cond-mat.str-el↗

London penetration depth in the tight binding approximation: Orthorhombic distortion and oxygen isotope effects in cuprates

We present a simple derivation of an expression for the superfluid density $ n_s \propto 1/λ^2 $ in superconductors with the tight binding energy dispersion. The derived expression is discussed in detail because of its distinction from the known expressions for ordinary superconductors with parabolic energy dispersion. We apply this expression for the experimental data analysis of the isotope effect in London penetration depth parameter $ λ$ in the BiSrCuO and YBaCuO family compounds near optimal doping, taking into account the orthorhombic distortion of crystal structure, and estimate the isotopic change of hopping parameters from the experimental data. We point out that $1/λ^2$ temperature behaviour is very sensitive to the ratio $ 2Δ_m(T=0)/ k_B T_c $ and estimate this quantity for a number of compounds.

cond-mat.supr-con↗

Towards the Theory of Isotope Effect of the London Penetration Depth in Cuprates

The expressions for the superfluid density have been discussed in both weak and strong coupling approaches. The numerical calculations of temperature and isotope composition dependencies have been performed for a number of High-Tc compounds. The tight-binding parameters and corresponding Fermi surfaces are taken in accord to the available photoemission data.

cond-mat.supr-con↗

Optical Spectroscopy in CoO: Phonons, Electric, and Magnetic Excitations

The reflectivity of single-crystalline CoO has been studied by optical spectroscopy for wave numbers ranging from 100 to 28,000\wn and for temperatures 8 $< T <$ 325 K\@. A splitting of the cubic IR-active phonon mode on passing the antiferromagnetic phase transition at $T_N$ = 289 K has been observed. At low temperatures the splitting amounts to 15.0\wn. In addition, we studied the splitting of the cubic crystal field ground state of the Co$^{2+}$ ions due to spin-orbit coupling, a tetragonal crystal field, and exchange interaction. Below $T_N$, magnetic dipole transitions between the exchange-split levels are identified and the energy-level scheme can be well described with a spin-orbit coupling $λ= 151.1\wn$, an exchange constant $J = 17.5\wn$, and a tetragonal crystal-field parameter $D = -47.8\wn$. Already in the paramagnetic state electric quadrupole transitions between the spin-orbit split level have been observed. At high frequencies, two electronic levels of the crystal-field-split $d$-manifold were identified at 8,000 and 18,500\wn.

cond-mat.str-el↗

Optical evidence for symmetry changes above the Neel temperature in KCuF3

We report on optical measurements of the 1D Heisenberg antiferromagnet KCuF3. The crystal-field excitations of the Cu2+ ions have been observed and their temperature dependence can be understood in terms of magnetic and exchange-induced dipole mechanisms and vibronic interactions. Above T_N we observe a new temperature scale T_S characterized by the emergence of narrow absorption features that correlate with changes of the orbital ordering as observed by Paolasini et al. [Phys. Rev. Lett. 88, 106403 (2002)]. The appearance of these optical transitions provides evidence for a symmetry change above the Neel temperature that affects the orbital ordering and paves the way for the antiferromagnetic ordering.

cond-mat.str-el↗

Dynamical Dzyaloshinsky-Moriya Interaction in KCuF3

The spin dynamics of the prototypical quasi one-dimensional antiferromagnetic Heisenberg spin S=1/2 chain KCuF3 is investigated by electron spin resonance spectroscopy. Our analysis shows that the peculiarities of the spin dynamics require a new dynamical form of the antisymmetric anisotropic spin-spin interaction. This dynamical Dzyaloshinsky-Moriya interaction is related to strong oscillations of the bridging fuorine ions perpendicular to the crystallographic c axis. This new mechanism allows to resolve consistently the controversies in observation of the magnetic and structural properties of this orbitally ordered perovskite compound.

cond-mat.str-el↗