arXiv subjects

D. Szaller

Publications and source records attributed to D. Szaller.

17 recordsLinked to original sources

arXiv2023

Giant natural optical rotation from chiral electromagnons in a collinear antiferromagnet

In NiTe$_3$O$_6$ with a chiral crystal structure, we report on a giant natural optical rotation of the lowest-energy magnon. This polarization rotation, as large as 140 deg/mm, corresponds to a path difference between right and left circular polarizations that is comparable to the sample thickness. Natural optical rotation, being a measure of structural chirality, is highly unusual for long-wavelength magnons. The collinear antiferromagnetic order of NiTe$_3$O$_6$ makes this giant effect even more peculiar: Chirality of the crystal structure does not affect the magnetic ground state but is strongly manifested in the lowest excited state. We show that the dynamic magnetoelectric effect, turning this magnon to a magnetic- and electric-dipole active hybrid mode, generates the giant natural optical rotation. In finite magnetic fields, it also leads to a strong optical magnetochiral effect.

cond-mat.str-el↗

arXiv2022

Refining magnetic interactions from the magnetic field dependence of spin-wave excitations in magnetoelectric LiFePO$_4$

We investigated the spin excitations of magnetoelectric $\text{LiFePO}_4$ by THz absorption spectroscopy in magnetic fields up to 33$\,$T. By studying their selection rules, we found not only magnetic-dipole, but also electric-dipole active (electromagnons) and magnetoelectric resonances. The magnetic field dependence of four strong low-energy modes is reproduced well by our four-sublattice spin model for fields applied along the three orthorhombic axes. From the fit, we refined the exchange couplings, single-ion anisotropies, and the Dzyaloshinskii-Moriya interaction parameters. Additional spin excitations not described by the mean-field model are observed at higher frequencies. Some of them shows a strong shift with magnetic field, up to 4$\,\text{cm}^{-1}/\text{T}$, when the field is applied along the easy axis. Based on this field dependence, we attribute these high frequency resonances to excitation of higher spin multipoles and of two magnons, which become THz-active due to the low symmetry of the magnetically ordered state.

cond-mat.str-el↗

arXiv2022

Coexistence of antiferromagnetism and ferrimagnetism in adjacent honeycomb layers

Antiferromagnetic and ferro/ferrimagnetic orders are typically exclusive in nature, thus, their co-existence in atomic-scale proximity is expected only in heterostructures. Breaking this paradigm and broadening the range of unconventional magnetic states, we report here on an atomic-scale hybrid spin state, which is stabilized in three-dimensional crystals of the polar antiferromagnet Co$_2$Mo$_3$O$_8$ by magnetic fields applied perpendicular to the \emph{Co} honeycomb layers and possesses a spontaneous in-plane ferromagnetic moment. Our microscopic spin model, capturing the observed field dependence of the longitudinal and transverse magnetization as well as the magnetoelectric/elastic properties, reveals that this novel spin state is composed of an alternating stacking of antiferromagnetic and ferrimagnetic honeycomb layers. The strong intra-layer and the weak inter-layer exchange couplings together with competing anisotropies at octahedral and tetrahedral \emph{Co} sites are identified as the key ingredients to stabilize antiferromagnetic and ferrimagnetic layers in such a close proximity. We show that the proper balance of magnetic interactions can extend the stability range of this hybrid phase down to zero magnetic field. The possibility to realize a layer-by-layer stacking of such distinct spin orders via suitable combinations of microscopic interactions opens a new dimension towards the nanoscale engineering of magnetic states.

cond-mat.str-el↗

arXiv2021

Confirming the trilinear form of the optical magnetoelectric effect in the polar honeycomb antiferromagnet Co$_{2}$Mo$_3$O$_8$

Magnetoelectric phenomena are intimately linked to relativistic effects and also require the material to break spatial inversion symmetry and time reversal invariance. Magnetoelectric coupling can substantially affect light-matter interaction and lead to non-reciprocal light propagation. Here, we confirm on a fully experimental basis, without invoking either symmetry-based or material-specific assumptions, that the optical magnetoelectric effect in materials with non-parallel magnetization ($\boldsymbol{M}$) and electric polarization ($\boldsymbol{P}$) generates a trilinear term in the refractive index, $δn\propto\boldsymbol{k}\cdot(\boldsymbol{P}\times\boldsymbol{M})$, where $\boldsymbol{k}$ is the propagation vector of light. Its sharp magnetoelectric resonances, that are simultaneously electric and magnetic dipole active excitations, make Co$_{2}$Mo$_3$O$_8$ an ideal compound to demonstrate this fundamental relation via independent variation of $\boldsymbol{M}$, $\boldsymbol{P}$ and $\boldsymbol{k}$. Remarkably, the material shows almost perfect one-way transparency in moderate magnetic fields at some of the magnetoelectric resonances.

cond-mat.str-el↗

arXiv2021

Selection rules and dynamic magnetoelectric effect of the spin waves in multiferroic BiFeO$_3$

We report the magnetic field dependence of the THz absorption and non-reciprocal directional dichroism spectra of BiFeO$_3$ measured on the three principal crystal cuts for fields applied along the three principal directions of each cut. From the systematic study of the light polarization dependence we deduced the optical selection rules of the spin-wave excitations. Our THz data, combined with small-angle neutron scattering results showed that i) an in-plane magnetic field rotates the $\mathbf{q}$ vectors of the cycloids perpendicular to the magnetic field, and ii) the selection rules are mostly determined by the orientation of the $\mathbf{q}$ vector with respect to the electromagnetic fields. We observed a magnetic field history dependent change in the strength and the frequency of the spin-wave modes, which we attributed to the change of the orientation and the length of the cycloidal $\mathbf{q}$ vector, respectively. Finally, we compared our experimental data with the results of linear spin-wave theory that reproduces the magnetic field dependence of the spin-wave frequencies and most of the selection rules, from which we identified the spin-polarization coupling terms relevant for the optical magnetoelectric effect.

cond-mat.str-el↗

arXiv2020

Magnetic equivalent of electric superradiance: radiative damping in yttrium-iron-garnet films

A dense system of independent oscillators, connected only by their interaction with the same cavity excitation mode, will radiate coherently, which effect is termed superradiance. In several cases, especially if the density of oscillators is high, the superradiance may dominate the intrinsic relaxation processes. This limit can be achieved, e.g., with cyclotron resonance in two-dimensional electron gases. In those experiments, the cyclotron resonance is coupled to the electric field of light, while the oscillator density can be easily controlled by varying the gate voltage. However, in the case of magnetic oscillators, to achieve the dominance of superradiance is more tricky, as material parameters limit the oscillator density, and the magnetic coupling to the light wave is rather small. Here we present quasi-optical magnetic resonance experiments on thin films of yttrium iron garnet. Due to the simplicity of experimental geometry, the intrinsic damping and the superradiance can be easily separated in the transmission spectra. We show that with increasing film thickness, the losses due to coherent radiation prevail the system's internal broadening.

cond-mat.mtrl-sci↗

arXiv2020

Magnetic anisotropy and exchange paths for octa- and tetrahedrally coordinated Mn$^{2+}$ ions in the honeycomb multiferroic Mn$_2$Mo$_3$O$_8$

We investigated the static and dynamic magnetic properties of the polar ferrimagnet Mn$_2$Mo$_3$O$_8$ in three magnetically ordered phases via magnetization, magnetic torque, and THz absorption spectroscopy measurements. The observed magnetic field dependence of the spin-wave resonances, including Brillouin zone-center and zone-boundary excitations, magnetization, and torque, are well described by an extended two-sublattice antiferromagnetic classical mean-field model. In this orbitally quenched system, the competing weak easy-plane and easy-axis single-ion anisotropies of the two crystallographic sites are determined from the model and assigned to the tetra- and octahedral sites, respectively, by ab initio calculations.

cond-mat.str-el↗

arXiv2020

Unusual magnetoelectric effect in paramagnetic rare-earth langasite

Violation of time reversal and spatial inversion symmetries has profound consequences for elementary particles and cosmology. Spontaneous breaking of these symmetries at phase transitions gives rise to unconventional physical phenomena in condensed matter systems, such as ferroelectricity induced by magnetic spirals, electromagnons, non-reciprocal propagation of light and spin waves, and the linear magnetoelectric (ME) effect - the electric polarization proportional to the applied magnetic field and the magnetization induced by the electric field. Here, we report the experimental study of the holmium-doped langasite, Ho$_{x}$La$_{3-x}$Ga$_5$SiO$_{14}$, showing a puzzling combination of linear and highly non-linear ME responses in the disordered paramagnetic state: its electric polarization grows linearly with the magnetic field but oscillates many times upon rotation of the magnetic field vector. We propose a simple phenomenological Hamiltonian describing this unusual behavior and derive it microscopically using the coupling of magnetic multipoles of the rare-earth ions to the electric field.

cond-mat.mtrl-sci↗

arXiv2019

Controlling of light with electromagnons

Magnetoelectric coupling in multiferroic materials opens new routes to control the propagation of light. The new effects arise due to dynamic magnetoelectric susceptibility that cross-couples the electric and magnetic fields of light and modifies the solutions of Maxwell equations in media. In this paper two major effects will be considered in detail: optical activity and asymmetric propagation. In case of optical activity the polarization plane of the input radiation rotates by an angle proportional to the magnetoelectric susceptibility. The asymmetric propagation is a counter-intuitive phenomenon and it represents different transmission coefficients for forward and backward directions. Both effects are especially strong close to resonance frequencies of electromagnons, i.e. excitations in multiferroic materials that reveal simultaneous electric and magnetic character.

cond-mat.mtrl-sci↗

arXiv2019

Sign change of polarization rotation under either time or space inversion in magnetoelectric YbAl3(BO3)4

Materials with optical activity can rotate the polarization plane of transmitted light. The most typical example is the natural optical activity, which has the symmetry property of changing sign after space inversion but being invariant to time inversion. Faraday rotation exhibits the opposite: it is invariant to space inversion but changes sign after time reversal. Here, we demonstrate that in a magnetoelectric material, another type of polarization rotation is possible. This effect is investigated in magnetoelectric YbAl3(BO3)4 under the viewpoint of time and space inversion symmetry arguments. We observe the sign change of the rotation sense under either time or space reversal. This investigation proves that the polarization rotation in YbAl3(BO3)4 must be classified as gyrotropic birefringence, which has been discussed within the idea of time-reversal breaking in underdoped cuprates. The diagonal terms in the magnetoelectric susceptibility are responsible for the observed signal of gyrotropic birefringence. Further analysis of the experimental spectra reveals a substantial contribution of the natural optical activity to the polarization rotation. We also demonstrate that the observed activity originates from the magnetoelectric susceptibility.

cond-mat.mtrl-sci↗

arXiv2018

Directional dichroism in the paramagnetic state of multiferroics: a case study of infrared light absorption in Sr2CoSi2O7 at high temperatures

The coexisting magnetic and ferroelectric orders in multiferroic materials give rise to a handful of novel magnetoelectric phenomena, such as the absorption difference for the opposite propagation directions of light called the non-reciprocal directional dichroism (NDD). Usually these effects are restricted to low temperature, where the multiferroic phase develops. In this paper we report the observation of NDD in the paramagnetic phase of Sr2CoSi2O7 up to temperatures more than ten times higher than its Néel temperature (7 K) and in fields up to 30 T. The magnetically induced polarization and NDD in the disordered paramagnetic phase is readily explained by the single-ion spin-dependent hybridization mechanism, which does not necessitate correlation effects between magnetic ions. The Sr2CoSi2O7 provides an ideal system for a theoretical case study, demonstrating the concept of magnetoelectric spin excitations in a paramagnet via analytical as well as numerical approaches. We applied exact diagonalization of a spin cluster to map out the temperature and field dependence of the spin excitations, as well as symmetry arguments of the single ion and lattice problem to get the spectrum and selection rules.

cond-mat.str-el↗

arXiv2017

Switching of magnons by electric and magnetic fields in multiferroic borates

Electric manipulation of magnetic properties is a key problem of materials research. To fulfil the requirements of modern electronics, these processes must be shifted to high frequencies. In multiferroic materials this may be achieved by electric and magnetic control of their fundamental excitations. Here we identify magnetic vibrations in multiferroic iron-borates which are simultaneously sensitive to external electric and magnetic fields. Nearly 100% modulation of the terahertz radiation in an external field is demonstrated for SmFe3(BO3)4. High sensitivity can be explained by a modification of the spin orientation which controls the excitation conditions in multiferroic borates. These experiments demonstrate the possibility to alter terahertz magnetic properties of materials independently by external electric and magnetic fields.

cond-mat.mtrl-sci↗

arXiv2017

Optical conductivity in multiferroic GaV$_4$S$_8$ and GeV$_4$S$_8$: Phonons and electronic transitions

We report on optical spectroscopy on the lacunar spinels GaV$_4$S$_8$ and GeV$_4$S$_8$ in the spectral range from 100 to 23000 cm$^{-1}$ and for temperatures from 5 to 300 K. These multiferroic spinel systems reveal Jahn-Teller driven ferroelectricity and complex magnetic order at low temperatures. We study the infrared-active phonon modes and the low-lying electronic excitations in the cubic high-temperature phase, as well as in the orbitally and in the magnetically ordered low-temperature phases. We compare the phonon modes in these two compounds, which undergo different symmetry-lowering Jahn-Teller transitions into ferroelectric and orbitally ordered phases, and exhibit different magnetic ground states. We follow the splitting of the phonon modes at the structural phase transition and detect additional splittings at the onset of antiferromagnetic order in GeV$_4$S$_8$. We observe electronic transitions within the $d$-derived bands of the V$_4$ clusters and document a significant influence of the structural and magnetic phase transitions on the narrow electronic band gaps.

cond-mat.str-el↗

arXiv2014

Evolution of the 2D antiferromagnetism with temperature and magnetic field in multiferroic Ba$_2$CoGe$_2$O$_7$

We report on spherical neutron polarimetry and unpolarized neutron diffraction in zero magnetic field as well as flipping ratio and static magnetization measurements in high magnetic fields on the multiferroic square lattice antiferromagnet Ba$_2$CoGe$_2$O$_7$. We found that in zero magnetic field the magnetic space group is $Cm'm2'$ with sublattice magnetization parallel to the [100] axis of this orthorhombic setting. The spin canting has been found to be smaller than $0.2^\circ$ in the ground state. This assignment is in agreement with the field-induced changes of the magnetic domain structure below 40 mT as resolved by spherical neutron polarimetry. The magnitude of the ordered moment has been precisely determined. Above the magnetic ordering temperature short-range magnetic fluctuations are observed. Based on the high-field magnetization data, we refined the parameters of the recently proposed microscopic spin model describing the multiferroic phase of Ba$_2$CoGe$_2$O$_7$.

cond-mat.str-el↗

arXiv2014

Simultaneously Magnetic- and Electric-dipole Active Spin Excitations Govern the Static Magnetoelectric Effect in Multiferroic Materials

We derive a sum rule to demonstrate that the static magnetoelectric (ME) effect is governed by optical transitions that are simultaneously excited via the electric and magnetic components of light. By a systematic analysis of magnetic point groups, we show that the ME sum rule is applicable to a broad variety of non-centrosymmetric magnets including ME multiferroic compounds. Due to the dynamical ME effect, the optical excitations in these materials can exhibit directional dichroism, i.e. the absorption coefficient can be different for counter-propagating light beams. According to the ME sum rule, the magnitude of the linear ME effect of a material is mainly determined by the directional dichroism of its low-energy optical excitations. Application of the sum rule to the multiferroic Ba$_2$CoGe$_2$O$_7$, Sr$_2$CoSi$_2$O$_7$ and Ca$_2$CoSi$_2$O$_7$ shows that in these compounds the static ME effect is mostly governed by the directional dichroism of the spin-wave excitations in the GHz-THz spectral range. On this basis, we argue that the studies of directional dichroism and the application of ME sum rule can promote the synthesis of new materials with large static ME effect.

cond-mat.mtrl-sci↗

arXiv2012

Malaria pigment crystals as magnetic micro-rotors: key for high-sensitivity diagnosis

The need to develop new methods for the high-sensitivity diagnosis of malaria has initiated a global activity in medical and interdisciplinary sciences. Most of the diverse variety of emerging techniques are based on research-grade instruments, sophisticated reagent-based assays or rely on expertise. Here, we suggest an alternative optical methodology with an easy-to-use and cost-effective instrumentation based on unique properties of malaria pigment reported previously and determined quantitatively in the present study. Malaria pigment, also called hemozoin, is an insoluble microcrystalline form of heme. These crystallites show remarkable magnetic and optical anisotropy distinctly from any other components of blood. As a consequence, they can simultaneously act as magnetically driven micro-rotors and spinning polarizers in suspensions. These properties can gain importance not only in malaria diagnosis and therapies, where hemozoin is considered as drug target or immune modulator, but also in the magnetic manipulation of cells and tissues on the microscopic scale.

physics.bio-ph↗

arXiv2012

Spin-stretching modes in anisotropic magnets: spin-wave excitations in the multiferroic Ba2CoGe2O7

We studied spin excitations of the multiferroic Ba2CoGe2O7 in high magnetic fields up to 33 T. In the electron spin resonance and far infrared absorption spectra we found several spin excitations beyond the two conventional magnon modes expected for such a two-sublattice antiferromagnet. We show that a multi-boson spin-wave theory can capture these unconventional modes, that include spin-stretching modes associated with an oscillating magnetic dipole (or only quadrupole) moment. The lack of the inversion symmetry allows these modes to become electric dipole active. We expect that the spin-stretching modes can be generally observed in inelastic neutron scattering and light absorption experiments in a broad class of ordered S > 1/2 spin systems with strong single-ion anisotropy and/or non-centrosymmetric lattice structure.

cond-mat.str-el↗