arXiv subjects

T. Rõõm

Publications and source records attributed to T. Rõõm.

At least 19 recordsLinked to original sources

arXiv2026

Chirality-resolved spectroscopy of Caroli-de Gennes-Matricon states in multiband FeTe$_{1-x}$Se$_{x}$ superconductors

We employ terahertz Faraday magneto-optical spectroscopy to probe the relaxation dynamics of quantized helical Caroli-de Gennes-Matricon (CdGM) states in epitaxial FeTe$_{1-x}$Se$_x$ thin films, nodeless multiband superconductors with short coherence lengths in the moderately clean limit. By exploiting polarization-selective optical transitions, we directly resolve the helicity and band origin of vortex-core quasiparticles. We observe long-lived CdGM resonances with opposite circular polarizations for electron- and hole-like bands. This enables independent, band-resolved determination of quasiparticle lifetimes, vortex masses, coherence lengths, and upper critical fields, and reveals their systematic evolution with isovalent substitution. The results establish terahertz magneto-optics as a direct probe of helical vortex-core excitations and provide dynamical evidence for multiband CdGM states in iron-based superconductors.

cond-mat.supr-con↗

arXiv2024

Modified Martin-Puplett interferometer for magneto-optical Kerr effect measurements at sub-THz frequencies

We present magneto-optical Kerr effect (MOKE) spectrometer based on a modified Martin-Puplett interferometer, utilizing continuous wave sub-THz low-power radiation in broad frequency range. This spectrometer is capable of measuring the frequency dependence of the MOKE response function, both the Kerr rotation and ellipticity, simultaneously with sub-milliradian accuracy without the need for reference measurement. The instrument's versatility allow it to be coupled to a cryostat with optical windows enabling studies of a variety of quantum materials such as unconventional superconductors, two-dimensional electron gas systems, quantum magnets, and other system showing optical Hall response, at sub-Kelvin temperatures and in high magnetic fields. We demonstrate the functionality of the MOKE spectrometer using an undoped InSb wafer as a test sample.

cond-mat.mtrl-sci↗

arXiv2024

Magnetic field-induced phases and spin Hamiltonian in Cs2CoBr4

Magnetic structures and spin excitations are studied across the phase diagram of the geometrically frustrated S = 3/2 quantum antiferromagnet Cs2CoBr4 in magnetic fields applied along the magnetic easy axis, using neutron diffraction, inelastic neutron scattering and THz absorption spectroscopy. The data are analyzed, where appropriate, using extended SU (4) linear spin wave theory. A minimal magnetic Hamiltonian is proposed based on measurements in the high field polarized state. It deviates considerably from the previously considered models. Additional dilatometry experiments highlight the importance of magnetoelastic coupling in this system.

cond-mat.str-el↗

arXiv2024

THz spin-wave excitations in the transverse conical phase of BiFeO$_3$

Although BiFeO$_3$ is one of the most studied multiferroic materials, recent magnetization and neutron scattering studies have revealed a new magnetic phase in this compound - the transverse conical phase. To study the collective spin excitations of this phase, we performed THz spectroscopy in magnetic fields up to 17 T at and above room temperature. We observed five spin-wave branches in the magnetic phase with long wavelength conical modulation. Using a numerical spin dynamics model we found two kinds of excitations with magnetic moments oscillating either along or perpendicular to the static fields. Remarkably, we detected strong directional dichroism, an optical manifestation of the magnetoelectric effect, for two spin-wave modes of the conical phase. According to our experiments, the stability of the conical state is sensitive to the magnetic field history and it can become (meta)stable at or close to zero magnetic field, which may allow exploiting its magnetoelectric properties at room temperature.

cond-mat.mtrl-sci↗

arXiv2023

Confinement of fractional excitations in a triangular lattice antiferromagnet

High-resolution neutron and THz spectroscopies are used to study the magnetic excitation spectrum of Cs$_2$CoBr$_4$, a distorted-triangular-lattice antiferromagnet with nearly XY-type anisotropy. What was previously thought of as a broad excitation continuum [Phys. Rev. Lett. 129, 087201 (2022)] is shown to be a series of dispersive bound states reminiscent of "Zeeman ladders" in quasi-one-dimensional Ising systems. At wave vectors where inter-chain interactions cancel at the Mean Field level, they can indeed be interpreted as bound finite-width kinks in individual chains. Elsewhere in the Brillouin zone their true two-dimensional structure and propagation are revealed.

cond-mat.str-el↗

arXiv2022

Spin excitations in the magnetically ordered phases of MnSc$_2$S$_4$

Recent neutron scattering experiments suggested that frustrated magnetic interactions give rise to antiferromagnetic spiral and fractional skyrmion lattice phases in MnSc$_2$S$_4$. Here, to trace the signatures of these modulated phases, we studied the spin excitations of MnSc$_2$S$_4$ by THz spectroscopy at 300 mK up to 12 T. We found a single magnetic resonance with linearly increasing frequency in field. The corresponding $g$-factor of Mn$^{2+}$ ions $g$ = 1.96, and the absence of other resonances imply very weak anisotropies and negligible contribution of higher harmonics to the spiral state. The significant difference between the dc magnetic susceptibility and the lowest-frequency ac susceptibility in our experiment implies the existence of mode(s) below 100 GHz.

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↗

arXiv2021

In-situ electric field control of THz non-reciprocal directional dichroism in the multiferroic Ba$_2$CoGe$_2$O$_7$

Non-reciprocal directional dichroism, also called the optical-diode effect, is an appealing functional property inherent to the large class of non-centrosymmetric magnets. However, the in-situ electric control of this phenomenon is challenging as it requires a set of conditions to be fulfilled: Special symmetries of the magnetic ground state, spin-excitations with comparable magnetic- and electric-dipole activity and switchable electric polarization. We demonstrate the isothermal electric switch between domains of Ba$_2$CoGe$_2$O$_7$ possessing opposite magnetoelectric susceptibilities. Combining THz spectroscopy and multiboson spin-wave analysis, we show that unbalancing the population of antiferromagnetic domains generates the non-reciprocal light absorption of spin excitations.

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 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↗

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

Magnetic Excitations and Continuum of a Field-Induced Quantum Spin Liquid in $α$-RuCl$_3$

We report on terahertz spectroscopy of quantum spin dynamics in $α$-RuCl$_3$, a system proximate to the Kitaev honeycomb model, as a function of temperature and magnetic field. An extended magnetic continuum develops below the structural phase transition at $T_{s2}=62$K. With the onset of a long-range magnetic order at $T_N=6.5$K, spectral weight is transferred to a well-defined magnetic excitation at $\hbar ω_1 = 2.48$meV, which is accompanied by a higher-energy band at $\hbar ω_2 = 6.48$meV. Both excitations soften in magnetic field, signaling a quantum phase transition at $B_c=7$T where we find a broad continuum dominating the dynamical response. Above $B_c$, the long-range order is suppressed, and on top of the continuum, various emergent magnetic excitations evolve. These excitations follow clear selection rules and exhibit distinct field dependencies, characterizing the dynamical properties of the field-induced quantum spin liquid.

cond-mat.str-el↗

arXiv2017

Competing Exchange Interactions in the Multiferroic and Ferrimagnetic CaBaCo$_4$O$_7$

Competing exchange interactions can produce complex magnetic states together with spin-induced electric polarizations. With competing interactions on alternating triangular and kagome layers, the swedenborgite CBO may have one of the largest measured spin-induced polarizations of about 1700 nC/cm$^2$ below its ferrimagnetic transition temperature at 70 K. Powder neutron-diffraction data, magnetization measurements, and spin-wave resonance frequencies in the THz range reveal that the complex spin order of multiferroic CBO can be described as a triangular array of c-axis chains ferrimagnetically coupled to each other in the ab plane. Magnetostriction on bonds that couple those chains produces the large spin-induced polarization of CBO.

cond-mat.mtrl-sci↗

arXiv2016

Unidirectional terahertz light absorption in the pyroelectric ferrimagnet CaBaCo4O7

Spin excitations were studied by absorption spectroscopy in CaBaCo4O7 which is a type-I multiferroic compound with the largest magnetic-order induced ferroelectric polarization (ΔP=17mC/m2) reported, so far. We observed two optical magnon branches: a solely electric dipole allowed one and a mixed magnetoelectric resonance. The entangled magnetization and polarization dynamics of the magnetoelectric resonance gives rise to unidirectional light absorption, i.e. that magnon mode absorbs the electromagnetic radiation for one propagation direction but not for the opposite direction. Our systematic study of the magnetic field and temperature dependence of magnon modes provides information about the energies and symmetries of spin excitations, which is required to develop a microscopic spin model of CaBaCo4O7.

cond-mat.str-el↗

arXiv2013

Terahertz spectroscopy of spin waves in multiferroic BiFeO$_3$ in high magnetic fields

We have studied the magnetic field dependence of far-infrared active magnetic modes in a single ferroelectric domain \BFO/ crystal at low temperature. The modes soften close to the critical field of 18.8\,T along the [001] (pseudocubic) axis, where the cycloidal structure changes to the homogeneous canted antiferromagnetic state and a new strong mode with linear field dependence appears that persists at least up to 31\,T. A microscopic model that includes two \DM/ interactions and easy-axis anisotropy describes closely both the zero-field spectroscopic modes as well as their splitting and evolution in a magnetic field. The good agreement of theory with experiment suggests that the proposed model provides the foundation for future technological applications of this multiferroic material.

cond-mat.str-el↗

arXiv2013

Infrared spectroscopy of small-molecule endofullerenes

Hydrogen is one of the few molecules which has been incarcerated in the molecular cage of C$_{60}$ and forms endohedral supramolecular complex H$_2$@C$_{60}$. In this confinement hydrogen acquires new properties. Its translational motion becomes quantized and is correlated with its rotations. We applied infrared spectroscopy to study the dynamics of hydrogen isotopologs H$_2$, D$_2$ and HD incarcerated in C$_{60}$. The translational and rotational modes appear as side bands to the hydrogen vibrational mode in the mid infrared part of the absorption spectrum. Because of the large mass difference of hydrogen and C$_{60}$ and the high symmetry of C$_{60}$ the problem is identical to a problem of a vibrating rotor moving in a three-dimensional spherical potential. The translational motion within the C$_{60}$ cavity breaks the inversion symmetry and induces optical activity of H$_2$. We derive potential, rotational, vibrational and dipole moment parameters from the analysis of the infrared absorption spectra. Our results were used to derive the parameters of a pairwise additive five-dimensional potential energy surface for H$_2$@C$_{60}$. The same parameters were used to predict H$_2$ energies inside C$_{70}$[Xu et al., J. Chem. Phys., {\bf 130}, 224306 (2009)]. We compare the predicted energies and the low temperature infrared absorption spectra of H$_2$@C$_{70}$.

physics.chem-ph↗

arXiv2012

Optical spectroscopy shows that the normal state of URu$_2$Si$_2$ is an anomalous Fermi liquid

Fermi showed that electrons, as a result of their quantum nature, form a gas of particles where the temperature and density follow the so called Fermi distribution. In a metal, as shown by Landau, that despite their strong Coulomb interaction with each other and the positive background ions, the electrons continue to act like free quantum mechanical particles but with enhanced masses. This state of matter, the Landau-Fermi liquid, is recognized experimentally by an electrical resistivity that is proportional to the square of the absolute temperature plus a term proportional to the square of the frequency of the applied field. Calculations show that, if electron-electron scattering dominates the resistivity in a Landau Fermi liquid, the ratio of the two terms, $b$ has the universal value of {\em b} = 4. We find that in the normal state of the heavy Fermion metal URu$_2$Si$_2$, instead of the Fermi liquid value of 4 the coefficient $b$ =1 $\pm$ 0.1. This unexpected result implies that the electrons in this material are experiencing a unique scattering process. This scattering is intrinsic and we suggest that, the uranium $f$ electrons do not hybridize to form a coherent Fermi liquid but instead act like a dense array of elastic impurities, interacting incoherently with the charge carriers. This behavior is not restricted to URu$_2$Si$_2$. Fermi liquid like states with $b \neq$ 4 have been observed in a number of disparate systems but the significance of this result has not been recognized.

cond-mat.str-el↗

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↗