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 [L. Facheris et al., Phys. Rev. Lett. 129, 087201 (2022)PRLTAO0031-900710.1103/PhysRevLett.129.087201] is shown to be a series of dispersive bound states reminiscent of "Zeeman ladders" in quasi-one-dimensional Ising systems. At wave vectors where interchain 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.

In Situ Electric-Field Control of THz Nonreciprocal Directional Dichroism in the Multiferroic Ba_{2}CoGe_{2}O_{7}.

Nonreciprocal directional dichroism, also called the optical-diode effect, is an appealing functional property inherent to the large class of noncentrosymmetric 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 nonreciprocal light absorption of spin excitations.

Infrared spectroscopy of an endohedral water in fullerene.

An infrared absorption spectroscopy study of the endohedral water molecule in a solid mixture of H2O@C60 and C60 was carried out at liquid helium temperature. From the evolution of the spectra during the ortho-para conversion process, the spectral lines were identified as para-H2O and ortho-H2O transitions. Eight vibrational transitions with rotational side peaks were observed in the mid-infrared: ω1, ω2, ω3, 2ω1, 2ω2, ω1 + ω3, ω2 + ω3, and 2ω2 + ω3. The vibrational frequencies ω2 and 2ω2 are lower by 1.6% and the rest by 2.4%, as compared to those of free H2O. A model consisting of a rovibrational Hamiltonian with the dipole and quadrupole moments of H2O interacting with the crystal field was used to fit the infrared absorption spectra. The electric quadrupole interaction with the crystal field lifts the degeneracy of the rotational levels. The finite amplitudes of the pure v1 and v2 vibrational transitions are consistent with the interaction of the water molecule dipole moment with a lattice-induced electric field. The permanent dipole moment of encapsulated H2O is found to be 0.50 ± 0.05 D as determined from the far-infrared rotational line intensities. The translational mode of the quantized center-of-mass motion of H2O in the molecular cage of C60 was observed at 110 cm-1 (13.6 meV).

Magnetic Excitations and Continuum of a Possibly 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. We follow the evolution of an extended magnetic continuum 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 ℏω_{1}=2.48 meV, which is accompanied by a higher-energy band at ℏω_{2}=6.48 meV. Both excitations soften in a magnetic field, signaling a quantum phase transition close to B_{c}=7 T, where a broad continuum dominates the dynamical response. Above B_{c}, the long-range order is suppressed, and on top of the continuum, emergent magnetic excitations evolve. These excitations follow clear selection rules and exhibit distinct field dependencies, characterizing the dynamical properties of a possibly field-induced quantum spin liquid.

Optical Diode Effect at Spin-Wave Excitations of the Room-Temperature Multiferroic BiFeO_{3}.

Multiferroics permit the magnetic control of the electric polarization and the electric control of the magnetization. These static magnetoelectric (ME) effects are of enormous interest: The ability to read and write a magnetic state current-free by an electric voltage would provide a huge technological advantage. Dynamic or optical ME effects are equally interesting, because they give rise to unidirectional light propagation as recently observed in low-temperature multiferroics. This phenomenon, if realized at room temperature, would allow the development of optical diodes which transmit unpolarized light in one, but not in the opposite, direction. Here, we report strong unidirectional transmission in the room-temperature multiferroic BiFeO_{3} over the gigahertz-terahertz frequency range. The supporting theory attributes the observed unidirectional transmission to the spin-current-driven dynamic ME effect. These findings are an important step toward the realization of optical diodes, supplemented by the ability to switch the transmission direction with a magnetic or electric field.

One-way transparency of four-coloured spin-wave excitations in multiferroic materials.

The coupling between spins and electric dipoles governs magnetoelectric phenomena in multiferroics. The dynamical magnetoelectric effect, which is an inherent attribute of the spin excitations in multiferroics, drastically changes the optical properties of these compounds compared with conventional materials where light-matter interaction is expressed only by the dielectric permittivity or magnetic permeability. Here we show via polarized terahertz spectroscopy studies on multiferroic Ca2CoSi2O7, Sr2CoSi2O7 and Ba2CoGe2O7 that such magnetoeletric spin excitations exhibit quadrochroism, that is, they have different colours for all the four combinations of the two propagation directions (forward or backward) and the two orthogonal polarizations of a light beam. We demonstrate that one-way transparency can be realized for spin-wave excitations with sufficiently strong optical magnetoelectric effect. Furthermore, the transparent and absorbing directions of light propagation can be reversed by external magnetic fields. This magnetically controlled optical-diode function of magnetoelectric multiferroics may open a new horizon in photonics.

Infrared spectroscopy of small-molecule endofullerenes.

Hydrogen is one of the few molecules that has been incarcerated in the molecular cage of C60 to form the endohedral supramolecular complex H2@C60. In this confinement, hydrogen acquires new properties. Its translation motion, within the C60 cavity, becomes quantized, is correlated with its rotation and breaks inversion symmetry that induces infrared (IR) activity of H2. We apply IR spectroscopy to study the dynamics of hydrogen isotopologues H2, D2 and HD incarcerated in C60. The translation and rotation modes appear as side bands to the hydrogen vibration mode in the mid-IR part of the absorption spectrum. Because of the large mass difference of hydrogen and C60 and the high symmetry of C60 the problem is almost identical to a vibrating rotor moving in a three-dimensional spherical potential. We derive potential, rotation, vibration and dipole moment parameters from the analysis of the IR absorption spectra. Our results were used to derive the parameters of a pairwise additive five-dimensional potential energy surface for H2@C60. The same parameters were used to predict H2 energies inside C70. We compare the predicted energies and the low-temperature IR absorption spectra of H2@C70.

Terahertz spectroscopy of spin waves in multiferroic BiFeO3 in high magnetic fields.

We have studied the magnetic field dependence of far-infrared active magnetic modes in a single ferroelectric domain BiFeO3 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 Dzyaloshinskii-Moriya 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.

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

We studied spin excitations in the magnetically ordered phase of the noncentrosymmetric Ba(2)CoGe(2)O(7) 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 multiboson spin-wave theory describes these unconventional modes, including spin-stretching modes, characterized by an oscillating magnetic dipole and quadrupole moment. The lack of inversion symmetry allows each mode 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 noncentrosymmetric lattice structure.

Infrared spectroscopy of endohedral HD and D2 in C60.

We report on the dynamics of two hydrogen isotopomers, D(2) and HD, trapped in the molecular cages of a fullerene C(60) molecule. We measured the infrared spectra and analyzed them using a spherical potential for a vibrating rotor. The potential, vibration-rotation Hamiltonian, and dipole moment parameters are compared with previously studied H(2)@C(60) parameters [M. Ge, U. Nagel, D. Hüvonen, T. Rõõm, S. Mamone, M. H. Levitt, M. Carravetta, Y. Murata, K. Komatsu, J. Y.-C. Chen, and N. J. Turro, J. Chem. Phys. 134, 054507 (2011)]. The isotropic part of the potential is similar for all three isotopomers. In HD@C(60), we observe mixing of the rotational states and an interference effect of the dipole moment terms due to the displacement of the HD rotation center from the fullerene cage center.

Interaction potential and infrared absorption of endohedral H2 in C60.

We have measured the temperature dependence of the infrared spectra of a hydrogen molecule trapped inside a C(60) cage, H(2)@C(60), in the temperature range from 6 to 300 K and analyzed the excitation spectrum by using a five-dimensional model of a vibrating rotor in a spherical potential. The electric dipole moment is induced by the translational motion of endohedral H(2) and gives rise to an infrared absorption process where one translational quantum is created or annihilated, ΔN = ±1. Some fundamental transitions, ΔN = 0, are observed as well. The rotation of endohedral H(2) is unhindered but coupled to the translational motion. The isotropic and translation-rotation coupling part of the potential are anharmonic and different in the ground and excited vibrational states of H(2). The vibrational frequency and the rotational constant of endohedral H(2) are smaller than those of H(2) in the gas phase. The assignment of lines to ortho- and para-H(2) is confirmed by measuring spectra of a para enriched sample of H(2)@C(60) and is consistent with the earlier interpretation of the low temperature infrared spectra [Mamone et al., J. Chem. Phys. 130, 081103 (2009)].

Optical spectroscopy of superconducting Ba0.55K0.45Fe2As2: evidence for strong coupling to low-energy bosons.

Normal state optical spectroscopy on single crystals of the new iron arsenide superconductor Ba0.55K0.45Fe2As2 shows that the infrared spectrum consists of two major components: a strong metallic Drude band and a well-separated midinfrared absorption centered at 0.7 eV. It is difficult to separate the two components unambiguously but several fits using Lorentzian peaks suggest a model with a Drude peak having a plasma frequency of 1.6 to 2.1 eV and a midinfrared peak with a plasma frequency of 2.5 eV. Detailed analysis of the frequency dependent scattering rate shows that the charge carriers interact with a broad bosonic spectrum extending beyond 100 meV with a very large coupling constant lambda=3.4 at low temperature. As the temperature increases this coupling weakens to lambda=0.78 at ambient temperature. This suggests a bosonic spectrum that is similar to what is seen in the lower Tc cuprates.

Rotor in a cage: Infrared spectroscopy of an endohedral hydrogen-fullerene complex.

We report the observation of quantized translational and rotational motion of molecular hydrogen inside the cages of C(60). Narrow infrared absorption lines at the temperature of 6 K correspond to vibrational excitations in combination with translational and rotational excitations and show well-resolved splittings due to the coupling between translational and rotational modes of the endohedral H(2) molecule. A theoretical model shows that H(2) inside C(60) is a three-dimensional quantum rotor moving in a nearly spherical potential. The theory provides both the frequencies and the intensities of the observed infrared transitions. Good agreement with the experimental results is obtained by fitting a small number of empirical parameters to describe the confining potential, as well as the relative concentration of ortho- and para-H(2).

Suppression of the charge-density-wave state in Sr14Cu24O41 by calcium doping.

The charge response in the spin chain and/or ladder compound Sr14-xCaxCu24O41 is characterized by dc resistivity, low-frequency dielectric spectroscopy and optical spectroscopy. We identify a phase transition below which a charge-density wave (CDW) develops in the ladder arrays. Calcium doping suppresses this phase with the transition temperature decreasing from 210 K for x=0 to 10 K for x=9, and the CDW gap from 130 meV down to 3 meV, respectively. This suppression is due to the worsened nesting originating from the increase of the interladder tight-binding hopping integrals, as well as from disorder introduced at the Sr sites. These results altogether speak in favor of two-dimensional superconductivity under pressure.

Temperature and frequency effects in tooth enamel electron spin resonance dosimetry.

Electron spin resonance of CO3(3-) molecule ions in human tooth enamel have been studied at various temperatures between 4 and 350 K and at various microwave powers in the 9 GHz (X) band. Signal saturation during cooling due to slowing down of the electron spin relaxation has been established. The 35 GHz (Q) band spectra of tooth enamel, irradiated with various gamma-ray doses, are also presented. Q band ESR dosimetry offers some advantages over the X-band dosimetry due to signal enhancement from the spin level population difference and especially due to a better filling factor which is important when only minute quantities (a few mg) of enamel are available.