Observation of Multiple-Gap Structure in Hidden Order State of URu2Si2 from Optical Conductivity

We have measured the far infrared reflectance of the heavy fermion compound URu$_2$Si$_2$ through the phase transition at T$_{HO}$=17.5 K dubbed 'hidden order' with light polarized along both the a- and c-axes of the tetragonal structure. The optical conductivity allows the formation of the hidden order gap to be investigated in detail. We find that both the conductivity and the gap structure are anisotropic, and that the c-axis conductivity shows evidence for a double gap structure, with $\Delta_{1,c}=2.7$ meV and $\Delta_{2,c}=1.8$ meV respectively at 4 K, while the gap seen in the a-axis conductivity has a value of $\Delta_a=3.2$ meV at 4 K. The opening of the gaps does not follow the behaviour expected from mean field theory in the vicinity of the transition.Comment: 6 pages, 5 figure

Magnetoelectric memory function with optical readout

The ultimate goal of multiferroic research is the development of new-generation non-volatile memory devices, the so-called magnetoelectric (ME) memories, where magnetic bits are controlled via electric fields without the application of electrical currents subject to dissipation. This low-power operation exploits the entanglement of the magnetization and the electric polarization coexisting in multiferroic materials. Here we demonstrate the optical readout of ME memory states in the antiferromagnetic (AFM) and antiferroelectric (AFE) LiCoPO$_4$, based on the strong absorption difference of THz radiation between its two types of ME domains. This unusual contrast is attributed to the dynamic ME effect of the spin-wave excitations, as confirmed by our microscopic model, which also captures the characteristics of the observed static ME effect. Our proof-of-principle study, demonstrating the control and the optical readout of ME domains in LiCoPO$_4$, lays down the foundation for future ME memory devices based on antiferroelectric-antiferromagnetic insulators.Comment: 6 pages, 4 figures + Supplementary (10 pages and 4 figures

Spin excitations of magnetoelectric LiNiPO4_4 in multiple magnetic phases

Spin excitations of magnetoelectric LiNiPO$_4$ are studied by infrared absorption spectroscopy in the THz spectral range as a function of magnetic field through various commensurate and incommensurate magnetically ordered phases up to 33\,T. Six spin resonances and a strong two-magnon continuum are observed in zero magnetic field. Our systematic polarization study reveals that some of the excitations are usual magnetic-dipole active magnon modes, while others are either electromagnons, electric-dipole active, or magnetoelectric, both electric- and magnetic-dipole active spin excitations. Field-induced shifts of the modes for all three orientations of the field along the orthorhombic axes allow us to refine the values of the relevant exchange couplings, single-ion anisotropies, and the Dzyaloshinskii-Moriya interaction on the level of a four-sublattice mean-field spin model. This model also reproduces the spectral shape of the two-magnon absorption continuum, found to be electric-dipole active in the experiment

Spin-induced polarizations and nonreciprocal directional dichroism of the room-temperature multiferroic BiFeO3

A microscopic model for the room-temperature multiferroic BiFeO3 that includes two Dzyaloshinskii-Moriya interactions and single-ion anisotropy along the ferroelectric polarization pre- dicts both the zero-field spectroscopic modes as well as their splitting and evolution in a magnetic field. Due to simultaneously broken time-reversal and spatial-inversion symmetries, the absorp- tion of light changes as the magnetic field or the direction of light propagation is reversed. We discuss three physical mechanisms that may contribute to this absorption asymmetry known as non-reciprocal directional dichroism: the spin current, magnetostriction, and single-ion anisotropy. We conclude that the non-reciprocal directional dichroism in BiFeO3 is dominated by the spin- current polarization and is insensitive to the magnetostriction and easy-axis anisotropy. With three independent spin-current parameters, our model accurately describes the non-reciprocal directional dichroism observed for magnetic field along [1, −1, 0]. Since some modes are almost transparent to light traveling in one direction but opaque for light traveling in the opposite direction, BiFeO3 can be used as a room-temperature optical diode at certain frequencies in the GHz to THz range. Our work demonstrates that an analysis of the non-reciprocal directional dichroism spectra based on an effective spin model supplemented by first-principles calculations can produce a quantitative microscopic theory of the magnetoelectric couplings in multiferroic materials

Observation of E8 Particles in an Ising Chain Antiferromagnet

Near the transverse-field induced quantum critical point of the Ising chain, an exotic dynamic spectrum consisting of exactly eight particles was predicted, which is uniquely described by an emergent quantum integrable field theory with the symmetry of the $E_8$ Lie algebra, but rarely explored experimentally. Here we use high-resolution terahertz spectroscopy to resolve quantum spin dynamics of the quasi-one-dimensional Ising antiferromagnet BaCo$_2$V$_2$O$_8$ in an applied transverse field. By comparing to an analytical calculation of the dynamical spin correlations, we identify $E_8$ particles as well as their two-particle excitations.Comment: 6 pages, 3 figures, plus supplementary material

Spin-induced polarizations and nonreciprocal directional dichroism of the room-temperature multiferroic BiFeO3

A microscopic model for the room-temperature multiferroic BiFeO3 that includes two Dzyaloshinskii-Moriya interactions and single-ion anisotropy along the ferroelectric polarization predicts both the zero-field spectroscopic modes as well as their splitting and evolution in a magnetic field. Due to simultaneously broken time-reversal and spatial-inversion symmetries, the absorption of light changes as the magnetic field or the direction of light propagation is reversed. We discuss three physical mechanisms that may contribute to this absorption asymmetry known as nonreciprocal directional dichroism: the spin current, magnetostriction, and single-ion anisotropy. We conclude that the nonreciprocal directional dichroism in BiFeO3 is dominated by the spin-current polarization and is insensitive to the magnetostriction and easy-axis anisotropy. With three independent spin-current parameters, our model accurately describes the nonreciprocal directional dichroism observed for magnetic field along [1,-1,0]. Since some modes are almost transparent to light traveling in one direction but opaque for light traveling in the opposite direction, BiFeO3 behaves as a room-temperature optical diode at certain frequencies in the gigahertz to terahertz range. Our work demonstrates that an analysis of the nonreciprocal directional dichroism spectra based on an effective spin model supplemented by first-principles calculations can produce a quantitative microscopic theory of the magnetoelectric couplings in multiferroic materials.clos

The Magnetoelastic Distortion of Multiferroic BiFeO3_3 in the Canted Antiferromagnetic State

Using THz spectroscopy, we show that the spin-wave spectrum of multiferroic BiFeO$_3$ in its high-field canted antiferromagnetic state is well described by a spin model that violates rhombohedral symmetry. We demonstrate that the monoclinic distortion of the canted antiferromagnetic state is induced by the single-ion magnetoelastic coupling between the lattice and the two nearly anti-parallel spins. The revised spin model for BiFeO$_3$ contains two new single-ion anisotropy terms that violate rhombohedral symmetry and depend on the direction of the magnetic field.Comment: 28 pages (main & supplementary), 2 figures (main article), 15 figures (supplementary material

Experimental determination of the interaction potential between a helium atom and the interior surface of a C60 fullerene molecule

The interactions between atoms and molecules may be described by a potential energy function of the nuclear coordinates. Non-bonded interactions are dominated by repulsive forces at short range and attractive dispersion forces at long range. Experimental data on the detailed interaction potentials for non-bonded interatomic and intermolecular forces is scarce. Here we use terahertz spectroscopy and inelastic neutron scattering to determine the potential energy function for the non-bonded interaction between single He atoms and encapsulating C60 fullerene cages, in the helium endofullerenes 3He and 4He, synthesised by molecular surgery techniques. The experimentally derived potential is compared to estimates from quantum chemistry calculations, and from sums of empirical two-body potentials.Comment: 25 pages, 14 figures, submitted to Journal of Chemical Physic

The dipolar endofullerene HF@C60

The cavity inside fullerenes provides a unique environment for the study of isolated atoms and molecules. We report encapsulation of hydrogen fluoride inside C60 using molecular surgery to give the endohedral fullerene HF@C60. The key synthetic step is the closure of the open fullerene cage while minimizing escape of HF. The encapsulated HF molecule moves freely inside the cage and exhibits quantization of its translational and rotational degrees of freedom, as revealed by inelastic neutron scattering and infrared spectroscopy. The rotational and vibrational constants of the encapsulated HF molecules were found to be redshifted relative to free HF. The NMR spectra display a large 1H-19F J coupling typical of an isolated species. The dipole moment of HF@C60 was estimated from the temperature-dependence of the dielectric constant at cryogenic temperatures and showed that the cage shields around 75% of the HF dipole