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We review electric dipole active magnetic resonance and nonreciprocal directional dichroism in magnetoelectric multiferroic materials in terahertz and millimeter wave regions. Owing to dynamical magnetoelectric coupling generated by the spin-dependent electric polarization, magnetic resonance, which usually occurs owing to magnetic dipole transition, can be induced by the oscillating electric fields of electromagnetic wave. This electric dipole active magnetic resonance can be useful for microscopic investigations of magnetic excitation in unconventional spin systems. The magnetoelectric coupling also induces the nonreciprocal directional dichroism, which provides a novel functionality to materials as an optical diode, in teraheltz and microwave absorption by magnetic resonance. As examples, we describe the results of the high field ESR measurements of the triangular lattice antiferromagnet $$\hbox {CuFeO}_{\mathrm{2}}$$ and the interacting quantum spin dimer systems $$\hbox {TlCuCl}_{\mathrm{3}}$$ and $$\hbox {KCuCl}_{\mathrm{3}}$$ .

KCuCl$_3$ is known to show a quantum phase transition from the disordered to antiferromagnetically ordered phases by applying pressure. There is a longitudinal excitation mode (Higgs amplitude mode) in the vicinity of the quantum critical point in the ordered phase. To detect the Higgs amplitude mode, high-pressure ESR measurements are performed in KCuCl$_3$. The experimental data are analyzed by the extended spin-wave theory on the basis of the vector spin chirality. We report the first ESR detection of the Higgs amplitude mode and the important role of the electric dipole described by the vector spin chirality., 24 pages, 12 figures

The presence of a Higgs amplitude mode is revealed in a two-dimensional spin-half quantum antiferromagnet, C9H18N2CuBr4 by means of neutron scattering. Spontaneous symmetry-breaking quantum phase transitions play an essential role in condensed-matter physics1,2,3. The collective excitations in the broken-symmetry phase near the quantum critical point can be characterized by fluctuations of phase and amplitude of the order parameter. The phase oscillations correspond to the massless Nambu–Goldstone modes whereas the massive amplitude mode, analogous to the Higgs boson in particle physics4,5, is prone to decay into a pair of low-energy Nambu–Goldstone modes in low dimensions2,6,7. Especially, observation of a Higgs amplitude mode in two dimensions is an outstanding experimental challenge. Here, using inelastic neutron scattering and applying the bond-operator theory, we directly and unambiguously identify the Higgs amplitude mode in a two-dimensional S = 1/2 quantum antiferromagnet C9H18N2CuBr4 near a quantum critical point in two dimensions. Owing to an anisotropic energy gap, it kinematically prevents such decay and the Higgs amplitude mode acquires an infinite lifetime.

The Bose–Einstein condensation is a fascinating phenomenon, which results from quantum statistics for identical particles with an integer spin. Surprising properties, such as superfluidity, vortex quantization or Josephson effect, appear owing to the macroscopic quantum coherence, which spontaneously develops in Bose–Einstein condensates. Realization of Bose–Einstein condensation is not restricted in fluids like liquid helium, a superconducting phase of paired electrons in a metal and laser-cooled dilute alkali atoms. Bosonic quasi-particles like exciton-polariton and magnon in solids-state systems can also undergo Bose–Einstein condensation in certain conditions. Here, we report that the quantum coherence in Bose–Einstein condensate of the magnon quasi particles yields spontaneous electric polarization in the quantum magnet TlCuCl3, leading to remarkable magnetoelectric effect. Very soft ferroelectricity is realized as a consequence of the O(2) symmetry breaking by magnon Bose–Einstein condensation. The finding of this ferroelectricity will open a new window to explore multi-functionality of quantum magnets., Magnons, quantized spin excitations in magnetic materials, may undergo Bose-Einstein condensation into a macroscopic correlated quantum state at low temperature. Here, the authors demonstrate how magnon condensation in quantum magnet TlCuCl3 generates an electrical polarization.