Directional Dichroism Research Articles

Nonreciprocal transport in the superconducting state of the chiral crystal NbGe2

Due to the lack of inversion, mirror or other roto-inversion symmetries, chiral crystals possess a well-defined handedness which, when combined with time-reversal symmetry breaking from the application of magnetic fields, can give rise to directional dichroism of the electrical transport phenomena via the magnetochiral anisotropy. In this study, we investigate the nonreciprocal magneto-transport in microdevices of NbGe2, a superconductor with structural chirality. A giant nonreciprocal signal from vortex motions is observed during the superconducting transition, with the ratio of nonreciprocal resistance to the normal resistance γ reaching 6×105 T−1⋅A−1. Interestingly, the intensity can be adjusted and even sign-reversed by varying the current, the temperature, and the crystalline orientation. Our findings illustrate intricate vortex dynamics and offer ways of manipulation on the rectification effect in superconductors with structural chirality.

Magnetochiral tunneling in paramagnetic Co1/3NbS2

Electric currents have the intriguing ability to induce magnetization in nonmagnetic crystals with sufficiently low crystallographic symmetry. Some associated phenomena include the non-linear anomalous Hall effect in polar crystals and the nonreciprocal directional dichroism in chiral crystals when magnetic fields are applied. In this work, we demonstrate that the same underlying physics is also manifested in the electronic tunneling process between the surface of a nonmagnetic chiral material and a magnetized scanning probe. In the paramagnetic but chiral metallic compound Co1/3NbS2, the magnetization induced by the tunneling current is shown to become detectable by its coupling to the magnetization of the tip itself. This results in a contrast across different chiral domains, achieving atomic-scale spatial resolution of structural chirality. To support the proposed mechanism, we used first-principles theory to compute the chirality-dependent current-induced magnetization and Berry curvature in the bulk of the material. Our demonstration of this magnetochiral tunneling effect opens up an avenue for investigating atomic-scale variations in the local crystallographic symmetry and electronic structure across the structural domain boundaries of low-symmetry nonmagnetic crystals.

Directing valley-polarized emission of 3 L WS2 by photonic crystal with directional circular dichroism.

The valley degree of freedom that results from broken inversion symmetry in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) has sparked a lot of interest due to its huge potential in information processing. In this experimental work, to optically address the valley-polarized emission from three-layer (3 L) thick WS2 at room temperature, we employ a SiN photonic crystal slab that has two sets of holes in a square lattice that supports directional circular dichroism engendered by delocalized guided mode resonances. By perturbatively breaking the inversion symmetry of the photonic crystal slab, we can simultaneously manipulate s and p components of the radiating field so that these resonances correspond to circularly polarized emission. The emission of excitons from distinct valleys is coupled into different radiative channels and hence separated in the farfield. This directional exciton emission from selective valleys provides a potential route for valley-polarized light emitters, which lays the groundwork for future valleytronic devices.

Berry-Curvature Engineering for Nonreciprocal Directional Dichroism in Two-Dimensional Antiferromagnets.

In two-dimensional antiferromagnets, we find that the mixed Berry curvature can be attributed as the geometrical origin of the nonreciprocal directional dichroism (NDD), which refers to the difference in light absorption between opposite propagation directions. This Berry curvature is closely related to the uniaxial strain in accordance with the symmetry constraint, leading to a highly tunable NDD, whose sign and strength can be tuned via strain direction. We choose the lattice model of MnBi_{2}Te_{4} as a concrete example. The coupling between mixed Berry curvature and strain also suggests the magnetic quadrupole of the Bloch wave packet as the macroscopic order parameter probed by the NDD in two dimensions, which is distinct from the multiferroic order P×M or the spin toroidal and quadrupole order within a unit cell in previous studies. Our work paves the way for the Berry-curvature engineering for optical nonreciprocity in two-dimensional antiferromagnets.

Visualization of antiferromagnetic domains by nonreciprocal directional dichroism and related optical responses

Nonreciprocal directional dichroism (NDD) is a phenomenon in which the optical absorption is changed by reversing the direction of light propagation or the sign of the magnetic order parameters. While the NDD has mostly been observed in materials with macroscopic magnetization, recent experiments have shown that the NDD can be induced by a specific antiferromagnetic (AFM) spin structure that breaks both space-inversion and time-reversal symmetries. This opens the possibility of visualizing the spatial distribution of AFM domains via the NDD effect. This article reviews the basic features of the NDD, a brief history of the NDD in AFM materials, and recent achievements in visualizing AFM domains via the NDD and related optical responses, and finally provides a perspective on applications of this method for future AFM spintronics research.

Nonreciprocal microwave response at room temperature in multiferroic Y-type hexaferrite BaSrCo2Fe11AlO22

We investigated the microwave response in room-temperature multiferroic BaSrCo2Fe11AlO22. Microwave absorption ascribed to magnetic resonances was observed in the frequency range from 6 to 20 GHz. When the ferroelectric polarization is aligned by the electric and magnetic fields, the magnitude depends on the sign of the microwave propagation vector that indicates the nonreciprocal directional dichroism (NDD). The phenomenon can be observed even at room temperature, the sign can be controlled by the external electric and magnetic fields, and the magnitude of NDD attained is approximately 11% at 300 K and 28% at 200 K. Such microwave properties will open the avenue of practical applications for future wireless communications.

Nonreciprocal Directional Dichroism in Magnetoelectric Spin Glass.

Optical absorption spectra in the visible and near-infrared light were measured for magnetoelectric spin glass Ni_{0.4}Mn_{0.6}TiO_{3} under various field-cooled conditions. Despite the absence of long-range magnetic-dipole order, this spin-glass system exhibits nonreciprocal directional dichroism (NDD) at zero external field after a magnetoelectric field-cooled procedure. This result is distinct from previous studies on NDD in systems with magnetic toroidal moments induced either by long-range magnetic-dipole order or by applying crossed electric and magnetic fields. The present Letter conclusively demonstrates that the observed NDD originates from magnetoelectrically induced ferroic order of magnetic toroidal moments without conventional magnetic-dipole order.

Chirality‐Dependent Magnetoelectric Responses in a Magnetic‐Field‐Induced Ferroelectric Phase of Pb(TiO)Cu4(PO4)4

AbstractMagnetoelectric multiferroic materials can exhibit a variety of functional properties such as electric field control of magnetization and nonreciprocal electromagnetic responses. Such a magnetoelectric response may be further enriched by the combination of the magnetoelectric order and a peculiar crystallographic order, such as crystal chirality. Recently, it was reported that a chiral‐lattice magnet Pb(TiO)Cu4(PO4)4 showing a magnetoelectric quadrupole order in its ground state exhibits anomalous chirality‐induced tilt of magnetization vector with respect to an applied magnetic field. In this progress report, additional results that advance the understanding of chirality‐induced tilt of magnetization vector are presented. It is found that chirality‐induced tilt of the magnetization vector also exists in a magnetic‐field‐induced ferroelectric (FI‐FE) phase of this compound that is stabilized in magnetic fields higher than 16 tesla. The resulting transverse component of the magnetization can be switched with an applied electric field through a polarization reversal. The analysis indicates that this transverse component is as large as ≈0.014 μB per f.u, suggesting that the tilting angle of the magnetization in the FI‐FE phase is much larger than that in the low‐field phase. Also, as another research progress, electric field control of nonreciprocal directional dichroism in the FI‐FE phase is demonstrated.

Nonreciprocal directional dichroism at telecom wavelengths

Magnetoelectrics with ultra-low symmetry and spin-orbit coupling are well known to display a number of remarkable properties including nonreciprocal directional dichroism. As a polar and chiral magnet, Ni3TeO6 is predicted to host this effect in three fundamentally different configurations, although only two have been experimentally verified. Inspired by the opportunity to unravel the structure-property relations of such a unique light-matter interaction, we combined magneto-optical spectroscopy and first-principles calculations to reveal nonreciprocity in the toroidal geometry and compared our findings with the chiral configurations. We find that formation of Ni toroidal moments is responsible for the largest effects near 1.1 eV—a tendency that is captured by our microscopic model and computational implementation. At the same time, we demonstrate deterministic control of nonreciprocal directional dichroism in Ni3TeO6 across the entire telecom wavelength range. This discovery will accelerate the development of photonics applications that take advantage of unusual symmetry characteristics.

Shedding Light on Nonreciprocal Directional Dichroism at High Magnetic Fields in a Multiferroic Material

Large optical nonreciprocal directional dichroism, coupled with an antiferromagnetic order parameter, is observed in a high magnetic field via magneto-optical spectroscopy combined with a pulse magnet technique.

Nonreciprocal Directional Dichroism in a Magnetic-Field-Induced Ferroelectric Phase of Pb(TiO)Cu4(PO4)4

We study nonreciprocal directional dichroism (NDD) of magnetoelectric Pb(TiO)Cu4(PO4)4 in magnetic fields up to 49 T via magneto-optical spectroscopy in the (near-)visible range. Measuring the opti...

Selection rules and dynamic magnetoelectric effect of the spin waves in multiferroic BiFeO3

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.

InSitu 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 insitu 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.

Second-harmonic generation via double topological valley-Hall kink modes in all-dielectric photonic crystals

Nonlinear topological photonics, which explores topics common to the fields of topological phases and nonlinear optics, is expected to open up a new paradigm in topological photonics. Here, we demonstrate second-harmonic generation (SHG) via nonlinear interaction of double topological valley-Hall kink modes in all-dielectric photonic crystals (PhCs). We first show that two topological frequency bandgaps can be created around a pair of frequencies, $\omega_0$ and $2\omega_0$, by gapping out the corresponding Dirac points in two-dimensional honeycomb PhCs. Valley-Hall kink modes along a kink-type domain wall interface between two PhCs placed together in a mirror-symmetric manner are generated within the two frequency bandgaps. Importantly, through full-wave simulations and mode dispersion analysis, we demonstrate that tunable, bi-directional phase-matched SHG via nonlinear interaction of the valley-Hall kink modes inside the two bandgaps can be achieved. In particular, by using Stokes parameters associated to the magnetic part of the valley-Hall kink modes, we introduce a new concept, SHG directional dichroism, which is employed to characterize optical probes for sensing chiral molecules. Our work opens up new avenues towards topologically protected nonlinear frequency mixing and active photonic devices implemented in all-dielectric material platforms.

Electric Dipole Active Magnetic Resonance and Nonreciprocal Directional Dichroism in Magnetoelectric Multiferroic Materials in Terahertz and Millimeter Wave Regions

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 $$\hbox {KCuCl}_{\mathrm{3}}$$ .

Nonreciprocal directional dichroism in multiferroics

Nonreciprocal directional dichroism in multiferroics, namely magnetoelectric coupling in the dynamic regime, is endowed with rich physics and promising applications, which are entangled with fundamental physical components, such as spin, orbital, lattice, charge, and topology. Such a linear nonreciprocal response behavior in the GHz-THz frequency range, represented by optical magnetoelectric effect and magnetochiral dichroism, occurs ubiquitously in material systems with the spontaneous breaking of space-time symmetry, and is subject to Onsager’s reciprocal theorem in the thermodynamic limit. Microscopically, these nonreciprocal responses are usually encoded by toroidization (chirality) and electromagnon (quasiparticle), thus establishing a comprehensive understanding of magnetoelectric coupling and irreversible dynamics. Herein, the basic mechanisms and emergent nonreciprocal directional dichroism in single-phase multiferroics are summarized. We expect that the present review will stimulate diverse possibilities toward nonreciprocal directional dichroism within and beyond multiferroics.

Magnetochiral Dichroism in a Collinear Antiferromagnet with No Magnetization.

We show the directional dichroism in a collinear antiferromagnet MnTiO_{3}. The dichroism between two distinctive antiferromagnetic states with opposite signs of staggered magnetic moments can be regarded as magnetochiral dichroism in the absence of external fields. Electric-field reversal of antiferromagnetic domain causes a change in the absorption intensity of unpolarized light around 2.15eV. The difference in optical absorption between two antiferromagnetic states is reversed for the light propagating in the opposite direction. The absorption coefficient displays a hysteretic behavior for a cycle of sweeping the external electric or magnetic field.

Nonreciprocal directional dichroism of a chiral magnet in the visible range

Nonreciprocal directional dichroism is an unusual light–matter interaction that gives rise to diode-like behavior in low-symmetry materials. The chiral varieties are particularly scarce due to the requirements for strong spin–orbit coupling, broken time-reversal symmetry, and a chiral axis. Here we bring together magneto-optical spectroscopy and first-principles calculations to reveal high-energy, broadband nonreciprocal directional dichroism in Ni3TeO6 with special focus on behavior in the metamagnetic phase above 52 T. In addition to demonstrating this effect in the magnetochiral configuration, we explore the transverse magnetochiral orientation in which applied field and light propagation are orthogonal to the chiral axis and, by so doing, uncover an additional configuration with a unique nonreciprocal response in the visible part of the spectrum. In a significant conceptual advance, we use first-principles methods to analyze how the Ni2+d-to-d on-site excitations develop magneto-electric character and present a microscopic model that unlocks the door to theory-driven discovery of chiral magnets with nonreciprocal properties.

Dynamical magnetoelectric phenomena of skyrmions in multiferroics

Abstract Magnetic skyrmions, nanoscopic spin vortices carrying a quantized topological number in chiral-lattice magnets, are recently attracting great research interest. Although magnetic skyrmions had been observed only in metallic chiral-lattice magnets such as B20 alloys in the early stage of the research, their realization was discovered in 2012 also in an insulating chiral-lattice magnet Cu 2 OSeO 3 $\textrm{Cu}_2\textrm{OSeO}_3$ . A characteristic of the insulating skyrmions is that they can host multiferroicity, that is, the noncollinear magnetization alignment of skyrmion induces electric polarizations in insulators with a help of the relativistic spin-orbit interaction. It was experimentally confirmed that the skyrmion phase in Cu 2 OSeO 3 $\textrm{Cu}_2\textrm{OSeO}_3$ is indeed accompanied by the spin-induced ferroelectricity. The resulting strong magnetoelectric coupling between magnetizations and electric polarizations can provide us with a means to manipulate and activate magnetic skyrmions by application of electric fields. This is in sharp contrast to skyrmions in metallic systems, which are driven through injection of electric currents. The magnetoelectric phenomena specific to the skyrmion-based multiferroics are attracting intensive research interest, and, in particular, those in dynamical regime are widely recognized as an issue of vital importance because their understanding is crucial both for fundamental science and for technical applications. In this article, we review recent studies on multiferroic properties and dynamical magnetoelectric phenomena of magnetic skyrmions in insulating chiral-lattice magnet Cu 2 OSeO 3 $\textrm{Cu}_2\textrm{OSeO}_3$ . It is argued that the multiferroic skyrmions show unique resonant excitation modes of coupled magnetizations and polarizations, so-called electromagnon excitations, which can be activated both magnetically with a microwave magnetic field and electrically with a microwave electric field. The interference between these two activation processes gives rise to peculiar phenomena in the gigahertz regime. As its representative example, we discuss a recent theoretical prediction of unprecedentedly large nonreciprocal directional dichroism of microwaves in the skyrmion phase of Cu 2 OSeO 3 $\textrm{Cu}_2\textrm{OSeO}_3$ . This phenomenon can be regarded as a one-way window effect on microwaves, that is, the extent of microwave absorption changes significantly when its incident direction is reversed. This dramatic effect was indeed observed by subsequent experiments. These studies demonstrated that the multiferroic skyrmions can be a promising building block for microwave devices.

Local-Site Dependency of Magneto-Chiral Dichroism in Enantiopure One-Dimensional Copper(II)–Chromium(III) Coordination Polymers

Magneto-chiral dichroism (MChD) is a nonreciprocal directional dichroism emerged by applying a magnetic field to chiral materials, which provides a clear distinction between light propagating paral...