Displacive martensitic phase transition is potentially promising in semiconductor based data storage applications with fast switching speed. In addition to traditional phase transition materials, the recently discovered two-dimensional ferroic materials are receiving lots of attention owing to their fast ferroic switching dynamics, which could tremendously boost data storage density and enhance read/write speed. In this study, we propose that a terahertz laser with an intermediate intensity and selected frequency can trigger ferroic order switching in two-dimensional multiferroics, which is a damage-free noncontacting approach. Through first-principles calculations, we theoretically and computationally investigate optically induced electronic, phononic, and mechanical responses of two experimentally fabricated multiferroic (with both ferroelastic and ferroelectric) materials, \b{eta}-GeSe and α-SnTe monolayer. We show that the relative stability of different orientation variants can be effectively manipulated via the polarization direction of the terahertz laser, which is selectively and strongly coupled with the transverse optical phonon modes. The transition from one orientation variant to another can be barrierless, indicating ultrafast transition kinetics and the conventional nucleation-growth phase transition process can be avoidable.
We detected broadband coherent terahertz (THz) emission from multiferroic BiFeO3 after illuminating a high-quality bulk single ferroelectric domain crystal with a ~100 fs optical pulse. The dependence of the emitted THz waveform on the energy and polarization of the optical pulse is consistent with the optical rectification mechanism of THz emission. The THz emission provides a sensitive probe of the electric polarization state of BiFeO3, enabling applications in ferroelectric memories and ferroelectric domain imaging. We also report room-temperature THz optical constants of BiFeO3.
Ferroelectric and multiferroic materials form an important class of functional materials. Over the last twenty years, first-principles-based effective Hamiltonian approaches have been successfully developed to simulate these materials. In recent years, effective Hamiltonian approaches were further combined with molecular dynamics methods to investigate terahertz dynamical properties of various perovskites. With this combination, a variety of ferroelectric and multiferroic materials, including BaTiO_{3}, Ba(Sr,Ti)O_{3}, Pb(Zr,Ti)O_{3}, BiFeO_{3}, and SrTiO_{3} bulks and films have been simulate…
We propose that concurrently magnetic and ferroelectric, i.e. multiferroic, compounds endowed with electrically-active magnetic excitations (electromagnons) provide a key to produce large directional dichroism for long wavelengths of light. By exploiting the control of ferroelectric polarization and magnetization in a multiferroic oxide Ba$_2$CoGe$_2$O$_7$, we demonstrate the realization of such a directional light-switch function at terahertz frequecies in resonance with the electromagnon absorption. Our results imply that this hidden potential is present in a broad variety of multiferroics.
Terahertz (THz) radiation has been observed from multiferroic BiFeO$_3$ thin films via ultrafast modulation of spontaneous polarization upon carrier excitation with illumination of femtosecond laser pulses. The radiated THz pulses from BiFeO$_3$ thin films were clarified to directly reflect the spontaneous polarization state, giving rise to a memory effect in a unique style and enabling THz radiation even at zero-bias electric field. On the basis of our findings, we demonstrate potential approaches to ferroelectric nonvolatile random access memory with nondestructive readability and ferroelect…
Electric manipulation of magnetic properties is a key problem of materials research. To fulfil the requirements of modern electronics, these processes must be shifted to high frequencies. In multiferroic materials this may be achieved by electric and magnetic control of their fundamental excitations. Here we identify magnetic vibrations in multiferroic iron-borates which are simultaneously sensitive to external electric and magnetic fields. Nearly 100% modulation of the terahertz radiation in an external field is demonstrated for SmFe3(BO3)4. High sensitivity can be explained by a modification…
High-frequency dielectric studies of Bi_0.85Nd_0.15FeO_3 ceramics performed betweeen 100 and 900 K reveal hardening of most polar phonons on cooling below antiferroelectric phase transition, which occurs near 600 K. Moreover, a strong THz dielectric relaxation is seen in paraelectric phase. Its relaxation frequency softens on cooling towards Tc ~ 600 K, its dielectric strength simultaneously decreases and finaly the relaxation disappears from the spectra below 450 K. Both phonon and dielectric relaxation behavior is responsible for a decrease in the dielectric permittivity at the antiferroelec…
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 evol…
Recent spectroscopic studies at terahertz frequencies for a variety of multiferroics endowed with both ferroelectric and magnetic orders have revealed the possible emergence of a new collective excitation, frequently referred to as electromagnon. It is magnetic origin, but becomes active in response to the electric field component of light. Here we give an overview on our recent advance in the terahertz time-domain spectroscopy of electromagnons or electric-dipole active magnetic resonances, focused on perovskite manganites--$R$MnO$_3$ ($R$ denotes rare-earth ions). The respective electric and…
We show theoretically with an accurate spin Hamiltonian describing the multiferroic Mn perovskites that the application of the picosecond optical pulse with a terahertz frequency can switch the spin chirality through intensely exciting the electromagnons. There are four states with different spin chiralities, i.e. clockwise and counterclockwise ab/bc-plane spin spirals, and by tuning the strength, shape and length of the pulse, the switching among these states can be controlled at will. Dynamical pattern formation during the switching is also discussed.
We used Raman and terahertz spectroscopies to investigate lattice and magnetic excitations and their cross-coupling in the hexagonal YMnO3 multiferroic. Two phonon modes are strongly affected by the magnetic order. Magnon excitations have been identified thanks to comparison with neutron measurements and spin wave calculations but no electromagnon has been observed. In addition, we evidenced two additional Raman active peaks. We have compared this observation with the anti-crossing between magnon and acoustic phonon branches measured by neutron. These optical measurements underly the unusual s…
We study theoretically the electromagnon and its optical spectrum (OS) of the terahertz-frequency regime in the magnetic-spiral-induced multiferroic phases of the rare-earth (R) Mn perovskites, RMnO3, taking into account the elliptical deformation or the higher harmonics of the spiral spin configuration, which has been missed so far. A realistic spin Hamiltonian, which gives phase diagrams in agreement with experiments, resolves a long standing puzzle, i.e., the double-peak structure of the OS with a larger low-energy peak originating from magnon modes hybridized with the zone-edge state. We a…
The control of optical fields is usually achieved through the electro-optic or acousto-optic effect in single-crystal ferroelectric or polar compounds such as LiNbO3 or quartz. In recent years, tremendous progress has been made in ferroelectric oxide thin film technology - a field which is now a strong driving force in areas such as electronics, spintronics and photovoltaics. Here, we apply epitaxial strain engineering to tune the optical response of BiFeO3 thin films, and find a very large variation of the optical index with strain, corresponding to an effective elasto-optic coefficient large…
The optical magnetoelectric effect, which is an inherent attribute of the spin excitations in multiferroics, drastically changes their optical properties compared to conventional materials where light-matter interaction is expressed only by the dielectric permittivity and magnetic permeability. Our polarized absorption experiments performed on multiferroic Ca2CoSi2O7 and Ba2CoGe2O7 in the THz spectral range demonstrate that such magnetoeletric spin excitations show quadrochroism, i.e. they have different colours for all the four combinations of the two propagation directions (forward or backwa…
Chirality, i.e., the right- and left-handedness of structure, is one of the key concepts in many fields of science including biology, chemistry and physics, and its manipulation is an issue of vital importance. The electron spins in solids can form chiral configurations. In perovskite manganites RMnO3 (R=Tb, Dy,...etc), the Mn-spins form a cycloidal structure, which induces ferroelectric polarization (P) through the relativistic spin-orbit interaction. This magnetism-induced ferroelectricity (multiferroics) and associated infrared-active spin waves (electromagnons) open a promising route to co…
An appealing mechanism for inducing multiferroicity in materials is the generation of electric polarization by a spatially varying magnetization that is coupled to the lattice through the spin-orbit interaction. Here we describe the reciprocal effect, in which a time-dependent electric polarization induces magnetization even in materials with no existing spin structure. We develop a formalism for this dynamical multiferroic effect in the case for which the polarization derives from optical phonons, and compute the strength of the phonon Zeeman effect, which is the solid-state equivalent of the…
We derive a sum rule to demonstrate that the static magnetoelectric (ME) effect is governed by optical transitions that are simultaneously excited via the electric and magnetic components of light. By a systematic analysis of magnetic point groups, we show that the ME sum rule is applicable to a broad variety of non-centrosymmetric magnets including ME multiferroic compounds. Due to the dynamical ME effect, the optical excitations in these materials can exhibit directional dichroism, i.e. the absorption coefficient can be different for counter-propagating light beams. According to the ME sum r…
Motivated by the search for type-II multiferroics, we present a comprehensive optical study of a complex oxide family of type-II multiferroic candidates: RbFe(MoO4)2, RbFe(SeO4)2, and RbFe(SO4)2. We employ rotational-anisotropy second harmonic generation spectroscopy (RA SHG), a technique sensitive to point symmetries, to address discrepancies in literature-assigned point/space groups and to identify the correct crystal structures. At room temperature we find that our RA SHG patterns rotate away from the crystal axes in RbFe(AO4)2 (A = Se, S), which identifies the lack of mirror symmetry and i…
Multiferroicity can be induced in strontium titanate by applying biaxial strain, resulting in the coexistence of both ferroelectric and antiferrodistortive domains. The magnitude and sign of the strain imposed on the lattice by design can be used to tune the phase transitions and interactions between these two phenomena. Using optical second harmonic generation, we report a transition from centrosymmetric 4/mmm phase to ferroelectric mm2, followed by an antiferrodistortive transition to a coupled ferroelastic-ferroelectric mm2 phase in a strontium titanate thin film strained in biaxial tension…
We propose an engineering of the optical properties of GaAs/AlGaAs quantum wells using AlAs and InAs monolayer insertions. A quantitative study of the effects of the monolayer position and the well thickness on the interband and intersubband transitions, based on the extended-basis sp3d5s* tight-binding model, is presented. The effect of insertion on the interband transitions is compared with existing experimental data. As for intersubband transitions, we show that in a GaAs/AlGaAs quantum well including two AlAs and one InAs insertions, a three level {e1 , e2 , e3 } system where the transitio…
The rôle of the magnetoelectric effect upon optical reflectivity is studied by adapting an electrodynamic-based model for a system composed by a 2D metallic film in contact with an extended multiferroic material exhibiting weak ferromagnetism. The well-known \emph{Nakayama's} boundary condition is reformulated by taking into account the magnetoelectric coupling as well as an externally applied magnetic field $\mathbf{B}$ in an arbitrary direction. It is found that the reflectance shows strong fluctuations for incident radiation close to the characteristic antiferromagnetic resonance frequency …
The linear electrodynamic properties of graphene -- the frequency-dependent conductivity, the transmission spectra and collective excitations -- are briefly outlined. The non-linear frequency multiplication effects in graphene are studied, taking into account the influence of the self-consistent-field effects and of the magnetic field. The predicted phenomena can be used for creation of new devices for microwave and terahertz optics and electronics.
We investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically-induced dynamics of both films and can be described by a two-temperature model. Surprisingly, gold can exhibit a much smaller terahertz pulse-induced reflectivity change and with opposite sign. For platinum, we estimate a 20% larger electron-phonon coupling for the terahertz-driven dynamics compared to the optically-induced one, which w…
Magnetic excitations in cycloidal magnet LiCu$_2$O$_2$ are explored using THz absorption spectroscopy in magnetic fields up to 12 T. Below the spin ordering temperature we observe eight optically active transitions in the spin system of LiCu$_2$O$_2$ in the energy range from 4 to 30 cm$^{-1}$. In magnetic field the number of modes increases and the electric polarization flop is seen as a change in magnetic field dependence of mode energies. The polarization dependence of two of the modes in zero magnetic field fits the selection rules for the cycloid tilted by $θ=41\pm1^{\circ}$ from the bc pl…
We studied the ultrafast third-order optical nonlinearity in a single crystal of multiferroic bismuth ferrite (BiFeO3) in the near-infrared range of 0.5-1.0 eV, where the material is fundamentally transparent,at room temperature. With pump pulses at 1.55 eV, which is off-resonant to the strong inter-band charge transfer (CT) transition, we observed instantaneous transient absorption with pencil-like temporal profile originating from the two-photon CT transition from the oxygen 2p to the iron 3p levels. In contrast, under pumping with 3.10-eV photons, the pencil-like absorption change was not o…
We studied magnetic excitations in a low-temperature ferroelectric phase of the multiferroic YMn2O5 using inelastic neutron scattering (INS). We identify low-energy magnon modes and establish a correspondence between the magnon peaks observed by INS and electromagnon peaks observed in optical absorption [1]. Furthermore, we explain the microscopic mechanism, which results in the lowest-energy electromagnon peak, by comparing the inelastic neutron spectral weight with the polarization in the commensurate ferroelectric phase.
Low-dimensional multiferroic materials hold great promises in miniaturized device applications such as nanoscale transducers, actuators, sensors, photovoltaics, and nonvolatile memories. Here, using first-principles theory we predict that two-dimensional (2D) monolayer Group IV monochalcogenides including GeS, GeSe, SnS, and SnSe are a class of 2D semiconducting multiferroics with strongly coupled giant in-plane spontaneous ferroelectric polarization and spontaneous ferroelastic lattice strain that are thermodynamically stable at room temperature and beyond, and can be effectively modulated by…
We present a modified $8f$ geometry for time domain terahertz (THz) spectroscopy (TDTS) experiments. We show, through simulations and data, that a simple rearranging of the off-axis parabolic mirrors, which are typically used to focus and direct THz radiation in TDTS experiments, results in a nearly 40% reduction in the THz focal spot diameter. This effect stems from significant reduction of the principle optical aberrations which are enhanced in the conventional $8f$ geometry but partially compensated in the modified $8f$ experimental setup. We compare data from our home-built TDTS spectromet…
