Ferroelectric switching in BiFeO$_3$ multiferroic thin films with intrinsic ``stripe-like'' and ``bubble-like'' polydomain configurations was studied by piezoresponse force microscopy. Using the local electric field applied by a scanning probe microscope tip, we observe reversal of both out-of-plane and in-plane components of the polarization, with the final domain state depending on the tip sweeping direction. In ``bubble-like'' samples, complete control of the polarization is achieved, with in-plane polarization change mediated and stabilized by out-of-plane polarization reversal. In ``stripe-like'' samples the intrinsic domain structure influences polarization switching and in-plane reversal may occur without out-of-plane change. The observed switching behaviour can be well correlated with the radial and vertical components of the highly inhomogeneous electric field applied by the tip.
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.
We present an ab initio study of the BFCO solid solution formed by multiferroics BiFeO3 (BFO) and BiCoO3 (BCO). We find that BFCO presents a strongly discontinuous morphotropic transition between BFO-like and BCO-like ferroelectric phases. Further, for all compositions such phases remain (meta)stable and retain well-differentiated properties. Our results thus suggest that an electric field can be used to switch between these structures, and show that such a switching involves large phase-change effects of various types, including piezoelectric, electric, and magnetoelectric ones.
We have analyzed the morphology of ferroelectric domains in very thin films of multiferroic BiFeO3. Unlike the more common stripe domains observed in thicker films BiFeO3 or in other ferroics, the domains tend not to be straight, but irregular in shape, with significant domain wall roughening leading to a fractal dimensionality. Also contrary to what is usually observed in other ferroics, the domain size appears not to scale as the square root of the film thickness. A model is proposed in which the observed domain size as a function of film thickness can be directly linked to the fractal dimen…
We studied the light-induced effects in BiFeO$_3$ single crystals as a function of temperature by means of optical spectroscopy. Here we report the observation of several light-induced absorption features, which are discussed in terms of the photostriction effect and are interpreted in terms of excitons. The temperature dependence of their energy position suggests a possible coupling between the excitons and the lattice vibrations. Moreover, there are hints for anomalies in the temperature evolution of the excitonic features, which might be related to the temperature-induced magnetic phase tra…
We report a comprehensive study of ultrafast carrier dynamics in single crystals of multiferroic BiFeO$_{3}$. Using femtosecond optical pump-probe spectroscopy, we find that the photoexcited electrons relax to the conduction band minimum through electron-phonon coupling with a $\sim$1 picosecond time constant that does not significantly change across the antiferromagnetic transition. Photoexcited electrons subsequently leave the conduction band and primarily decay via radiative recombination, which is supported by photoluminescence measurements. We find that despite the coexisting ferroelectri…
Multiferroic BiFeO3 undergoes a transition from a distorted spiral phase to a G-type antiferromagnet above a critical field H_c that depends on the orientation m of the field. We show that H_c(m) has a maximum when oriented along a cubic diagonal parallel to the electric polarization P and a minimum in the equatorial plane normal to P when two magnetic domains with the highest critical fields are degenerate. The measured critical field along a cubic axis is about 19 T but H_c is predicted to vary by as much as 2.5 T above and below this value. The orientational dependence of H_c(m) is more com…
The magnetic-field-dependent spin ordering of strained BiFeO3 films is determined using nuclear resonant scattering and Raman spectroscopy. The critical field required to destroy the cycloidal modulation of the Fe spins is found to be significantly lower than in the bulk, with appealing implications for field-controlled spintronic and magnonic devices.
We report the direct observation of a "resonance" mode in the lowest-energy optic phonon very near the zone center around (111) in the multiferroic BiFeO$_3$ using neutron scattering methods. The phonon scattering intensity is enhanced when antiferromagnetic (AFM) order sets in at T$_N = 640$~K, and it increases on cooling. This "resonance" is confined to a very narrow region in energy-momentum space where no spin-wave excitation intensity is expected, and it can be modified by an external magnetic field. Our results suggest the existence of a novel coupling between the lattice and spin fluctu…
We report local probe investigations of the magnetic interaction between BiFeO3 films and a ferromagnetic Co0.9Fe0.1 layer. Within the constraints of intralayer exchange coupling in the Co0.9Fe0.1, the multiferroic imprint in the ferromagnet results in a collinear arrangement of the local magnetization and the in-plane BiFeO3 ferroelectric polarization. The magnetic anisotropy is uniaxial, and an in-plane effective coupling field of order 10 mT is derived. Measurements as a function of multiferroic layer thickness show that the influence of the multiferroic layer on the magnetic layer becomes …
Multiferroics permit the magnetic control of the electric polarization and 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 unpolarize…
A morphotropic phase boundary driven by epitaxial strain has been observed in a lead-free multiferroic BiFeO3 thin films and the strain-driven phase transitions were widely reported to be iso-symmetric Cc-Cc ones by recent works. In this paper, we suggest that the tetragonal-like BiFeO3 phase identified in epitaxial films on (001) LaAlO3 single crystal substrates is monoclinic MC. This MC phase is different from MA type monoclinic phase reported in BiFeO3 films grown on low mismatch substrates, such as SrTiO3. This is confirmed not only by synchrotron x-ray studies but also by piezoresponse fo…
Recent works have shown that the domain walls of room-temperature multiferroic BiFeO3 (BFO) thin films can display distinct and promising functionalities. It is thus important to understand the mechanisms underlying domain formation in these films. High-resolution x-ray diffraction and piezo-force microscopy, combined with first-principles simulations, have allowed us to characterize both the atomic and domain structure of BFO films grown under compressive strain on (001)-SrTiO3, as a function of thickness. We derive a twining model that describes the experimental observations and explains why…
The pressure dependence of light-induced effects in single-crystalline BiFeO$_3$ is studied by optical spectroscopy. At low pressures, we observe three light-induced absorption features with energies just below the two crystal field excitations and the absorption onset, respectively. These absorption features were previously ascribed to excitons, possibly connected with the ultra-fast photostriction effect in BiFeO$_3$. The pressure-induced redshift of the absorption features follows the pressure dependence of the corresponding crystal field excitations and absorption onset, suggesting the lin…
The temperature dependence of exchange bias properties are studied in polycrystalline $ \mathrm{BiFeO_3} / \mathrm{Ni_{81}Fe_{19}} $ bilayers, for different $ \mathrm{BiFeO_3} $ thicknesses. Using a field cooling protocol, a non-monotonic behavior of the exchange bias field is shown in the exchange-biased bilayers. Another thermal protocol, the Soeya protocol, related to the $ \mathrm{BiFeO_3} $ thermal activation energies was carried out and reveals a two-step evolution of the exchange bias field. The results of these two different protocols are similar to the ones obtained for measurements p…
In this article the mechanism of the linear magnetoelectric (ME) effect in the rhombohedral multiferroic BiFeO$_3$ is considered. The study is based on the symmetry approach of the GinzburgLandau type, in which polarization, antiferrodistortion, and antiferromagnetic momentum vectors are viewed as ordering parameters. We demonstrate that the linear ME effect in BFO is caused by reorientation of the antiferrodistortion vector in either electric or magnetic field. The numerical estimations, which show quantitative agreement with the results of the recent measurements in film samples, have been p…
We have combined neutron scattering and piezoresponse force microscopy to study the relation between the exchange bias observed in CoFeB/BiFeO3 heterostructures and the multiferroic domain structure of the BiFeO3 films. We show that the exchange field scales with the inverse of the ferroelectric and antiferromagnetic domain size, as expected from Malozemoff's model of exchange bias extended to multiferroics. Accordingly, polarized neutron reflectometry reveals the presence of uncompensated spins in the BiFeO3 film at the interface with the CoFeB. In view of these results we discuss possible st…
Epitaxial Mn-doped BiFeO3 (MBFO) thin films were grown on GaAs (001) substrate with SrTiO3 (STO) buffer layer by pulsed laser deposition. X-ray diffraction results demonstrate that the films show pure (00l) orientation, and MBFO(100)//STO(100), whereas STO (100)//GaAs (110). Piezoresponse force microscopy images and polarization versus electric field loops indicate that the MBFO films grown on GaAs have an effective ferroelectric switching. The MBFO films exhibit good ferroelectric behavior (2Pr ~ 92 μC/cm2 and 2EC ~ 372 kV/cm). Ferromagnetic property with saturated magnetization of 6.5 emu/cm…
Using the results of x-ray and neutron diffraction experiments, we show that the ferroelectric polarization, in ~22 nm particles of BiFeO3, exhibits a jump by ~30% around the magnetic transition point T_N (~635 K) and a suppression by ~7% under 5T magnetic field at room temperature (<<T_N). These results confirm presence of strong multiferroic coupling even in nanoscale BiFeO3 and thus could prove to be quite useful for applications based on nanosized devices of BiFeO3.
The spectroscopic modes of multiferroic BiFeO$_3$ provide detailed information about the very small anisotropy and Dzyaloshinskii-Moriya (DM) interactions responsible for the long-wavelength, distorted cycloid below $\TN = 640$ K. A microscopic model that includes two DM interactions and easy-axis anisotropy predicts both the zero-field spectroscopic modes as well as their splitting and evolution in a magnetic field applied along a cubic axis. While only six modes are optically active in zero field, all modes at the cycloidal wavevector are activated by a magnetic field. The three magnetic dom…
An experimental study of the in-plane azimuthal behaviour and frequency dependence of the ferromagnetic resonance field and the resonance linewidth as a function of BiFeO$_3$ thickness is carried out in a polycrystalline exchange-biased BiFeO$_3$/Ni$_{81}$Fe$_{19}$ system. The magnetization decrease of the Pt/BiFeO$_3$/Ni$_{81}$Fe$_{19}$/Pt heterostructures with BiFeO$_3$ thickness deduced from static measurements has been confirmed by dynamic investigations. Ferromagnetic resonance measurements have shown lower gyromagnetic ratio in a perpendicular geometry compared with that of a parallel ge…
Magnetic phase transitions in multiferroic bismuth ferrite (BiFeO3) induced by magnetic field, epitaxial strain, and composition modification are considered. These transitions from a spatially modulated spin spiral state to a homogenous antiferromagnetic one are accompanied by the release of latent magnetization and a linear magnetoelectric effect that makes BiFeO3-based materials efficient room-temperature single phase multiferroics.
The incommensurate magnetic structures and phase diagrams of multiferroics has been explored on the basis of accurate micromagnetic analysis taking into account the spin flexoelecric interaction (Lifshitz invariant). The objects of the study are BiFeO_3-like single crystals and epitaxial films grown on the <111> substrates. The main control parameters are the magnetic field, the magnetic anisotropy, and the epitaxial strain in the case of films. We predict novel quasi-cycloidal structures induced by external magnetic field or by epitaxial strain in the BiFeO_3-films. Phase diagrams representin…
Artificial superlattices of (BiFeO3)m(SrTiO3)m (m= 1 to 10 unit cells) consisting of multiferroic BiFeO3 and insulating SrTiO3 layers were fabricated on (100)-oriented SrTiO3 substrates by pulsed laser ablation. The remnant polarization and leakage current behavior were studied varying the periodicity (8-80A) of the superlattice. The leakage current was reduced by few orders of magnitude on increase of periodicity compared to single layer BiFeO3 thin films. Reduced leakage and intrinsic polarization hysteresis was observed and was confirmed by PUND analysis for periodicities in the range 20-60…
In this investigation, undoped BiFeO$_3$, Gd doped Bi$_{0.9}$Gd$_{0.1}$FeO$_3$, and Gd-Ti co-doped Bi$_{0.9}$Gd$_{0.1}$Fe$_{1-x}$Ti$_x$O$_3$ (x = 0.10, 0.20) materials were synthesized to report their multiferroic properties. The structural analysis and phase identification of these multiferroic ceramics were performed using Rietveld refinement. The Rietveld analysis has confirmed the high phase purity of the 10% Gd-Ti co-doped Bi$_{0.9}$Gd$_{0.1}$Fe$_{0.9}$Ti$_{0.1}$O$_3$ sample compared to that of other compositions under investigation. The major phase of this particular composition is of rh…
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…
A remarkably high saturation magnetization of ~0.4mu_B/Fe along with room temperature ferromagnetic hysteresis loop has been observed in nanoscale (4-40 nm) multiferroic BiFeO_3 which in bulk form exhibits weak magnetization (~0.02mu_B/Fe) and an antiferromagnetic order. The magnetic hysteresis loops, however, exhibit exchange bias as well as vertical asymmetry which could be because of spin pinning at the boundaries between ferromagnetic and antiferromagnetic domains. Interestingly, like in bulk BiFeO_3, both the calorimetric and dielectric permittivity data in nanoscale BiFeO_3 exhibit chara…
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…
We report on the functionalization of multiferroic BiFeO3 epitaxial films for spintronics. A first example is provided by the use of ultrathin layers of BiFeO3 as tunnel barriers in magnetic tunnel junctions with La2/3Sr1/3MnO3 and Co electrodes. In such structures, a positive tunnel magnetoresistance up to 30% is obtained at low temperature. A second example is the exploitation of the antiferromagnetic spin structure of a BiFeO3 film to induce a sizeable (~60 Oe) exchange bias on a ferromagnetic film of CoFeB, at room temperature. Remarkably, the exchange bias effect is robust upon magnetic f…
We apply ultrafast X-ray diffraction with femtosecond temporal resolution to monitor the lattice dynamics in a thin film of multiferroic BiFeO$_3$ after above-bandgap photoexcitation. The sound-velocity limited evolution of the observed lattice strains indicates a quasi-instantaneous photoinduced stress which decays on a nanosecond time scale. This stress exhibits an inhomogeneous spatial profile evidenced by the broadening of the Bragg peak. These new data require substantial modification of existing models of photogenerated stresses in BiFeO$_3$: the relevant excited charge carriers must rem…
The spin wave spectra of multiferroic BiFeO3 films is calculated using a phenomenological Landau theory that includes magnetostatic effects. The lowest frequency magnon dispersion is shown to be quite sensitive to the angle between spin wave propagation vector and the Neel moment. Since electrical switching of the Neel moment has recently been demonstrated in this material, the sensitivity of the magnon dispersion permits direct electrical switching of spin wave propagation. This effect can be used to construct spin wave logical gates without current pulses, potentially allowing reduced power …
In multiferroic BiFeO3 thin films grown on highly mismatched LaAlO3 substrates, we reveal the coexistence of two differently distorted polymorphs that leads to striking features in the temperature dependence of the structural and multiferroic properties. Notably, the highly distorted phase quasi-concomitantly presents an abrupt structural change, transforms from a hard to a soft ferroelectric and transitions from antiferromagnetic to paramagnetic at 360+/-20 K. These coupled ferroic transitions just above room temperature hold promises of giant piezoelectric, magnetoelectric and piezomagnetic …
In the last few years, some ideas of electric manipulations in ferromagnetic heterostructures have been proposed for developing next generation spintronic devices. Among them, the magnetization switching driven by spin-orbit torque (SOT) is being intensely pursued. Especially, how to control the switching current density, which is expected to enrich device functionalities, has aroused much interest among researchers all over the world. In this paper, a novel method to adjust the switching current is proposed, and the BiFeO3 (BFO) based heterostructures with opposite spontaneous polarizations f…
Multiferroic BiFeO3 epitaxial films with thickness ranging from 40 nm to 960 nm were grown by pulsed laser deposition on SrTiO3 (001) substrates with SrRuO3 bottom electrodes. X-ray characterization shows that the structure evolves from angularly-distorted tetragonal with c/a ~ 1.04 to more bulk-like distorted rhombohedral (c/a ~ 1.01) as the strain relaxes with increasing thickness. Despite this significant structural evolution, the ferroelectric polarization along the body diagonal of the distorted pseudo-cubic unit cells, as calculated from measurements along the normal direction, barely ch…
We report polarized neutron scattering and piezoresponse force microscopy studies of millimeter-sized single crystals of multiferroic BiFeO$_3$. The crystals, grown below the Curie temperature, consist of a single ferroelectric domain. Two unique electric polarization directions, as well as the populations of equivalent spiral magnetic domains, can be switched reversibly by an electric field. A ferroelectric monodomain with a single-$q$ single-helicity spin spiral can be obtained. This level of control, so far unachievable in thin films, makes single-crystal BiFeO$_3$ a promising object for mu…
We report the epitaxial growth of BiFeO3 by pulsed electron deposition and the resulting crystal quality, magnetic and nanoscale switching properties. X-ray diffraction shows high quality single phase, epitaxial (001) oriented films grown on SrTiO3 (001) substrates. Both field and temperature dependent magnetic properties reveal an antiferromagnetic behavior of the films. For the film with a SrRuO3 bottom electrode, an exchange-enhancement effect between antiferromagnetic BiFeO3 and ferromagnetic SrRuO3 was observed at low temperature. The piezoelectric force microscopy and switching spectrosc…
We have identified three of the four magnetoelectric modes of multiferroic BiFeO$_3$ measured using THz spectroscopy. Excellent agreement with the observed peaks is obtained by including the effects of easy-axis anisotropy along the direction of the electric polarization. By distorting the cycloidal spin state, anisotropy splits the $Ψ_{\pm 1}$ mode into peaks at 20 and 21.5 cm$^{-1}$ and activates the lower $Φ_{\pm 2}$ mode at 27 cm$^{-1}$ (T=200 K). An electromagnon is identified with the upper $Ψ_{\pm 1}$ mode at 21.5 cm$^{-1}$. Our results also explain recent Raman and inelastic neutron-sc…
We describe the directional growth of ferroelectric domains in a multiferroic BiFeO3 thin film, which was grown epitaxially on a vicinal (001) SrTiO3 substrate. A detailed structural analysis of the film shows that a strain gradient, which can create a symmetry breaking in a ferroelectric double well potential, causes ferroelectric domains to grow with preferred directionality under the influence of an electric field. Our results suggest the possibility of controlling the direction of domain growth with an electric field by imposing constraints on ferroelectric films, such as a strain gradient…
We report results of a comprehensive study of the phase transition at T_N (~643 K) as a function of particle size in multiferroic BiFeO3 system. We employed electrical, thermal, and temperature dependent X-ray diffraction (XRD) studies in order to characterize the transition in a host of samples. We also carried out detailed magnetic measurements over a temperature regime 2-300 K under a magnetic field 100-10000 Oe both on bulk and nano-crystalline systems. While in the bulk system a sharp endothermic peak at T_N together with a broad feature, ranging over nearly ~150 K (Delta_T), could be obs…
The perovskite (1-x)YMnO$_3$-xBiFeO$_3$ binary system is very promising because of its multiferroic end members. Nanocrystalline phases have been recently obtained by mechanosynthesis across the system, and the perovskite structural evolution has been described. Two continuous solid solutions with orthorhombic Pnma and rhombohedral R3c symmetries were found, which coexist within a broad compositional interval of 0.5 < x < 0.9. This might be a polar-nonpolar morphotropic phase boundary region, at which strong phase-change magnetoelectric responses can be expected. A major issue is phase decompo…
Multiferroic bismuth ferrite (BiFeO3) thin films were prepared by pulsed laser deposition (PLD) technique. Electronic structures of the film have been studied by in situ photoemission spectroscopy (PES) and x-ray absorption spectroscopy (XAS). Both the Fe 2p PES and XAS spectra show that Fe ion is formally in +3 valence state. The Fe 2p and O K edge XAS spectra indicate that the oxygen octahedral crystal ligand field splits the unoccupied Fe 3d state to t2g and eg states. Valence band Fe 2p-3d resonant photoemission results indicate that hybridization between Fe 3d and O 2p plays important rol…
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.
BiFeO3 thin films with various thicknesses were grown epitaxially on (001) LaSrAlO4 single crystal substrates using pulsed laser deposition. High resolution x-ray diffraction measurements revealed that a tetragonal-like phase with c-lattice constant ~4.65 Å is stabilized by a large misfit strain. Besides, a rhombohedral-like phase with c-lattice constant ~3.99 Å was also detected at film thickness of ~50 nm and above to relieve large misfit strains. In-plane piezoelectric force microscopy studies showed clear signals and self-assembled nanoscale stripe domain structure for the tetragonal-like …
We have investigated the effect of temperature on magnetic properties of Bi$_{0.9}$Gd$_{0.1}$Fe$_{1-x}$Ti$_x$O$_3$ (x = 0.00-0.20) multiferroic system. Unexpectedly, the coercive fields ($H_{c}$) of this multiferroic system increased with increasing temperature. The coercive fields and remanent magnetization were higher over a wide range of temperatures in sample x = 0.10 i.e. in sample having composition Bi$_{0.9}$Gd$_{0.1}$Fe$_{0.9}$Ti$_{0.1}$O$_3$ than those of x = 0.00 and 0.20 compositions. Therefore, we have carried out temperature dependent magnetization experiments extensively for samp…
Low-energy magnon excitations in multiferroic BiFeO$_3$ were measured in detail as a function of temperature around several Brillouin zone centers by inelastic neutron scattering experiments on single crystals. Unique features around 1 meV are directly associated with the interplay of the Dzyaloshinskii-Moriya interaction and a small single-ion anisotropy. The temperature dependence of these and the exchange interactions were determined by fitting the measured magnon dispersion with spin-wave calculations. The spectra best fits an easy-axis type magnetic anisotropy and the deduced exchange and…
Over the years attempts have been made to compensate for the inherent weaknesses in the bulk state of the multiferroic BiFeO3, such as high leakage current and the absence of ferromagnetic correlation, and exploit its magnetoelectric potential by forming solid solutions with other perovskites. Studies in the recent few years have shown that alloying of BiFeO3 with BaTiO3, both with and without additives, can induce both ferroelectric and ferromagnetic switching. While the coexistence of both the ferroic orders is encouraging from the view point of technological applications, the origin of ferr…
We present results of an {\it ab initio} density functional theory study of three bismuth-based multiferroics, BiFeO$_{3}$, Bi$_{2}$FeCrO$_{6}$, and BiCrO$_{3}$. We disuss differences in the crystal and electronic structure of the three systems, and we show that the application of the LDA+$U$ method is essential to obtain realistic structural parameters for Bi$_{2}$FeCrO$_{6}$. We calculate the magnetic nearest neighbor coupling constants for all three systems and show how Anderson's theory of superexchange can be applied to explain the signs and relative magnitudes of these coupling constants…
The spin-driven polarizations of type-I multiferroics are veiled by the preexisting ferroelectric (FE) polarization. Using first-principles calculations combined with a spin model, we uncover two hidden but huge spin-driven polarizations in the room-temperature multiferroic BiFeO3. One is associated with the global inversion symmetry broken by a FE distortion and the other is associated with the local inversion symmetry broken by an antiferrodistortive octahedra rotation. Comparison with recent neutron scatterings reveals that first polarization reaches 3.0 $μ$C/cm$^2$, which is larger than in…
The anisotropic optical properties of multiferroic BiFeO$_3$ thin films have been determined with Mueller matrix ellipsometry at room-temperature. The full dielectric tensors of tetragonal-like and rhombohedral-like BiFeO$_3$ phases epitaxially grown on LaAlO$_3$ and SrTiO$_3$ single crystal substrates, respectively, within the spectral range of 0.6 and 6.5 eV are reported. Strain-driven anisotropy changes and transition shifts are observed as well as evidence of sub-band gap many-particle excitations are found. The transition shifts, mostly to higher energies for the highly strained tetragona…
We have investigated the nanoscale switching properties of strain-engineered BiFeO3 thin films deposited on LaAlO3 substrates using a combination of scanning probe techniques. Polarized Raman spectral analysis indicate that the nearly-tetragonal films have monoclinic (Cc) rather than P4mm tetragonal symmetry. Through local switching-spectroscopy measurements and piezoresponse force microscopy we provide clear evidence of ferroelectric switching of the tetragonal phase but the polarization direction, and therefore its switching, deviates strongly from the expected (001) tetragonal axis. We also…
BiFeO$_3$ is the most famous multiferroic material, but it has no strong spontaneous magnetization due to its antiferromagnetism. Here we show that giant ferroelectric polarization and strong spontaneous magnetization can be both realized in double perovskite Bi$_2$FeMoO$_6$ with R3 (\#146) space group based on BiFeO$_3$. Our first-principles phonon spectra establishes that this multiferroic R3 phase is stable. Our systematic calculations show that it is a spin-polarized semiconductor with gap reaching to 0.54 eV and has a strong ferroelectric polarization of 85$μ$C/cm$^2$. This ferroelctricit…
Predictability as a probe of manifest and latent physics: The case of atomic scale structural, chemical, and polarization behaviors in multiferroic Sm-doped BiFeO3
The nanostructural evolution of the strain-induced structural phase transition in BiFeO3 is examined. Using high-resolution X-ray diffraction and scanning-probe microscopy-based studies we have uniquely identified and examined the numerous phases present at these phase boundaries and have discovered an intermediate monoclinic phase in addition to the previously observed rhombohedral- and tetragonal-like phases. Further analysis has determined that the so-called mixed-phase regions of these films are not mixtures of rhombohedral- and tetragonal-like phases, but intimate mixtures of highly-disto…
We report our observation of the training effect on dc electrical properties in a nanochain of BiFeO$_3$ as a result of large scale migration of defects under combined influence of electric field and Joule heating. We show that an optimum number of cycles of electric field within the range zero to $\sim$1.0 MV/cm across a temperature range 80-300 K helps in reaching the stable state via a glass-transition-like process in the defect structure. Further treatment does not give rise to any substantial modification. We conclude that such a training effect is ubiquitous in pristine nanowires or chai…
We have studied the magnetic field dependence of far-infrared active magnetic modes in a single ferroelectric domain \BFO/ crystal at low temperature. The modes soften close to the critical field of 18.8\,T along the [001] (pseudocubic) axis, where the cycloidal structure changes to the homogeneous canted antiferromagnetic state and a new strong mode with linear field dependence appears that persists at least up to 31\,T. A microscopic model that includes two \DM/ interactions and easy-axis anisotropy describes closely both the zero-field spectroscopic modes as well as their splitting and evol…
Bismuth ferrite (BiFeO$_3$) is one of the very few known single-phase multiferroic materials. While the bulk compound is rhombohedral (R), the discovery of an epitaxial strain-induced structural transition into a so-called 'super tetragonal-phase' (T-phase) in this material incited a flurry of research activity focused on gaining an understanding of this phase transition and its possible functionalities. This metastable phase of BiFeO$_3$ is also multiferroic, with giant ferroelectric polarization and coexisting antiferromagnetic order, but above all it is the strain relaxation-induced phase m…
Enabling the light-control of complex systems on ultra-short timescales gives rise to rich physics with promising applications. While crucial, the quantitative determination of both the longitudinal and shear photo-induced strains still remains challenging. Here, by scrutinizing asymmetric Bragg peaks pairs $(\pm h01)$ using picosecond time-resolved X-ray diffraction experiments in BiFeO$_3$, we simultaneously determine the longitudinal and shear strains. The relative amplitude of those strains can be explained only if both thermal and non-thermal processes contribute to the acoustic phonon ph…
