Multiferroic behavior confined by symmetry in EuTiO3 films
P. J. Ryan, G. E. Sterbinsky, Y. Choi, J. C. Woicik, Leyi Zhu, J. S. Jiang, J-H. Lee, D. G. Schlom, T. Birol, S. D. Brown, P. B. J. Thompson, P. S. Normile, J. Lang, J. -W. Kim
We have elucidated the spin, lattice, charge and orbital coupling mechanism underlying the multiferroic character in tensile strained EuTiO3 films. Symmetry determined by oxygen octahedral tilting shapes the hybridization between the Eu 4f and Ti 3d orbitals and this inhibits predicted Ti displacement proper ferroelectricity. Instead, phonon softening emerges at low temperatures within the pseudo-cube (110) plane, orthogonal to the anticipated ferroelectric polarization symmetry. Additionally, the magnetic anisotropy is determined by orbital distortion through hybridization between the Ti 3d and typically isotropic Eu2+ 4f. This unique scenario demonstrates the critical role symmetry plays in the coupling of order parameters defining multiferroic behaviour.
In this work multiferroic thin films of Bi containing perovskite oxides are discussed, where the driving force for ferroelectricity are the Bi3+ lone-pair electrons. First, a brief introduction of Bi containing multiferroic perovskite oxides will be presented to describe the mechanisms for establishing magnetic and ferroelectric order in these compounds and some recent developments in this field of research are reported. The second section addresses experimental aspects of epitaxial thin film growth of BiMnO3, (Bi0.9La0.1)2NiMnO6 (BLNMO) and BiFeO3 thin films by pulsed laser deposition. The th…
We have grown epitaxial thin films of multiferroic BiMnO$_3$ using pulsed laser deposition. The films were grown on SrTiO$_3$ (001) substrates by ablating a Bi-rich target. Using x-ray diffraction we confirmed that the films were epitaxial and the stoichiometry of the films was confirmed using Auger electron spectroscopy. The films have a ferromagnetic Curie temperature ($T_C$) of 85$\pm$5 K and a saturation magnetization of 1 $μ_B$/Mn. The electric polarization as a function of electric field ($P-E$) was measured using an interdigital capacitance geometry. The $P-E$ plot shows a clear hystere…
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…
In this work, we report the growth and functional characterizations of multiferroic TbMnO3 thin films grown on Nb-doped SrTiO3 (001) substrates using pulsed laser deposition. By performing detailed magnetic and ferroelectric properties measurements, we demonstrate that the multiferroicity of spin origin known in the bulk crystals can be successfully transferred to TbMnO3 thin films. Meanwhile, anomalous magnetic transition and unusual magnetoelectric coupling related to Tb moments are observed, suggesting a modified magnetic configuration of Tb in the films as compared to the bulk counterpart.…
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 …
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…
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 …
Multiferroics with the coexistence of ferroelectric and ferromagnetic orders are ideal candidates for magnetoelectric applications. Unfortunately, only very few ferroelectric-ferromagnetic multiferroics (with low magnetic critical temperature) were discovered. Here we perform first principles calculations to investigate the effects of the epitaxial strain on the properties of BiMnO3 films grown along the pseudocubic [001] direction. Unlike the ground state with the centrosymmetric C2/c space group in bulk, we reveal that the tensile epitaxial strain stabilizes the ferromagnetic and ferroelectr…
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…
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…
Temperature dependent impedance spectroscopy enables the many contributions to the dielectric and resistive properties of condensed matter to be deconvoluted and characterized separately. We have achieved this for multiferroic epitaxial thin films of BiFeO3 (BFO) and BiMnO3 (BMO), key examples of materials with strong magneto-electric coupling. We demonstrate that the true film capacitance of the epitaxial layers is similar to that of the electrode interface, making analysis of capacitance as a function of film thickness necessary to achieve deconvolution. We modeled non-Debye impedance respon…
Multiferroic properties of orthorhombic HoMnO3 (Pbnm space group) are significantly modified by epitaxial compressive strain along the a-axis. We are able to focus on the effect of strain solely along the a-axis by using an YAlO3 (010) substrate, which has only a small lattice mismatch with HoMnO3 along the other in-plane direction (the c-axis). Multiferroic properties of strained and relaxed HoMnO3 thin films are compared with those reported for bulk, and are found to differ widely. A relaxed film exhibits bulk-like properties such as a ferroelectric transition temperature of 25 K and an inco…
We investigated the magnetic structure of an orthorhombic YMnO3 thin film by resonant soft x-ray and hard x-ray diffraction. We observed a temperature-dependent incommensurate magnetic reflection below 45 K and a commensurate lattice-distortion reflection below 35 K. These results demonstrate that the ground state is composed of coexisting E-type and cycloidal states. Their different ordering temperatures clarify the origin of the large polarization to be caused by the E-type antiferromagnetic states in the orthorhombic YMnO3 thin film.
The quantitative understanding of converse magnetoelectric effects, i.e., the variation of the magnetization as a function of an applied electric field, in extrinsic multiferroic hybrids is a key prerequisite for the development of future spintronic devices. We present a detailed study of the strain-mediated converse magnetoelectric effect in ferrimagnetic Fe3O4 thin films on ferroelectric BaTiO3 substrates at room temperature. The experimental results are in excellent agreement with numerical simulation based on a two-region model. This demonstrates that the electric field induced changes of …
Multiferroic materials have received an astonishing attention in the last decades due to expectations that potential coupling between distinct ferroic orders could inspire new applications and new device concepts. As a result, a new knowledge on coupling mechanisms and materials science has dramatically emerged. Multiferroic RMnO3 perovskites are central to this progress providing a suitable platform to tailor spin-spin and spin-lattice interactions. With views towards applications, development of thin films of multiferroic materials have also progressed enormously and nowadays thin film manga…
Octahedral distortion plays a key role in engineering the physical properties of heterostructures composed of perovskite oxides. We observe a strong in-plane uniaxial magnetic anisotropy in a strain-enabled multiferroic EuTiO3 thin film epitaxially grown on a (110)o DyScO3 substrate. First principles calculations show that the magnetic anisotropy is closely correlated with the uniaxial TiO6 octahedral tilting and the ferroelectric polarization of the film, indicating potential strong magnetoelectric coupling in the strain-engineered multiferroic system.
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 report on epitaxial growth of single-phase [Pb(Zr0.57Ti0.43)O3]0.8[Pb(Fe2/3W1/3)O3]0.2 (PZT-PFW) solid-solution thin films using pulsed laser deposition. X-ray diffraction measurements reveal that the films have a tetragonal structure. The films exhibit ferroelectric properties and weak ferromagnetic responses at room temperature. Magnetoelectric effects were investigated; the nonlinear magnetoelectric coefficient was measured and found to be comparable to those of multiferroic hexagonal manganites, but at least two orders of magnitude smaller than that for polycrystalline PZT-PFW films.
We report the first magnetic-field-dependent Raman scattering studies on Pb(Zr,Ti)O3-CoFe2O4 bilayer multiferroic system. The phonon frequencies of the nano-bilayers obviously change with magnetic field, which is absent in the single Pb(Zr,Ti)O3 films. The magnetostriction of the CoFe2O4 layer generates stress mechanically transferred to the Pb(Zr,Ti)O3 layer, resulting in the mode changes. The observed magnetic-field-induced softening of the soft mode in the Pb(Zr,Ti)O3 layer bears a striking resemblance to direct magnetoelectric output in the bilayers, providing evidence for stress-mediated …
Multiferroics in which giant ferroelectric polarization and magnetism coexist are of tremendous potential for engineering disruptive applications in information storage and energy conversion. Yet the functional properties of multiferroics are thought to be affected detrimentally by the presence of point defects, which may be abundant due to the volatile nature of some constituent atoms and high temperatures involved in materials preparation. Here, we demonstrate with theoretical methods that oxygen vacancies may enhance the functionality of multiferroics by radically changing their magnetic in…
The crystal and magnetic structures of single-crystalline hexagonal LuFeO$_3$ films have been studied using x-ray, electron and neutron diffraction methods. The polar structure of these films are found to persist up to 1050 K; and the switchability of the polar behavior is observed at room temperature, indicating ferroelectricity. An antiferromagnetic order was shown to occur below 440 K, followed by a spin reorientation resulting in a weak ferromagnetic order below 130 K. This observation of coexisting multiple ferroic orders demonstrates that hexagonal LuFeO$_3$ films are room-temperature mu…
We report the structural and magnetoelectrical properties of La$_{0.7}$Ca$_{0.3}$MnO$_3$/BaTiO$_3$ perovskite superlattices grown on (001)-oriented SrTiO$_3$ by the pulsed laser deposition technique. Magnetic hysteresis loops together with temperature dependent magnetic properties exhibit well-defined coercivity and magnetic transition temperature (T$_C$) \symbol{126}140 K. $DC$ electrical studies of films show that the magnetoresistance (MR) is dependent on the BaTiO$_3$ thickness and negative $MR$ as high as 30% at 100K are observed. The $AC$ electrical studies reveal that the impedance and …
In this work we elaborated and characterized nanocomposite thin films using a preselected multiferroic matrix Bi$_{0.9}$Gd$_{0.1}$Fe$_{0.9}$Mn$_{0.1}$O$_3$ (BGFMO) in the aim to enhance their basic ferroelectric and magnetic properties. The local ferroelectric character of these nanocomposites thin films was investigated by piezoresponse force microscopy (PFM). Switching behavior for ferroelectric domains was probed by locally manipulating domains. The magnetic investigation showed that the incorporation of transition metal elements in the BGFMO matrix brings out interesting increase in the ma…
Cross-coupling of ordering parameters in multiferroic materials by multiple external stimuli other than electric field and magnetic field is highly desirable from both practical application and fundamental study points of view. Recently, mechanical force has attracted great attention in switching of ferroic ordering parameters via electro-elastic coupling in ferroelectric materials. In this work, mechanical force induced polarization and magnetization switching were investigated in a polycrystalline multiferroic Bi0.9La0.1FeO3 thin film using a scanning probe microscopy system. The piezorespon…
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…
We report the structural and physical properties of epitaxial Bi2FeCrO6 thin films on epitaxial SrRuO3 grown on (100)-oriented SrTiO3 substrates by pulsed laser ablation. The 300 nm thick films exhibit both ferroelectricity and magnetism at room temperature with a maximum dielectric polarization of 2.8 microC/cm2 at Emax = 82 kV/cm and a saturated magnetization of 20 emu/cc (corresponding to ~ 0.26 Bohr magneton per rhombohedral unit cell), with coercive fields below 100 Oe. Our results confirm the predictions made using ab-initio calculations about the existence of multiferroic properties in …
We present a phenomenological scheme to study the size-dependent electric voltage-controlled magnetic anisotropy in ferromagnetic (FM)/ferroelectric (FE) heterostructures. The FM layers are either metallic Fe(001), Ni(001), Co(0001), or half-metallic (La, Sr)MnO3 films. Two magnetoelectric mechanisms, i.e., interface-charge and strain-mediated couplings, are considered. We show that the interface-charge mediated coupling is the main mechanism for the magnetoelectic coupling when the FM film thickness is below a certain transition thickness dtr while the strain-mediated coupling dominates above…
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…
It is reported that both dielectricity and magnetism at room temperature have been appreciably improved in Bi4Fe2TiO12 film compared with that of Bi4Fe2TiO12 bulk. X-ray diffraction profiles reveal similar crystalline nature and random orientation of the two but X-ray photoelectron spectroscopy (XPS) experiments indicate 1.4 eV lower binding energy of core-state O 1s in film relative to those of bulk, so the improvement of multiferroics in film are attributed to the oxygen vacancies and high fraction of interface. The results have promising applications in multifunctional integrated devices.
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 ``strip…
A series of superlattices composed of ferromagnetic La$_{0.7}$Ca$_{0.3}$MnO$_3$ (LCMO) and ferroelectric/paraelectric Ba$_{1-x}$Sr$_x$TiO$_3$ (0$\leq $x$\leq $1) were deposited on SrTiO$_3$ substrates using the pulsed laser deposition. Films of epitaxial nature comprised of spherical mounds having uniform size are obtained. Magnetotransport properties of the films reveal a ferromagnetic Curie temperature in the range of 145-158 K and negative magnetoresistance as high as 30%, depending on the type of ferroelectric layers employed for their growth (\QTR{it}{i.e.} '\QTR{it}{x'} value). Ferroelec…
We have investigated the effect of epitaxial strain on the magnetic properties and $B$-site cation ordering in multiferroic Bi$_2$FeCrO$_6$ (001) thin films using a density-functional theory approach. We find that in thin films with rock-salt ordering of Fe and Cr the ground state is characterised by C-type anti-ferromagnetic (AFM) order. This is in contrast to the bulk form of the material which was predicted to be a ferrimagnet with G-type AFM order. Furthermore, the cation ordered thin-films undergo a transition with epitaxial strain from C to A-type AFM order. Other magnetic orders appear …
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…
Ultrafast optical pump-probe spectroscopy is used to reveal the coexistence of coupled antiferromagnetic/ferroelectric and ferromagnetic orders in multiferroic TbMnO3 films through their time domain signatures. Our observations are explained by a theoretical model describing the coupling between reservoirs with different magnetic properties. These results can guide researchers in creating new kinds of multiferroic materials that combine coupled ferromagnetic, antiferromagnetic and ferroelectric properties in one compound.
Elastic strain is potentially an important approach in tuning the properties of the improperly multiferroic hexagonal ferrites, the details of which have however been elusive due to the experimental difficulties. Employing the method of restrained thermal expansion, we have studied the effect of isothermal biaxial strain in the basal plane of h-LuFeO3 (001) films. The results indicate that a compressive biaxial strain significantly enhances the ferrodistortion, and the effect is larger at higher temperatures. The compressive biaxial strain and the enhanced ferrodistortion together, cause an in…
We present electric and magnetic properties of 0.8Pb(Fe1/2Nb1/2)O3-0.2Pb(Mg1/2W1/2)O3 films epitaxially grown on (001) SrTiO3 substrates using pulsed laser deposition. A narrow deposition window around 710 oC and 0.2 mbar has been identified to achieve epitaxial single-phase thin films. A typical Vogel-Fulcher relaxor-like dielectric and magnetic susceptibility dispersion is observed, suggesting magnetoelectric relaxor behavior in these films similar to the bulk. We determine a magnetic cluster freezing temperature of 36 K, while observing weak ferromagnetism via magnetic hysteresis loops up t…
Epitaxial thin films of Bi2FeCrO6 have been synthesized by pulsed laser deposition on SrRuO3 on (100)- and (111)-oriented SrTiO3 substrates. Detailed X-ray diffraction and cross-section transmission electron microscopy analysis revealed a double perovskite crystal structure of the Bi2FeCrO6 epitaxial films very similar to that of BiFeO3 along with a particularly noteworthy Fe3+/Cr3+ cation ordering along the [111] direction. The films contain no detectable magnetic iron oxide impurities and have the correct cationic average stoichiometry throughout their thickness. They however exhibit a sligh…
In spite of being highly relevant for the development of a new generation of information storage devices, not many single-phase materials displaying magnetic and ferroelectric orders above room temperature are known. Moreover, these uncommon materials typically display insignificant values of the remanent moment in one of the ferroic orders or are complex multicomponent oxides which will be very challenging to integrate in devices. Here we report on the strategy to stabilize the metastable epsilon-Fe2O3 in thin film form, and we show that besides its already known ferrimagnetic nature, the fil…
We report first-principles calculations for one of the few materials that is believed to be a ferroelectric ferromagnet, Bi$_2$NiMnO$_6$. Our calculations show that, contrary to what it has been reported so far, bulk Bi$_2$NiMnO$_6$ does not have a polarization. Instead, like BiMnO$_3$, it crystallizes into a centrosymmetric structure with space group $C2/c$. We also predict that Bi$_2$NiMnO$_6$ will indeed be a ferroelectric ferromagnet if it is grown as an epitaxial film on a substrate with in-plane square symmetry and a lattice constant around 4~Å, such as BaTiO$_3$ or PbZr$_{1-x}$Ti$_{x}$O…
We report on the growth of epitaxial bilayers of the La2/3Sr1/3MnO3 (LSMO) half-metallic ferromagnet and the BiFeO3 (BFO) multiferroic, on SrTiO3(001) by pulsed laser deposition. The growth mode of both layers is two-dimensional, which results in unit-cell smooth surfaces. We show that both materials keep their properties inside the heterostructures, i.e. the LSMO layer (11 nm thick) is ferromagnetic with a Curie temperature of ~330K, while the BFO films shows ferroelectricity down to very low thicknesses (5 nm). Conductive-tip atomic force microscope mappings of BFO/LSMO bilayers for differen…
Multiferroic materials open up the possibility to design novel functionality in electronic devices, with low energy consumption. However, there are very few materials that show multiferroicity at room temperature, which is essential to be practically useful. AlxFe2-xO3 (x-AFO) thin films, belonging to the k-Al2O3 family are interesting because they show room temperature ferrimagnetism and have a polar crystal structure. However, it is difficult to realise its ferroelectric properties at room temperature, due to low resistivity of the films. In this work, we have deposited x-AFO (0.5 <= x <= 1)…
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…
Infrared reflectance spectra of an epitaxial Bi2FeCrO6 thin film prepared by pulsed laser deposition on LaAlO3 substrate were recorded between 10 and 900 K. No evidence for a phase transition to the paraelectric phase was observed, but some phonon anomalies were revealed near 600 K. Most of the polar modes exhibit only a gradual softening, which results in a continuous increase of the static permittivity on heating. It indicates that the ferroelectric phase transition should occur somewhere above 900 K. Magnetic measurements performed up to 1000 K, revealed a possible magnetic phase transition…
The recent study of oxides led to the discovery of several new fascinating physical phenomena. High-temperature superconductivity, colossal magnetoresistance, dilute magnetic doping, or multiferroicity were discovered and investigated in transition-metal oxides, representing a prototype class of strongly correlated electronic systems. This development was accompanied by an enormous progress regarding thin film fabrication. Within the past two decades, epitaxial thin films with crystalline quality approaching semiconductor standards became available using laser molecular beam epitaxy. This evol…
Refrigeration systems based on compression of greenhouse gases are environmentally threatening and cannot be scaled down to on-chip dimensions. In the vicinity of a phase transition caloric materials present large thermal responses to external fields, which makes them promising for developing alternative solid-state cooling devices. Electrocaloric effects are particularly well-suited for portable refrigeration applications; however, most electrocaloric materials operate best at non-ambient temperatures or require the application of large electric fields. Here, we predict that modest electric f…
Experimental results on Bi2FeCrO6 (BFCO) epitaxial films deposited by laser ablation on SrTiO3 substrates are presented. It has been theoretically predicted using first-principles density functional theory that BFCO is ferrimagnetic (with a magnetic moment of 2muB per formula unit) and ferroelectric (with a polarization of ~80 microC/cm2 at 0K). The crystal structure investigated using X-ray diffraction shows that the films are epitaxial with a high degree of crystallinity. Chemical analysis carried out by X-ray Microanalysis and X-ray Photoelectron Spectroscopy indicates the correct cationic …
Oxygen vacancies (VOs) effects on magnetic ordering in Eu0.5Ba0.5TiO3-δ (EBTO3-δ) thin films have been investigated using a combination of experimental measurements and first-principles density-functional calculations. Two kinds of EBTO3-δthin films with different oxygen deficiency have been fabricated. A nuclear resonance backscattering spectrometry technique has been used to quantitatively measure contents of the VOs. Eu0.5Ba0.5TiO3 ceramics have been known to exhibit ferroelectric (FE) and G-type antiferromagnetic (AFM) properties. While, a ferromagnetic (FM) behavior with a Curie temperatu…
We have made magnetization and x-ray diffraction measurements on an epitaxial Pb(Fe1/2Nb1/2)O3 200 nm film. From the temperature dependence of the out-of-plane lattice parameter we can assign a Burns' temperature at Td ~ 640 K, a temperature at T* ~ 510 K, related to the appearance of static polar nanoregions, and an anomaly occurring at 200 K. The latter is precisely the Néel temperature TN determined from magnetization and points to spin-lattice coupling at TN ~ 200 K. We also observe "weak ferromagnetism" up to 300K and propose superantiferromagnetic clusters as a plausible scenario to expl…
Double perovskites provide a unique opportunity to induce and control multiferroic behaviors in oxide systems. The appealing possibility to design materials with a strong coupling between the magnetization and the polarization fields may be achieved in this family since these magnetic insulators can present structural self-ordering in the appropriate growth conditions. We have studied the functional properties of La2CoMnO6 and Bi2CoMnO6 epitaxial thin films grown by pulsed laser deposition. Cation-ordered La2CoMnO6 films display a magnetic Curie temperature of 250 K while cation-disordered Bi2…
We report on the spin-Hall magnetoresistance (SMR) and spin Seebeck effect (SSE) in multiferroic CoCr2O4 (CCO) spinel thin films with Pt contacts. We observe a large enhancement of both signals below the spin-spiral (Ts = 28 K) and the spin lock-in transitions (T_{lock_in} = 14 K). The SMR and SSE response in the spin lock-in phase are one order of magnitude larger than those observed at the ferrimagnetic transition temperature (Tc = 94 K), which indicates that the interaction between spins at the Pt|CCO interface is more efficient in the non-collinear magnetic state below Ts and T_{lock-in}. …
Structural, electronic and dielectric properties of high-quality ultrathin BaTiO3 films are investigated. The films, which are grown by ozone-assisted molecular beam epitaxy on Nb-doped SrTiO3 (001) substrates and having thicknesses as thin 8 unit cells (3.2 nm), are unreconstructed and atomically smooth with large crystalline terraces. A strain-driven transition to 3D island formation is observed for films of of 13 unit cells thickness (5.2 nm). The high structural quality of the surfaces, together with the dielectric properties similar to bulk BaTiO3 and dominantly TiO2 surface termination, …
Domains in BaTiO$_3$ induces a regular modulation of uniaxial magnetic anisotropy in CoFeB via an inverse magnetostriction effect. As a result, the domain structures of the CoFeB wedge film and BaTiO$_3$ substrate correlate fully and straight ferroelectric domain boundaries in BaTiO$_3$ pin magnetic domain walls in CoFeB. We use x-ray photoemission electron microscopy and magneto-optical Kerr effect microscopy to characterize the spin structure of the pinned domain walls. In a rotating magnetic field, abrupt and reversible transitions between two domain wall types occur, namely, narrow walls w…
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 …
Magnetoelectric coupling in multiferroic heterostructures can produce large lateral modulations of magnetic anisotropy enabling the imprinting of ferroelectric domains into ferromagnetic films. Exchange and magnetostatic interactions within ferromagnetic films oppose the formation of such domains. Using micromagnetic simulations and a 1-D model, we demonstrate that competing energies lead to the breakdown of domain pattern transfer below a critical domain width. Moreover, rotation of the magnetic field results in abrupt transitions between two scaling regimes with different magnetic anisotropy…
We present here experimental results obtained on Bi2FeCrO6 (BFCO) epitaxial films deposited by laser ablation directly on SrTiO3 substrates. It has been theoretically predicted, by Baettig and Spaldin, using first-principles density functional theory that BFCO is ferrimagnetic (with a magnetic moment of 2 Bohr magneton per formula unit) and ferroelectric (with a polarization of ~80 microC/cm2 at 0K). The crystal structure has been investigated using X-ray diffraction which shows that the films are epitaxial with a high crystallinity and have a degree of orientation depending of the deposition …
Understanding the polarization switching mechanisms at play in ferroelectric materials is crucial for their exploitation in electronic devices. The conventional centrosymmetric reference structure-based mechanism which accounts for ferroelectricity in most of the usual displacive ferroelectric materials is too energy-demanding for some newly diagnosed ferroelectric materials such as the Ga2-xFexO3 (0.8 < x < 1.4) compounds. Some alternative theoretical propositions have been made and need experimental confirmation. A dual-scale electron microscopy study is performed on thin films of the Ga0.6F…
Deterministic polarization reversal in ferroelectric and multiferroic films is critical for their exploitation in nanoelectronic devices. While ferroelectricity has been studied for nearly a century, major discrepancies in the reported values of coercive fields and saturation polarization persist in literature for many materials. This raises questions about the atomic-scale mechanisms behind polarization reversal. Unconventional ferroelectric switching in $ε$-Fe2O3 films, a material that combines ferrimagnetism and ferroelectricity at room temperature, is reported here. High-resolution in-situ…
We fabricated epitaxial thin films of hexagonal DyMnO3, which otherwise form in a bulk perovskite structure, via deposition on Pt(111)//Al2O3 (0001) and YSZ(111) substrates: each of which has in-plane hexagonal symmetry. The polarization hysteresis loop demonstrated the existence of ferroelectricity in our hexagonal DyMnO3 films at least below 70 K. The observed 2.2 uC/cm^2 remnant polarization at 25 K corresponded to a polarization enhancement by a factor of 10 compared to that of the bulk orthorhombic DyMnO3. Interestingly, this system showed an antiferroelectric-like feature in its hysteres…
