A rapidly developing field of spintronics is based on the premise that substituting charge with spin as a carrier of information can lead to new devices with lower power consumption, non-volatility and high operational speed. Despite efficient magnetization detection, magnetization manipulation is primarily performed by current-generated local magnetic fields and is very inefficient. Here we report a novel non-volatile hybrid multiferroic memory cell with electrostatic control of magnetization based on strain-coupled GaMnAs ferromagnetic semiconductor and a piezoelectric material. We use the crystalline anisotropy of GaMnAs to store information in the orientation of the magnetization along one of the two easy axes, which is monitored via transverse anisotropic magnetoresistance. The magnetization orientation is switched by applying voltage to the piezoelectric material and tuning magnetic anisotropy of GaMnAs via the resulting stress field.
Extrinsic multiferroic hybrid structures consisting of ferromagnetic and ferroelectric layers elastically coupled to each other are promising due to their robust magnetoelectric effects even at room temperature. For a quantitative analysis of these magnetoelectric effects, a detailed knowledge of the piezoelectric and magnetoelastic behavior of both constituents as well as their mutual elastic coupling is mandatory. We here report on a theoretical and experimental study of the magnetic behavior of BaTiO3-based extrinsic multiferroic structures. An excellent agreement between molecular dynamics…
We have investigated the magnetic properties of a piezoelectric actuator/ferromagnetic semiconductor hybrid structure. Using a GaMnAs epilayer as the ferromagnetic semiconductor and applying the piezo-stress along its [110] direction, we quantify the magnetic anisotropy as a function of the voltage V_p applied to the piezoelectric actuator using anisotropic magnetoresistance techniques. We find that the easy axis of the strain-induced uniaxial magnetic anisotropy contribution can be inverted from the [110] to the [1-10] direction via the application of appropriate voltages V_p. At T=5K the mag…
We demonstrate efficient spin-polarized tunneling between a ferromagnetic metal and a ferromagnetic semiconductor with highly mismatched conductivities. This is indicated by a large tunneling magnetoresistance (up to 30%) at low temperatures in epitaxial magnetic tunnel junctions composed of a ferromagnetic metal (MnAs) and a ferromagnetic semiconductor (GaMnAs) separated by a nonmagnetic semiconductor (AlAs). Analysis of the current-voltage characteristics yields detailed information about the asymmetric tunnel barrier. The low temperature conductance-voltage characteristics show a zero bias …
Spintronics has attracted wide attention by promising novel functionalities derived from both the electron charge and spin. While branching into new areas and creating new themes over the past years, the principal goals remain the spin and magnetic control of the electrical properties, essentially the I-V characteristics, and vice versa. There are great challenges ahead to meet these goals. One challenge is to find niche applications for ferromagnetic semiconductors, such as GaMnAs. Another is to develop further the science of hybrid ferromagnetic metal/semiconductor heterostructures, as alter…
The electronic structure of the new diluted magnetic semiconductor Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$ ($x=0.30$, $y=0.15$) in single crystal form has been investigated by angle-resolved photoemission spectroscopy (ARPES). %High density of states of nondispersive bands composed of the Zn $3d$ orbitals are observed with ultraviolet incident light. Measurements with soft x-rays clarify the host valence-band electronic structure primarily composed of the As $4p$ states. Two hole pockets around the $Γ$ point, a hole corrugated cylinder surrounding the $Γ$ and Z points, and an elect…
We report on magnetization precession induced in (Ga,Mn)As by an optical spin transfer torque (OSTT). This phenomenon, which corresponds to a transfer of angular momentum from optically-injected spin-polarized electrons to magnetization, was predicted theoretically in 2004 and observed experimentally by our group in 2012. In this paper we provide experimental details about the observation of OSTT by a time-resolved pump-and-probe magneto-optical technique. In particular, we show that the precession of magnetization due to OSTT can be experimentally separated from that induced by the well known…
University of Wollongong（伍伦贡大学）；Singapore University of Technology and Design（新加坡科技设计大学）；Tiangong University（天津工业大学）；The Hong Kong Polytechnic University（香港理工大学）
By using polarized inelastic neutron scattering measurements, we show that the spin-lattice quantum entanglement in mutliferroics results in hybrid elementary excitations, involving spin and lattice degrees of freedom. These excitations can be considered as multiferroic Godstone modes. We argue that the Dzyaloshinskii-Moriya interaction could be at the origin of this hybridization.
An investigation of the spatially resolved distribution of domains in the multiferroic phase of MnWO$_4$ reveals that characteristic features of magnetic and ferroelectric domains are inseparably entangled. Consequently, the concept of "multiferroic hybrid domains" is introduced for compounds in which ferroelectricity is induced by magnetic order. The three-dimensional structure of the domains is resolved. Annealing cycles reveal a topological memory effect that goes beyond previously reported memory effects and allows one to reconstruct the entire multiferroic multidomain structure subsequent…
We present a detailed study of the structural, electronic, magnetic and ferroelectric properties of prototypical \textit{proper} and \textit{improper} multiferroic (MF) systems such as BiFeO$_{3}$ and orthorhombic HoMnO$_{3}$, respectively, within density functional theory (DFT) and using the Heyd-Scuseria-Ernzerhof hybrid functional (HSE). By comparing our results with available experimental data as well as with state-of-the-art GW calculations, we show that the HSE formalism is able to account well for the relevant properties of these compounds and it emerges as an accurate tool for predicti…
There is great interest in hybrid organic-inorganic materials such as metal-organic frameworks (MOFs). The compounds [C(NH$_{2}$)$_{3}$]M(HCOO)$_{3}$, where M=Cu$^{2+}$ or Cr$^{2+}$ are Jahn-Teller (JT) active ions, are MOF with perovskite topology which crystallizes in polar space group Pna2$_{1}$. In inorganic compounds, octahedral tilting and Jahn-Teller structural distortions are usually non-polar distortions. However, in this MOF cooperative interactions between the antiferro-distortive distortions of the framework and the C(NH2)$_{3}$ organic cation via hydrogen bonding breaks the invers…
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 …
We demonstrate that ethylammonium copper chloride, (C2H5NH3)2CuCl4, a member of the hybrid perovskite family is an electrically polar and magnetic compound with dielectric anomaly around the Curie point (247 K). We have found large spontaneous electric polarization below this point accompanied with a color change in the sample. The system is also ferroelectric, with large remnant polarization (37μC/cm2) that is comparable to classical ferroelectric compounds. The results are ascribed to hydrogen-bond ordering of the organic chains. The coexistence of ferroelectricity and dominant ferromagnetic…
By performing accurate ab-initio density functional theory calculations, we study the role of $4f$ electrons in stabilizing the magnetic-field-induced ferroelectric state of DyFeO$_{3}$. We confirm that the ferroelectric polarization is driven by an exchange-strictive mechanism, working between adjacent spin-polarized Fe and Dy layers, as suggested by Y. Tokunaga [Phys. Rev. Lett, \textbf{101}, 097205 (2008)]. A careful electronic structure analysis suggests that coupling between Dy and Fe spin sublattices is mediated by Dy-$d$ and O-$2p$ hybridization. Our results are robust with respect to t…
Neutron spherical polarimetry, which is directly sensitive to the absolute magnetic configuration and domain population, has been used in this work to unambiguously prove the multiferroicity of (ND4)2[FeCl5(D2O)]. We demonstrate that the application of an electric field upon cooling results in the stabilization of a single-cycloidal magnetic domain below 6.9 K, while poling in the opposite electric field direction produces the full population of the domain with opposite magnetic chirality. We prove the complete switchability of the magnetic domains at low temperature by the applied electric fi…
Nowdays, multiferroic materials with magnetoelectric coupling have many real-world applications in the fields of novel memory devices. It is challenging is to create multiferroic materials with strongly coupled ferroelectric and ferrimagnetic orderings at room temperature. The single crystal of ferric selenide (Fe3Se4) shows type-II multiferroic due to the coexistence of ferroelectric as well as magnetic ordering at room temperature. We have investigated the lattice instability, electronic structure, ferroelectric, ferrimagnetic ordering and transport properties of ferroelectric metal Fe3Se4. …
Tunneling magnetoresistance (TMR) via oxides or molecules includes fruitful physics, such as spin filtering and hybridized interface states, in addition to various practical applications using large TMR ratio at room temperature. Then, a larger TMR effect with a new fundamental physics is awaited because further progress on spintronics can be realized. Here we report a discovery of a gigantic TMR ratio of 1,400,000% in a C60-Co nanocomposite spin device. The observed effect is induced by a combination of a Coulomb blockade effect and a novel magnetic switching effect. Theoretical investigation…
Within the broad class of multiferroics (compounds showing a coexistence of magnetism and ferroelectricity), we focus on the subclass of "improper electronic ferroelectrics", i.e. correlated materials where electronic degrees of freedom (such as spin, charge or orbital) drive ferroelectricity. In particular, in spin-induced ferroelectrics, there is not only a {\em coexistence} of the two intriguing magnetic and dipolar orders; rather, there is such an intimate link that one drives the other, suggesting a giant magnetoelectric coupling. Via first-principles approaches based on density functiona…
Colossal Type-II Multiferroic Polarization Driven by Collinear Spin Orders
Nanjing University of Science and Technology（南京理工大学）；School of Physics, Nanjing University（南京大学物理学院）；Collaborative Innovation Center of Advanced Microstructures, Nanjing University（南京大学先进微结构协同创新中心）；Hefei National Laboratory（合肥国家实验室）；Jiangsu Physical Science Research Center, Nanjing University（南京大学江苏省物理科学研究中心）
Multiferroics, materials where spontaneous long-range magnetic and dipolar orders coexist, represent an attractive class of compounds, which combine rich and fascinating fundamental physics with a technologically appealing potential for applications in the general area of spintronics. Ab-initio calculations have significantly contributed to recent progress in this area, by elucidating different mechanisms for multiferroicity and providing essential information on various compounds where these effects are manifestly at play. In particular, here we present examples of density-functional theory i…
Our results describe an unprecedented example of change in the mechanism of magnetically-induced electric polarization from spin current to spin-dependent p-d hybridization model. We have followed the evolution of the magnetic structures of (ND4)2[FeCl5 D2O] compound using single crystal neutron diffraction under external magnetic field. The spin arrangements change from incommensurate cycloidal to commensurate distorted-cycloidal and finally to quasi-collinear. The determination of the magnetic structures allows us to explain the observed electric polarization in the different ferroelectric p…
Structural, impedance, ferroelectric and magnetic properties were examined in multiferroic Bi_{2}Fe_{4(1-x)}Co_{4x}O_{9} (0$\leq$x$\leq$0.02) ceramics synthesized via solid-state reaction method. X-ray diffraction analysis and Rietveld refinement showed secondary phase formation (for x$\geq$0.01) which was subsequently confirmed from room temperature Raman spectroscopy study. The frequency dependence of impedance and electric modulus of the material showed the presence of non-Debye type relaxation in all the samples. The values of the activation energies calculated from imaginary impedance and…
We present spin transport studies on a low-field, room-temperature magnetoelectric multiferroic polycrystalline $\text{Sr}_{3}\text{Co}_{2}\text{Fe}_{24}\text{O}_{41}$ (SCFO)|Pt heterostructure wherein a highly tunable transverse conical magnetic phase is responsible for static and dynamic magnetoelectric coupling. We measured angular dependence of spin Hall magnetoresistance (SMR) at constant magnetic fields ($H$) in the range of 50 to 100 kOe. Application of field below the critical value (2.5 kOe), yielded negative SMR and the $H$-evolution of normalized SMR exhibited a negative gradient. F…
We study the dynamical interplay between ferroelectricity and magnetism in a multiferroic with a helical magnetic order. We show that the dynamical exchange-striction induces a biquadratic interaction between the spins and transverse phonons resulting in quantum fluctuations of the spontaneous ferroelectric polarization $\mathbf{P}$ in the ferroelectric phase. The hybridization between the spin wave and the fluctuation of the electric polarization leads to low-lying transverse phonon modes. Those are perpendicular to $\mathbf{P}$ and to the helical spins at small wave vector but then turn para…
The coexisting magnetic and ferroelectric orders in multiferroic materials give rise to a handful of novel magnetoelectric phenomena, such as the absorption difference for the opposite propagation directions of light called the non-reciprocal directional dichroism (NDD). Usually these effects are restricted to low temperature, where the multiferroic phase develops. In this paper we report the observation of NDD in the paramagnetic phase of Sr2CoSi2O7 up to temperatures more than ten times higher than its Néel temperature (7 K) and in fields up to 30 T. The magnetically induced polarization and…
The idea of embedding and transmitting information within the fluctuations of the magnetic moments of spins (spin waves) has been recently proposed and experimentally tested. The coherence of spin waves, which describes how well defined these excitations are, is of course vital to this process, and themost significant factor that affects the spin-wave coherence is temperature. Here we present neutron inelastic scattering measurements of the full threedimensional spin-wave dispersion in BiFeO3, which is one of the most promising functional multiferroic material, for temperatures from 5K to 700K…
Ba2CoGe2O7, crystallizing in the noncentrosymmetric but nonpolar structure, belongs to a special class of multiferroic materials, whose properties are predetermined by the rotoinversion symmetry. Unlike inversion, the rotoinversion symmetry can be easily destroyed by the magnetization. Moreover, due to specific structural pattern, the magnetic structure of Ba2CoGe2O7 is relatively soft. Altogether, this leads to the rich variety of multiferroic properties, where the magnetic structure can be easily deformed by the magnetic field, inducing the electric polarization in the direction, which depen…
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…
Ab initio calculations of the electric polarization of correlation-driven insulating materials, namely Mott insulators, have not been possible so far. Using a combination of density functional theory and dynamical-mean-field theory we study the electric polarization of the Mott insulator Sr$_{0.5}$Ba$_{0.5}$MnO$_{3}$. We predict a ferroelectric polarization of $\simeq 16.5 μC/cm^2$ in the high temperature paramagnetic phase and recover the measured value of $\simeq 13.3 μC/cm^2$ in the low temperature antiferromagnetic phase. Our calculations reveal that the driving force for the ferroelectric…
Searching for new functionality in next generation electronic devices is a principal driver of material physics research. Multiferroics simultaneously exhibit electric and magnetic order parameters that may be coupled through magnetoelectric (ME) effects. In single-phase materials the ME effect arises from one of three known mechanisms: inverse Dzyaloshinskii-Moriya (IDM) interaction, spin dependent ligand-metal (p-d) orbital hybridization, and exchange striction. However, the coupling among these mechanisms remains largely unexplored despite envisioned potential capabilities. Here, we present…
For broad nanoscale applications, it is crucial to implement more functional properties, especially those ferroic orders, into two-dimensional materials. Here GdI$_3$ is theoretically identified as a honeycomb antiferromagnet with large $4f$ magnetic moment. The intercalation of metal atoms can dope electrons into Gd's $5d$-orbitals, which alters its magnetic state and lead to Peierls transition. Due to the strong electron-phonon coupling, the Peierls transition induces prominent ferroelasticity, making it a multiferroic system. The strain from undirectional stretching can be self-relaxed via …
Metal-organic frameworks (MOFs) possess a hybrid nature, combining the inorganic properties from the metal ions and the organic properties from the molecular linkers. Stroppa, \textit{et al.}, showed that the perovskite-type MOF [C(NH$_2$)$_3$]M[(HCOO)$_3$] (M = Cr, Cu) exhibits the magneto-electric coupled multiferroicity [Angew. Chem. Int. Ed. 50, 5847 (2011) and Adv. Mater. 25, 2284 (2013)]. Moreover, their ferroelectricity arises from the hybrid improper mechanism, which also explains the magneto-electric coupling. In this work, we further examine the electric and magnetic properties of [C…
Hybrid systems coupling quantum spin defects (QSD) and magnons can enable unique spintronic device functionalities and probes for magnetism. Here, we add electric field control of magnon-QSD coupling to such systems by integrating ferromagnet-ferroelectric multiferroic with nitrogen-vacancy (NV) center spins. Combining quantum relaxometry with ferromagnetic resonance measurements and analytical modeling, we reveal that the observed electric-field tuning results from ferroelectric polarization control of the magnon-generated fields at the NV. Exploiting the demonstrated control, we also propose…
Titanates with the perovskite structure, including ferroelectrics (e.g., BaTiO$_3$) and ferromagnetic ones (e.g., YTiO$_3$), are important functional materials. Recent theoretical studies predicted multiferroic states in strained EuTiO$_3$ and titanate superlattices, the former of which has already been experimental confirmed. Here, a first-principles calculation is performed to investigate the structural, magnetic, and electronic properties of Y half-substituted LaTiO3. Our results reveal that the magnetism of Y$_{0.5}$La$_{0.5}$TiO$_3$ sensitively depends on its structural details because of…
Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material, CoCr$_2$O$_4$, is a particularly interesting example of a multiferroic material, because evidence for magnetoelectric behavior in the ferrimagnetic phase seems to conflict with traditional noncollinear-spin-driven mechanisms for inducing a macroscopic polarization. This paper repo…
The research on multiferrocity and magnetoelectric coupling in metal-organic system is rare. Very few hybrid organic-inorganic frameworks (HOIF) exhibit direct magnetoelectric coupling (coupling between spins and dipoles) and also restricted to particular COOH-based system. We show how one can design a hybrid system to obtain such coupling based on the rational design of the organic ligands. The layered phosphonate, MnO3PC6H5.H2O, consisting of perovskite layers stacked with organic phenyl layers, is used as a starting potential candidate. To introduce dipole moment, a closely related metal-ph…
The interactions between elementary excitations such as phonons, plasmons, magnons, or particle-hole pairs, drive emergent functionalities and electronic instabilities such as multiferroic behaviour, anomalous thermoelectric properties, polar order, or superconductivity. Whereas various hybrid excitations have been studied extensively, the feed-back of prototypical elementary excitations on the crystal electric fields (CEF), defining the environment in which the elementary excitations arise, has been explored for very strong coupling only. We report high-resolution neutron spectroscopy and ab-…
The spin-driven component of electric polarization in a single crystal of multiferroic BiFeO$_{3}$ was experimentally investigated in pulsed high magnetic fields up to 41 T. Sequential measurements of electric polarization for various magnetic field directions provide clear evidence of electric polarization normal to the hexagonal $c$ axis (${\bf P}_{\rm t}$) in not only the cycloidal phase, but also the field-induced canted antiferromagnetic phase. The direction of ${\bf P}_{\rm t}$ is directly coupled with the ferromagnetic moment in the canted antiferromagnetic phase, and thus controlled by…
Hybridization of semiconducting and magnetic materials into a single heterostructure is believed to be potentially applicable to the design of novel functional spintronic devices. In the present work we report epitaxial stabilization of four magnetically ordered iron oxide phases (Fe3O4, γ-Fe2O3, α-Fe2O3 and most exotic metastable ε-Fe2O3) in the form of nanometer sized single crystalline films on GaN(0001) surface. The epitaxial growth of as many as four distinctly different iron oxide phases is demonstrated within the same single-target Laser MBE technological process on a GaN semiconductor …
Electric field controlled spin transport in a topological insulator interfaced with a ferroelectric antiferromagnet
Materials Science Division, Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室材料科学部）；Department of Materials Science and Engineering, University of California, Berkeley（加州大学伯克利分校材料科学与工程系）；Rice Advanced Materials Institute, Rice University（莱斯大学莱斯先进材料研究所）；Department of Materials Science and Engineering, Cornell University（康奈尔大学材料科学与工程系）；Department of Physics, University of California, Berkeley（加州大学伯克利分校物理系）；Kavli Institute at Cornell for Nanoscale Science, Cornell University（康奈尔大学卡弗里纳米科学研究所）；Leibniz-Institut für Kristallzüchtung（莱布尼兹晶体生长研究所）
