We present a theoretical study of the onset of electric polarization close to a surface in magnetic materials and in thin films and multilayers. We consider two different paths that lead to the onset of multiferroic behavior at the boundary in materials that are bulk collinear ferromagnets or antiferromagnets. These two paths are distinguished by the presence or absence of a surface induced Dzyaloshinskii-Moriya interaction which can be taken into account through Lifshitz invariants in the free energy of the system. Experimental consequences are discussed in the light of the developed theory.
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.…
Room-temperature magnetoelectric multiferroicity has been observed in c-axis oriented GaFeO$_3$ thin films (space group $Pna2_1$), grown on economic and technologically important (100)Si substrates by pulsed laser deposition technique. Structural analysis and comprehensive mapping of Ga:Fe ratio across a length scale range of 10$^4$ reveal coexistence of epitaxial and chemical strain. It induces formation of finer magnetic domains and large magnetoelectric coupling - decrease in remanent polarization by $\sim$21\% under $\sim$50 kOe. Magnetic force microscopy reveals presence of both finer ($<…
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…
The observation of ferroelectric, ferromagnetic and ferroelastic phases in thin films of binary oxides attract the broad interest of scientists and engineers. However, the theoretical consideration of observed behaviour physical nature was performed mainly for HfO2 thin films from the first principles, and in the framework of Landau-Ginzburg-Devonshire (LGD) phenomenological approach with a special attention to the role of oxygen vacancies in both cases. Allowing for generality of the LGD theory we applied it to the group of binary oxides in this work. The calculations have been performed in t…
Two-dimensional (2D) multiferroics are key candidate materials towards advancement of smart technology. Here, we employed a simple synthesis approach to address the long-awaited dream of developing ferroelectric and multiferroic 2D materials, specially in the new class of materials called MXenes. The etched Ti$_3$C$_2$T$_x$ MXene was first synthesized after HF-treatment followed by delamination process for successful synthesis of free-standing Ti$_3$C$_2$T$_x$ film. The free-standing film was then exposed to air at room-temperature as well as heated at different temperature to form TiO$_2$ lay…
Multiferroicity in the two-dimensional limit in hexagonal LuFeO3 films
Fudan University（复旦大学）；University of Science and Technology Beijing（北京科技大学）；Brookhaven National Laboratory（布鲁克海文国家实验室）；Hefei National Laboratory（合肥国家实验室）；Shanghai Research Center for Quantum Sciences（上海量子科学研究中心）；Zhangjiang Fudan International Innovation Center（张江复旦国际创新中心）；University of Nebraska, Lincoln（内布拉斯加大学林肯分校）
Strain-Induced Relaxor Multiferroicity at Room Temperature in Hexaferrite BaFe12O19 Thin Films
Cornell University（康奈尔大学）；The Pennsylvania State University（宾夕法尼亚州立大学）；Leibniz-Institut für Kristallzüchtung（莱布尼兹晶体生长研究所）；Oak Ridge National Laboratory（橡树岭国家实验室）；University of Tennessee（田纳西大学）；University of California, Berkeley（加州大学伯克利分校）；University of North Texas（北德克萨斯大学）；University of Southern California（南加州大学）；Kavli Institute at Cornell for Nanoscale Science（康奈尔纳米科学卡弗里研究所）
We report observation of surface-defect-induced room temperature multiferroicity - surface ferromagnetism ($M_S$ at 50 kOe $\sim$0.005 emu/g), ferroelectricity ($P_R$ $\sim$2 nC/cm$^2$), and significantly large magnetoelectric coupling (decrease in $P_R$ by $\sim$80\% under $\sim$15 kOe field) - in nanorods (diameter $\sim$100 nm) of double perovskite Y$_2$NiMnO$_6$ compound. In bulk form, this system exhibits multiferroicity only below its magnetic transition temperature $T_N$ $\approx$ 70 K. On the other hand, the oxygen vacancies, formed at the surface region (thickness $\sim$10 nm) of the …
Skyrmions are nanoscale spin configurations with topological properties that hold great promise for spintronic devices. Here, we establish their Néel texture, helicity, and size in Ir/Fe/Co/Pt multilayer films by constructing a multipole expansion to model their stray field signatures and applying it to magnetic force microscopy (MFM) images. Furthermore, the demonstrated sensitivity to inhomogeneity in skyrmion properties, coupled with a unique capability to estimate the pinning force governing dynamics, portends broad applicability in the burgeoning field of topological spin textures.
Sol-gel spin coating technique was employed to synthesize CuO thin films at 1500 rpm, 2200 rpm and 2400 rpm for 30 seconds, and subsequently annealed at 150-550°C for 1 hour. Multi-layered CuO thin films with 3 and 5 layers were prepared. These thin films were characterized using XRD, FTIR and polarizing light microscopy. The XRD and FTIR analysis confirmed the crystallization of CuO phase in thin films annealed above 350 °C, and corresponding crystallite sizes were observed to be increasing with the annealing temperature. The Scherrer formula was applied for (111) and peaks of XRD patterns of…
Ferroelectric films usually have phase states and physical properties very different from those of bulk ferroelectrics. Here we propose free-standing ferroelectric-elastic multilayers as a bridge between these two material systems. Using a nonlinear thermodynamic theory, we determine phase states of such multilayers as a function of temperature, misfit strain, and volume fraction fi of ferroelectric material. The numerical calculations performed for two classical ferroelectrics - PbTiO3 and BaTiO3 - demonstrate that polarization states of multilayers in the limiting cases fi -> 0 and fi -> 1 c…
The anomalous Nernst effect (ANE) has been investigated in alternately-stacked multilayer films comprising paramagnetic and ferromagnetic metals. We found that the ANE is enhanced with increasing the number of the paramagnet/ferromagnet interfaces with keeping the total thickness of the films constant, and that the enhancement appears even in the absence of magnetic proximity effects; similar behavior was observed not only in Pt/Fe multilayers but also in Au/Fe and Cu/Fe multilayers free from proximity ferromagnetism. This universal enhancement of the ANE in the metallic multilayers suggests t…
Competing interactions produce finite-size textures in myriad condensed matter systems, typically forming elongated stripe or round bubble domains. Transitions between stripe and bubble phases, driven by field or temperature, are expected to be reversible in nature. Here we report on the distinct character of the analogous transition for nanoscale spin textures in chiral Co/Pt-based multilayer films, known to host Néel skyrmions, using microscopy, magnetometry, and micromagnetic simulations. Upon increasing field, individual stripes fission into multiple skyrmions, and this transition exhibits…
Magnetic skyrmions form in chiral multilayers from the shrinking or fission of elongated stripe textures. Here we report an experimental and theoretical study of the temperature dependence of this stripe-to-skyrmion transition in Co/Pt-based multilayers. Field-reversal magnetometry and Lorentz microscopy experiments over 100 - 350 K establish the increased efficacy of stripe-to-skyrmion fission at higher temperatures - driven primarily by the thermal evolution of key magnetic interactions - thereby enhancing skyrmion density. Atomistic calculations elucidate that the energy barrier to fission …
Short review on the different models for the electro-thermal 3-omega method. We present the deduction of the fundamental relation between the 3-omega voltage with the temperature rise to determine the thermal conductivity. The usage of the anisotropy of the films allows a smooth transition between 1D and 2D models. A comparison between the multilayer methods and analytical solutions are presented.
In this paper we use density functional theory combined with dynamical mean-field theory (DFT+DMFT) to study interface effects between thin films of the correlated metal CaVO$_3$ and the two typical substrate materials SrTiO$_3$ and LaAlO$_3$. We find that the CaVO$_3$/SrTiO$_3$ interface has only a marginal influence on the CaVO$_3$ thin film, with the dominant effect being the (bulklike) epitaxial strain imposed by the large lattice mismatch, rendering the CaVO$_3$ film insulating due to the enhanced orbital polarization related to the strong level splitting between the t$_{\mathrm{2g}}$ orb…
Oxide thin films exhibit versatile physical properties such as magnetism, ferroelectricity, piezoelectricity, metal-insulator transition (MIT), multiferroicity, colossal magnetoresistivity, switchable resistivity, etc. More importantly, the exhibited multifunctionality could be tuned by various external fields, which has enabled demonstration of novel electronic devices. In this article, recent studies of the multi-fields modulation of physical properties in oxide thin films have been reviewed. Some of the key issues and prospects about this field are also addressed.
Magnetic skyrmions are nanoscale spin structures recently discovered at room temperature (RT) in multilayer films. Employing their novel topological properties towards exciting technological prospects requires a mechanistic understanding of the excitation and relaxation mechanisms governing their stability and dynamics. Here we report on the magnetization dynamics of RT Néel skyrmions in Ir/Fe/Co/Pt multilayer films. We observe a ubiquitous excitation mode in the microwave absorption spectrum, arising from the gyrotropic resonance of topological skyrmions, and robust over a wide range of tempe…
Ag nanorod arrays/dielectrics/mirror-structured multilayer thin-film are well known, highly sensitive surface-enhanced Raman scattering (SERS) substrates that enhance the Raman scattering cross-section by the interference of light. However, extracting biomarkers directly from human skin using these solid substrates is difficult. To overcome this problem, we propose a multilayer thin-film flake dispersion gel by centrifugal mixing of the multilayer thin-film and hydroxyethyl cellulose (HEC) gel. The multilayer thin-film was prepared by serial bideposition using the dynamic oblique angle deposit…
We report on the heteroepitaxial stabilization of YCrO3 ultra-thin films on LSAT (001) substrate. Using a combination of resonant X-ray absorption spectroscopy (XAS) and atomic multiplet cluster calculation, the electronic structure of YCrO3 thin film was investigated. Polarization dependent Cr L3,2 edge XAS measurement reveal the presence of an anomalous orbital polarization uncharacteristic of a 3d3 electronic system. Atomic multiplet calculations demonstrate the critical importance of charge transfer energy, Coulomb correlation strength and hopping interaction in stabilizing this unusual or…
Multifunctional materials composed of ultrathin magnetic films with perpendicular magnetic anisotropy combined with ferroelectric substrates represent a new approach toward low power, fast, high density spintronics. Here we demonstrate Co/Ni multilayered films with tunable saturation magnetization and perpendicular anisotropy grown directly on ferroelectric PZT [Pb(Zr_xTi_1-x)O_3] substrate plates. Electric fields up to +/- 2 MV/m expand the PZT by 0.1% and generate at least 0.02% in-plane compression in the Co/Ni multilayered film. Modifying the strain with a voltage can reduce the coercive f…
We experimentally demonstrate the formation of room-temperature skyrmions with radii of about 25\,nm in easy-plane anisotropy multilayers with interfacial Dzyaloshinskii-Moriya interaction (DMI). We detect the formation of individual magnetic skyrmions by magnetic force microscopy and find that the skyrmions are stable in out-of-plane fields up to about 200 mT. We determine the interlayer exchange coupling as well as the strength of the interfacial DMI. Additionally, we investigate the dynamic microwave spin excitations by broadband magnetic resonance spectroscopy. From the uniform Kittel mode…
Ferromagnet/heavy metal (FM/HM) multilayer thin films with $C_{2v}$ symmetry have the potential to host antiskyrmions and other chiral spin textures via an anisotropic Dzyaloshinkii-Moriya interaction (DMI). Here, we present a candidate material system that also has a strong uniaxial magnetocrystalline anisotropy aligned in the plane of the film. This system is based on a new Co/Pt epitaxial relationship, which is the central focus of this work: hexagonal closed-packed Co$(10\bar{1}0)[0001]$ $\parallel$ face-centered cubic Pt$(110)[001]$. We characterized the crystal structure and magnetic pro…
We report a study of the magnetization reversals and skyrmion configurations in two systems - Pt/Co/MgO and Ir/Fe/Co/Pt multilayers, where magnetic skyrmions are stabilized by a combination of dipolar and Dzyaloshinskii-Moriya interactions (DMI). First Order Reversal Curve (FORC) diagrams of low-DMI Pt/Co/MgO and high-DMI Ir/Fe/Co/Pt exhibit stark differences, which are identified by micromagnetic simulations to be indicative of hybrid and pure Néel skyrmions, respectively. Tracking the evolution of FORC features in multilayers with dipolar interactions and DMI, we find that the negative FORC …
A correlation of structural changes with nanomechanical properties in TiN-AlN multilayer films
Tampere University（坦佩雷大学）；VTT Technical Research Center of Finland（芬兰技术研究中心）；Empa- Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科技与工程研究所）；TU Wien（维也纳工业大学）；École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；Indian Institute of Technology Roorkee（鲁尔基印度理工学院）
Quasiperiodic systems show a universal gap structure due to quasiperiodicity which is analogous to gap openings at the Brillouin zone boundary in periodic systems. The integrated density of states (IDoS) below those energy gaps are characterized by a few integers, which is known as the ``gap labeling theorem'' (GLT) for quasiperiodic systems. In this study, focusing on multilayer thin film systems such as twisted bilayer graphene and stacked transition metal dichalcogenides, we extend the GLT for multilayer systems of arbitrary dimensions and number of layers, using an approach based on the al…
We study the optical transmittance of multilayer graphene films up to 65 layers thick. By combing large-scale tight-binding simulation and optical measurement on CVD multilayer graphene, the optical transmission through graphene films in the visible region is found to be solely determined by the number of graphene layers. We argue that the optical transmittance measurement is more reliable in the determination of the number of layers than the commonly used Raman Spectroscopy. Moreover, optical transmittance measurement can be applied also to other 2D materials with weak van der Waals interlaye…
Interface effects on an ultrathin Co film in multilayers based on the organic semiconductor Alq3
利用原子力显微镜、SQUID磁谱仪和核磁共振（NMR）研究了AlOx阻挡层厚度对Ta/Co/（AlOx）/Alq 3/Si混合结构磁性能和形貌的影响。所有使用的技术都指出，需要2nm的阻挡层厚度来在Alq 3的顶部上获得磁性良好的钴层。59 Co NMR测量结果表明，AlOx阻挡层导致形成具有“缺陷”钴的界面层，有利于具有良好磁性能的“大块”钴的生长。
The irradiation with the 10 ns pulsed infrared Nd:YAG laser was applied to transform FePdCu multilayers into chemically ordered L10 phase. The X-ray diffraction methods (Theta/2Theta scan, psi-scan, omega-scan) were used to trace the presence of L10 phase after laser annealing with different number of pulses. The size and shape of crystallites was determined depending on their orientation with respect to film plane. The (111) oriented crystallites of constituent metals were built as coherent domains spreading through multilayers during deposition of films. Laser annealing induced the transform…
Using wide-band (0.5-6.5 eV) spectroscopic ellipsometry we study ultrathin [Bi(0.6-2.5 nm)-FeNi(0.8,1.2 nm)]N multilayer films grown by rf sputtering deposition, where the FeNi layer has a nanoisland structure and its morphology and magnetic properties change with decreasing the nominal layer thickness. From the multilayer model simulations of the ellipsometric angles, Psi(omega) and Delta(omega), the complex (pseudo)dielectric function spectra of the Bi layer were extracted. The obtained results demonstrate that the Bi layer can possess the surface metallic conductivity, which is strongly aff…
Facing the ever-growing demand for data storage will most probably require a new paradigm. Magnetic skyrmions are anticipated to solve this issue as they are arguably the smallest spin textures in magnetic thin films in nature. We designed cobalt-based multilayered thin films where the cobalt layer is sandwiched between two heavy metals providing additive interfacial Dzyaloshinskii-Moriya interactions, which reach about 2 mJ/m2 in the case of the Ir/Co/Pt multilayers. Using a magnetization-sensitive scanning x-ray transmission microscopy technique, we imaged magnetic bubble-like domains in the…
The spectral signatures of magnetic skyrmions under microwave field excitation are of fundamental interest and can be an asset for high frequency applications. These topological solitons can be tailored in multilayered thin films, but the experimental observation of their spin wave dynamics remains elusive, in particular due to large damping. Here, we study Pt/FeCoB/AlO$_x$ multilayers hosting dense and robust skyrmion lattices at room temperature with Gilbert damping of $\sim 0.02$. We use magnetic force microscopy to characterise their static magnetic phases and broadband ferromagnetic reson…
Superconducting Nb3Sn films can be synthesized by controlling the atomic concentration of Sn. Multilayer sequential sputtering of Nb and Sn thin films followed by high temperature annealing is considered as a method to fabricate Nb3Sn films, where the Sn composition of the deposited films can be controlled by the thickness of alternating Nb and Sn layers. We report on the structural, morphological and superconducting properties of Nb3Sn films fabricated by multilayer sequential sputtering of Nb and Sn films on sapphire substrates followed by annealing at 950 °C for 3 h. We have investigated th…
Thermal stability of nanocrystalline multilayer thin film is of paramount importance as the applications often involve high temperature. Here we report on the layer instability phenomenon in binary polycrystalline thin film initiating from the grain boundary migrations at higher temperatures using phase-field simulations. Effect of layer thickness, bilayer spacing and the absence of grain boundary are also investigated along with the grain boundary mobility of individual phases on the layer stability. Layer instability in the polycrystalline film is shown to arise from the grain boundary groov…
Highly Uniform 300 mm Wafer-Scale Deposition of Single and Multilayered Chemically Derived Graphene Thin Films
报道了在300 mm SiO2/Si晶片上沉积原子级薄、高度均匀的化学衍生石墨烯（CDG）薄膜的方法。我们证明了非常薄的薄膜可以被剥离，形成均匀的膜，而不是可以自立或转移到任何基板上。使用拉曼光谱和原子力显微镜（AFM）的高度分布的厚度的详细地图显示，膜厚度是非常均匀和高度可控的，范围从1-2层到30层。在使用各种方法还原之后，CDG膜是透明的并且与FET器件电活性，从而在约70%透明度下产生约15 cm 2/Vs的异常高的迁移率和约lk欧姆/平方的薄层电阻。
Static and dynamic properties of ferroelectric thin film multilayers
发展了铁电薄膜多层膜的热力学理论。自由能函数使用多层模型写下，其中一种铁电材料的c-畴层与第二铁电材料的a-畴层交替。我们假设界面是完全尖锐的，并且在这些边界处的极化为零。考虑到由于薄膜中的应力和去极化场的自由能系数的重正化，以及极化梯度系数的重正化。平衡非均匀极化温度和它的厚度依赖性确定从Euler-Lagrange方程的自由能泛函的最小化所产生的解决方案。结果表明，存在厚度诱导铁电相变，其相变温度和临界层厚度依赖于畴取向。通过自由能量密度和层厚系数计算并表示了“a/c”、“c/c”和“a/a”畴多层的判据。计算的多层膜的磁化率发散的厚度诱导铁电相的转变温度。这种分歧被证明是在一些多层膜中观察到的巨介电响应的起源。该理论对最近在PbTiO $_{3}$ -Pb $_{1-x}$ La $_{x}$ TiO $_{3}$（$x=0.28$）多层膜中观察到的巨磁化率的温度依赖性给出了很好的拟合。
Under the correct conditions, Dzyaloshinskii-Moriya interactions (DMI) can lead to topologically protected spin textures such as skyrmions. The application of DMI for spin-based computation and memory technologies is promising and requires a detailed consideration of the role intrinsic energies have on stabilizing the diverse textures observed thus far. Here we experimentally investigate the effect of dipolar energy from interlayer coupling on the remanent spin textures found at room temperature for interfacial DMI multilayers of [ Pt \ Co \ Ir ]$_{\times N}$. The total dipolar energy is modif…
Anti-ThCr$_2$Si$_2$ type $RE_2$O$_2$Sb ($RE$ = rare earth) with Sb square net has shown insulating conduction so far. Here we report the synthesis of La$_2$O$_2$Sb epitaxial thin films for the first time by multilayer solid-phase epitaxy. The valence state of Sb was about -2 evaluated from X-ray photoemission spectroscopy measurement, and the indirect band gap of 0.17 eV was observed. The La$_2$O$_2$Sb epitaxial thin film showed unexpectedly high electrical conduction as a narrow gap semiconductor, whose resistivity at room temperature was approximately ten-thousand-fold lower than that of La$…
Multiferroic materials are potential to be applied in novel magnetoelectric devices, for example, high-density non-volatile storage. Last decades, research on multiferroic materials was focused on three-dimensional (3D) materials. However, 3D materials suffer from the dangling bonds and quantum tunneling in the nano-scale thin films. Two-dimensional (2D) materials might provide an elegant solution to these problems, and thus are highly on demand. Using first-principles calculations, we predict ferromagnetism and driven ferroelectricity in the monolayer and even a few-layers of CuCrP2S6. Althou…
There is currently a renewed interest in the development of experimental methods to achieve the elastic characterization of thin films, multilayers and acoustic resonators operating in the GHz range of frequencies. The potentialities of surface Brillouin light scattering (surf-BLS) for this aim are reviewed in this paper, addressing the various situations that may occur for the different types of structures. In particular, the experimental methodology and the amount of information that can be obtained depending on the transparency or opacity of the film material, as well as on the ratio betwee…
