Among the class of strongly-correlated oxides, La1-xSrxMnO3 $-$ a half metallic ferromagnet with a Curie temperature above room temperature $-$ has sparked a huge interest as a functional building block for memory storage and spintronic applications. In this respect, defect engineering has been in the focus of a long-standing quest for fabricating LSMO thin films with highest quality in terms of both structural and magnetic properties. Here, we discuss the correlation between structural defects, such as oxygen vacancies and impurity islands, and magnetism in La0.74Sr0.26MnO3/SrTiO3 (LSMO/STO) epitaxial heterostructures by systematic control of the growth temperature and post-deposition annealing conditions. Upon increasing the growth temperature within the 500 $-$ 700 $^{\circ}$C range, the epitaxial LSMO films experience a progressive improvement in oxygen stoichiometry, leading to enhanced magnetic characteristics. Concurrently, however, the use of a high growth temperature triggers the diffusion of impurities from the bulk of STO, which cause the creation of off-stoichiometric, dendritic-like SrMoOx islands at the film/substrate interface. As a valuable workaround, post-deposition annealing of the LSMO films grown at a relatively-low temperature of about 500 $^{\circ}$C permits to obtain high-quality epitaxy, atomically-flat surface as well as a sharp magnetic transition above room temperature and robust ferromagnetism. Furthermore, under such optimized fabrication conditions possible scenarios for the formation of the magnetic dead layer as a function of LSMO film thickness are discussed. Our findings offer effective routes to finely tailor the complex interplay between structural and magnetic properties of LSMO thin films via temperature-controlled defect engineering.
We report on a strain-induced martensitic transformation, accompanied by a suppression of magnetic order in epitaxial films of chemically disordered FeRh. X-ray diffraction, transmission electron microscopy and electronic structure calculations reveal that the lowering of symmetry (from cubic to tetragonal) imposed by the epitaxial relation leads to a further, unexpected, tetragonal-to-orthorhombic transition, triggered by a band-Jahn-Teller-type lattice instability. The collapse of magnetic order is a direct consequence of this structural change, which upsets the subtle balance between ferrom…
There has been renewed interest in the use of magnetic nanoparticles to convert high frequency electromagnetic energy into heat. During the last decade, numerous examples in the field of catalysis, lightweight thermoplastic composites for aeronautical and automotive engineering, and biomedical applications as well, have flourished. In a recent Letter "Ultrathin Interface Regime of Core-Shell Magnetic Nanoparticles for Effective Magnetism Tailoring", Moon et al. DOI: 10.1021/acs.nanolett.6b04016 claim to have observed a new interface spin canting phenomenon in core-shell ferrrites that pushes h…
Ferroelectric BaTiO3 films with large polarization have been integrated with Si(001) by pulsed laser deposition. High quality c-oriented epitaxial films are obtained in a substrate temperature range of about 300 deg C wide. The deposition temperature critically affects the growth kinetics and thermodynamics balance, resulting on a high impact in the strain of the BaTiO3 polar axis, which can exceed 2% in films thicker than 100 nm. The ferroelectric polarization scales with the strain and therefore deposition temperature can be used as an efficient tool to tailor ferroelectric polarization. The…
We investigate the growth of the graphene buffer layer and the involved step bunching behavior of the silicon carbide substrate surface using atomic force microscopy. The formation of local buffer layer domains are identified to be the origin of undesirably high step edges in excellent agreement with the predictions of a general model of step dynamics. The applied polymer-assisted sublimation growth method demonstrates that the key principle to suppress this behavior is the uniform nucleation of the buffer layer. In this way, the silicon carbide surface is stabilized such that ultra-flat surfa…
Interest for layered Ruddlesden-Popper strongly correlated manganites of Pr$_{0.5}$Ca$_{1.5}$MnO$_4$ as well as to their thin film polymorphs is motivated by the high temperature of charge orbital ordering above room temperature. We report on the tailoring of the c-axis orientation in epitaxial RP-PCMO films grown on SrTiO$_3$ (STO) substrates with different orientations as well as the use of CaMnO$_3$ (CMO) buffer layers. Films on STO(110) reveal in-plane alignment of the c-axis lying along to the [100] direction. On STO(100), two possible directions of the in-plane c-axis lead to a mosaic li…
We demonstrate control of the magnetism of Pd(100) ultrathin films, which show d-electron quantum-well induced ferromagnetism, via modulation of the interface electronic state using density functional calculation. From an analysis based on the phase model, forming the Au/Pd(100) interface induces hybridization of the wave function of d-electron quantum-well states, and modulates the term of the scattering phase shift as a function of the reciprocal lattice point. In contrast, forming the Al interface, which has only s-electrons at the Fermi energy, cannot modify the scattering phase shift. Our…
Emergent Interfacial Magnetism in Epitaxial RuO$_2$
Zhejiang University（浙江大学）；Westlake University（西湖大学）；Institute of Natural Sciences, Westlake Institute for Advanced Study（西湖高等研究院自然科学院）；Institute for Theoretical Sciences, Westlake Institute for Advanced Study（西湖高等研究院理论科学研究所）；New Cornerstone Science Laboratory, Department of Physics, Westlake University（西湖大学物理学院新基石科学实验室）
Thin epitaxial films of Tb metal were grown on a clean W(110) substrate in ultra-high vacuum and studied in-situ by low-energy electron microscopy. Annealed films present magnetic contrast in spin-polarized low-energy electron microscopy. The energy dependence of the electron reflectivity was determined and a maximum value of its spin asymmetry of about 1\% was measured. The magnetization direction of the Tb films is in-plane. Upon raising the temperature, no change in the domain distribution is observed, while the asymmetry in the electron reflectivity decreases when approaching the critical …
The double perovskite La2NiMnO6 (LNMO) exhibits complex magnetism due to the competition of magnetic interactions that are strongly affected by structural and magnetic inhomogeneities. In this work, we study the effect of oxygen annealing on the structure and magnetism of epitaxial thin films grown by pulsed laser deposition. The key observations are that a longer annealing time leads to a reduction of saturation magnetization and an enhancement in the ferromagnetic transition temperature. We explain these results based upon epitaxial strain and oxygen defect engineering. The oxygen enrichment…
Atomically engineered oxide heterostructures provide a fertile ground for creating novel states. For example, a two-dimensional electron gas at the interface between two oxide insulators, giant thermoelectric Seebeck coefficient, emergent ferromagnetism from otherwise nonmagnetic components, and colossal ionic conductivity. Extensive research efforts reveal that oxygen deficiency or lattice strain play an important role in determining these unexpected properties. Herein, by studying the abrupt presence of robust ferromagnetism (up to 1.5 uB/Mn) in LaMnO3-based heterostructures, we find the mul…
Tailoring magnetism of nanographenes via tip-controlled dehydrogenation
Empa—Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科技研究院）；Technical University of Dresden（德累斯顿工业大学）；University of Zurich（苏黎世大学）；University of Bern（伯尔尼大学）；Max Planck Institute of Microstructure Physics（马克斯·普朗克微观结构物理研究所）
Magnetic transition metal dichalcogenide (TMD) films have recently emerged as promising candidates to host novel magnetic phases relevant to next-generation spintronic devices. However, systematic control of the magnetization orientation, or anisotropy, and its thermal stability, characterized by Curie temperature (Tc) remains to be achieved in such films. Here we present self-intercalated epitaxial Cr1+δTe2 films as a platform for achieving systematic/smooth magnetic tailoring in TMD films. Using a molecular beam epitaxy (MBE) based technique, we have realized epitaxial Cr1+δTe2 films with sm…
Ferrimagnetic Mn$_2$Fe$_x$Ga $(0.26 \leq x \leq 1.12)$ thin films have been characterised by X-ray diffraction, SQUID magnetometry, X-ray absorption spectroscopy, X-ray magnetic circular dichroism and Mössbauer spectroscopy with the aim of determining the structure and site-specific magnetism of this tetragonal, D0$_{22}$-structure Heusler compound. High-quality epitaxial films with low RMS surface roughness ($\sim 0.6$ nm) are grown by magnetron co-sputtering. The tetragonal distortion induces strong perpendicular magnetic anisotropy along the $c$-axis with a typical coercive field $μ_0 H\sim…
We report on the effect of epitaxial strain on magnetic and optical properties of perovskite LaCrO3 (LCO) single crystal thin films. Epitaxial LCO thin films are grown by pulsed laser deposition on proper choice of substrates to impose different strain states. A combined experimental and theoretical approach is used to demonstrate the direct correlation between lattice-strain and functional properties. The magnetization results show that the lattice anisotropy plays a critical role in controlling the magnetic behavior of LCO films. The strain induced tetragonality in the film lattice strongly …
Magnetism of ordered Sm/Co(0001) surface structures
研究了Sm/Co（0001）外延系统，在Sm/Co/W（110）外延膜上的Sm覆盖率达到1个单层（ML）。发现1/3和1 ML Sm分别有两个有序相。利用光电子能谱确定了Sm的价态，利用磁光克尔效应测量了Sm的磁性。我们发现，1 ML Sm引起的相对于下面的10 ML Co膜的矫顽力的强烈增加。元素特定的磁滞回线，通过使用共振软X射线反射率测量，显示出相同的磁性行为的两个元素。
We have carried out the growth of h-RFeO3 (001) (R=Lu, Yb) thin films on Fe3O4 (111)/Al2O3 (001) substrates, and studied the effect of the h-RFeO3 (001)/Fe3O4 (111) interfaces on the epitaxy and magnetism. The observed epitaxial relations between h-RFeO3 and Fe3O4 indicates an unusual matching of Fe sub-lattices rather than a matching of O sub-lattices. The out-of-plane direction was found to be the easy magnetic axis for h-YbFeO3 (001) but the hard axis for Fe3O4 (111) in the h-YbFeO3 (001)/Fe3O4 (111)/Al2O3 (001) films, suggesting a perpendicular magnetic alignment at the h-YbFeO3 (001)/Fe3O…
Tailoring Gilbert damping of metallic ferromagnetic thin films is one of the central interests in spintronics applications. Here we report a giant Gilbert damping anisotropy in epitaxial Co$_{50}$Fe$_{50}$ thin film with a maximum-minimum damping ratio of 400 \%, determined by broadband spin-torque as well as inductive ferromagnetic resonance. We conclude that the origin of this damping anisotropy is the variation of the spin orbit coupling for different magnetization orientations in the cubic lattice, which is further corroborate from the magnitude of the anisotropic magnetoresistance in Co$_…
Origin and tailoring of the antiferromagnetic domain structure in $α$-Fe$_2$O$_3$ thin films unraveled by statistical analysis of dichroic spectro-microscopy (X-PEEM) images
用统计图象分析法确定了反铁磁$α$ O $_3$外延层的磁结构和畴壁分布.使用二向色光谱显微镜图像，我们表明，域结构是统计不变的厚度和反铁磁畴结构的薄膜是继承自亚铁磁性前体层之一，即使在完全转变成反铁磁$α$ -Fe $_2$ O $_3$。我们表明，修改前体层的磁畴结构是一种真正的方式来调整反铁磁层的磁畴结构和畴壁。
Intrinsic Even-Odd Thickness-Driven Anomalous Hall in Epitaxial MnBi2Te4 Thin Films
Oak Ridge National Laboratory（橡树岭国家实验室）；Pennsylvania State University（宾夕法尼亚州立大学）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Argonne National Laboratory（阿贡国家实验室）；University of Pennsylvania（宾夕法尼亚大学）
In this work, we demonstrate a massive intrinsic exchange bias (3 kOe) in epitaxial CoFe2O4(111) thin films deposited on Al2O3(0001) substrates. This exchange bias is indicative of intrinsic exchange or a ferromagnetic material combined with an antiferromagnet. The analysis of structure, magnetism and electronic states corroborate that there is an interfacial layer CoO between the CoFe2O4(111) thin film and the Al2O3(0001) substrate. The power-law thickness dependence of the intrinsic exchange bias verifies its interfacial origin. This work suggests interfacial engineering can be an effective …
Mismatched lattice-constants at a van-der-Waals epitaxy interface often introduce in-plane strains to the lattice of the epitaxial layer, termed epitaxy-strain, where the strains do not follow the intra-layer Poisson's relation. Here, we presented the magnetic phase diagrams of the CrSe2 and CrTe2 mono- and bi-layers under epitaxy-strain up to 8 %, as predicted using density-functional-theory calculations. They show that the in-plane epitaxy-strain manipulates either the intra- or inter-layer magnetism of them. The in-plane strain varies the interlayer distance, defined using an inter-layer Po…
Structural stability, electronic structure, and magnetism of the $d^9$ double infinite-layer La$_3$Ni$_2$O$_5$F under chemical pressure and epitaxial strain
Magnetism in lanthanum cobaltite (LCO, LaCoO$_3$) appears to be strongly dependent on strain, defects, and nanostructuring. LCO on strontium titanate (STO, SrTiO$_3$) is a ferromagnet with an interesting strain relaxation mechanism that yields a lattice modulation. However, the driving force of the ferromagnetism is still controversial. Experiments debate between a vacancy-driven or strain-driven mechanism for the ferromagnetism of epitaxial LCO. We found that a weak lateral modulation of the superstructure is sufficient to promote ferromagnetism. We find that ferromagnetism appears under unia…
Magnetic materials with kagome crystal structure exhibit rich physics such as frustrated magnetism, skyrmion formation, topological flat bands, and Dirac/Weyl points. Until recently, most studies on kagome magnets have been performed on bulk crystals or polycrystalline films. Here we report the synthesis of high-quality epitaxial films of topological kagome magnet Fe$_3$Sn$_2$ by atomic layer molecular beam epitaxy. Structural and magnetic characterization of Fe$_3$Sn$_2$ on epitaxial Pt(111) identifies highly ordered films with c-plane orientation and an in-plane magnetic easy axis. Studies o…
Highly ordered Bi2FeMnO6 epitaxial thin films have been successfully grown on SrTiO3 substrate. Both synchrotron X-ray reciprocal space mapping and high resolution transmission electron microscopy confirmed the alternative alignment of Fe and Mn along [111] direction of Bi2FeMnO6 films. Magnetic and ferroelectric properties of Bi2FeMnO6 films are characterized and analyzed. The room-temperature ferroelectricity is well kept in Bi2FeMnO6 film as expected. However, it is very interesting that Bi2FeMnO6 film exhibits a typical spin-glass behavior and very weak magnetism rather than a ferri/ferrom…
We show tunable strain-induced perpendicular magnetic anisotropy (PMA) over a wide range of thicknesses in epitaxial ferrimagnetic insulator Eu3Fe5O12 (EuIG) and Tb3Fe5O12 (TbIG) thin films grown by pulsed-laser deposition on Gd3Ga5O12 with (001) and (111) orientations, respectively. The PMA field is determined by measuring the induced anomalous Hall loops in Pt deposited on the garnet films. Due to positive magnetostriction constants, compressive in-plane strain induces a PMA field as large as 32.9 kOe for 4 nm thick EuIG and 66.7 kOe for 5 nm thick TbIG at 300 K, and relaxes extremely slowly…
Two-dimensional (2D) palladium ditelluride (PdTe2) and platinum ditelluride (PtTe2) are two Dirac semimetals which demonstrate fascinating quantum properties such as superconductivity, magnetism and topological order, illustrating promising applications in future nanoelectronics and optoelectronics. However, the synthesis of their monolayers is dramatically hindered by strong interlayer coupling and orbital hybridization. In this study, an efficient synthesis method for monolayer PdTe2 and PtTe2 is demonstrated. Taking advantages of the surface reaction, epitaxial growth of large-area and high…
Layered transition-metal compounds with controllable magnetic behaviors provide many fascinating opportunities for the fabrication of high-performance magneto-electric and spintronic devices. The tuning of their electronic and magnetic properties is usually limited to the change of layer thickness, electrostatic doping, and the control of electric and magnetic fields. However, pressure has been rarely exploited as a control parameter for tailoring their magneto-electric properties. Here, we report a unique pressure-driven isostructural phase transition in layered CrCl3 accompanied by a simulta…
Control of oxygen stoichiometry in complex oxides via topotactic phase transition is an interesting avenue to not only modifying the physical properties, but utilizing in many energy technologies, such as energy storage and catalysts. However, detailed structural evolution in the close proximity of the topotactic phase transition in multivalent oxides has not been much studied. In this work, we used strontium cobaltites (SrCoOx) epitaxially grown by pulsed laser epitaxy (PLE) as a model system to study the oxidation-driven evolution of the structure, electronic, and magnetic properties. We gre…
Temperature and crystallographic orientation dependence of the anisotropic magnetoresistance in epitaxial Fe65Co35 thin films
Universidad Nacional de Ingeniería（国立工程学院）；Universidad Católica San Pablo（圣保罗天主教大学）；Instituto Balseiro, Universidad Nacional de Cuyo, Comisión Nacional de Energía Atómica（巴尔塞罗研究所，门多萨国立大学，国家原子能委员会）；Instituto de Nanociencia y Nanotecnología (CNEA - CONICET)（纳米科学与技术研究所（国家原子能委员会-国家科学研究和技术委员会））；Comisión Nacional de Energía Atómica（国家原子能委员会）
The discoveries of intrinsic ferromagnetism in atomically-thin van der Waals crystals have opened up a new research field enabling fundamental studies on magnetism at two-dimensional (2D) limit as well as development of magnetic van der Waals heterostructures. To date, a variety of 2D ferromagnetism has been explored mainly by mechanically exfoliating 'originally ferromagnetic (FM)' van der Waals crystals, while bottom-up approach by thin film growth technique has demonstrated emergent 2D ferromagnetism in a variety of 'originally non-FM' van der Waals materials. Here we demonstrate that V5Se8…
The rapid discovery of two-dimensional (2D) van der Waals (vdW) quantum materials has led to heterostructures that integrate diverse quantum functionalities such as topological phases, magnetism, and superconductivity. In this context, the epitaxial synthesis of vdW heterostructures with well-controlled interfaces is an attractive route towards wafer-scale platforms for systematically exploring fundamental properties and fashioning proof-of-concept devices. Here, we use molecular beam epitaxy to synthesize a vdW heterostructure that interfaces two material systems of contemporary interest: a 2…
Polycrystalline Sr$_3$OsO$_6$, which is an ordered double-perovskite insulator, is synthesized via solid-state reaction under high-temperature and high-pressure conditions of 1200 $^\circ$C and 6 GPa. The synthesis enables us to conduct a comparative study of the bulk form of Sr$_3$OsO$_6$ toward revealing the driving mechanism of 1000 K ferromagnetism, which has recently been discovered for epitaxially grown Sr$_3$OsO$_6$ films. Unlike the film, the bulk is dominated by antiferromagnetism rather than ferromagnetism. Therefore, robust ferromagnetic order appears only when Sr$_3$OsO$_6$ is unde…
With reduced degrees of freedom, structural defects are expected to play a greater role in two-dimensional materials in comparison to their bulk counterparts. In particular, mechanical strength, electronic properties, and chemical reactivity are strongly affected by crystal imperfections in the atomically thin limit. Here, ultra-high vacuum (UHV) scanning tunneling microscopy (STM) and spectroscopy (STS) are employed to interrogate point and line defects in monolayer MoS2 grown on epitaxial graphene (EG) at the atomic scale. Five types of point defects are observed with the majority species sh…
