Electron Energy-loss Magnetic Chiral Dichroism Research Articles

Experimental evidence of magnetism in a 2D electron gas at the CoO/Co3O4 interface by employing EMCD

In the present study we investigate the CoO/Co3O4 interface in order to determine its intriguing magnetic behavior, which can be utilized for tailoring magnetic properties, enabling spin transport, enhancing magnetic coupling, tuning device functionalities, and realizing miniaturized magnetic devices for various technological applications. We decipher the magnetic properties of the CoO/Co3O4 interface from first principles calculations using Wien2k and probe them experimentally by employing electron energy-loss magnetic chiral dichroism (EMCD), which is an electron-energy loss spectrometry (EELS) based technique in the transmission electron microscope (TEM). Both, theory and experiment, are in perfect agreement and result in a ferromagnetic 2D-electron gas of 5Å thickness directly at the interface.

A study on the relationship of magnetic moments orientation in L10 FePt network nanostructured film by electron energy-loss magnetic chiral dichroism using semi-core excitation spectra

In this study, we applied electron energy-loss magnetic chiral dichroism (EMCD), an electron counterpart of X-ray magnetic circular dichroism (XMCD), to a network nanostructured FePt L10 ordered alloy film to examine the relative orientation of magnetic moments between neighboring Fe and Pt atoms using the Fe-M2,3, Pt-O2,3, and Pt-N6,7 semi-core excitation spectra with transmission electron microscopy and electron energy-loss spectroscopy. EMCD signals were successfully extracted from a large number of spectra using a dedicated data analysis procedure to obtain sufficient noise statistics. Results showed that the relative sign relation of the EMCD signals between the Fe and Pt absorption edges was consistent with that of the theoretical dielectric tensor while assuming that parallel magnetic moments exist between neighboring Fe and Pt. We believe the results of this study can be applied to alloys with different nanostructures to determine whether the spin configuration depends on the size and geometry of the nanostructures.

A Study on the Relationship of Magnetic Moments Orientation in L10 Fept Network Nanostructured Film by Electron Energy-Loss Magnetic Chiral Dichroism Using Semi-Core Excitation Spectra

A Study on the Relationship of Magnetic Moments Orientation in L10 Fept Network Nanostructured Film by Electron Energy-Loss Magnetic Chiral Dichroism Using Semi-Core Excitation Spectra

Dynamical diffraction effects in STEM orbital angular momentum resolved electron energy-loss magnetic chiral dichroism

In this work we derive sum rules for orbital angular momentum(OAM) resolved electron magnetic chiral dichroism (EMCD) which enable the evaluation of the strength of spin and orbital components of the atomic magnetic moments in a crystalline sample. We also demonstrate through numerical simulations that these rules appear to be only slightly dependent from the dynamical diffraction of the electron beam in the sample, making possible their application without the need of additional dynamical diffraction calculations.

Electron energy-loss magnetic chiral dichroism of magnetic iron film affected by an underlayer in a double-layer structure

The electron energy-loss magnetic chiral dichroism (EMCD) technique has been generally applied to single-phase magnetic crystals while rarely used for composite structures. It is mainly due to the lack of in-depth understanding of EMCD in the latter case where an additional phase may present under or above the investigated magnetic phase in the electron beam path. Here, we report EMCD signals acquired on a 15-nm-thick magnetic iron film with different thicknesses of the MgO substrate underlayer. By comparison, for areas with total thicknesses of t=0.59λ and t=1.02λ expressed with the mean free inelastic path of electron λ, the relative dichroic signals at the Fe-L3 edge are 3.8%±1.0% and 3.5%±1.6%, respectively, demonstrating no significant difference within the error range. However, the dichroic signal intensity at the Fe-L2 edge peak is 77.6% larger in the thinner area of t=0.59λ. Accordingly, the extracted mL/ms ratio of Fe 3d moments is 63% smaller in the thinner area even after the plural scattering is removed. Then, we confirm that the presence of an additional nonmagnetic phase under a magnetic iron crystal can noticeably affect the quantified value of the mL/ms ratio of iron moment determined from the EMCD measurements. Furthermore, the larger thickness of the underlayer may result in relatively higher valuation of the mL/ms ratio of the upper layer. A correction method, considering the different influence of the underlayer on the Fe-L3 and L2 edges, is in demand for developing potential applications of the EMCD technique to such composite nanomaterial systems.

Nanoscale measurement of giant saturation magnetization in α″-Fe16N2 by electron energy-loss magnetic chiral dichroism

Metastable α″-Fe16N2 thin films were reported to have a giant saturation magnetization of above 2200 emu/cm3 in 1972 and have been considered as candidates for next-generation rare-earth-free permanent magnetic materials. However, their magnetic properties have not been confirmed unequivocally. As a result of the limited spatial resolution of most magnetic characterization techniques, it is challenging to measure the saturation magnetization of the α″-Fe16N2 phase, as it is often mixed with the parent α′-Fe8N phase in thin films. Here, we use electron energy-loss magnetic chiral dichroism (EMCD), aberration-corrected transmission electron microscopy, X-ray diffraction and macroscopic magnetic measurements to study α″-Fe16N2 (containing ordered N atoms) and α′-Fe8N (containing disordered N atoms). The ratio of saturation magnetization in α″-Fe16N2 to that in α′-Fe8N is determined to be 1.31 ± 0.10 from quantitative EMCD measurements and dynamical diffraction calculations, confirming the giant saturation magnetization of α″-Fe16N2. Crystallographic information is also obtained about the two phases, which are mixed on the nanoscale.

Effect of cation ratio and order on magnetic circular dichroism in the double perovskite Sr2Fe1+xRe1-xO6

Superexchange-based magnetic coupling of the two B-site cations in rock-salt-ordered double perovskite oxides is extremely sensitive to the cation ratio and degree of order. However, as a result of the limited spatial resolution of most magnetic characterization techniques, it is challenging to establish a direct relationship between magnetic properties and structure in these materials, including the effects of elemental segregation and cation disorder. Here, we use electron energy-loss magnetic chiral dichroism together with aberration-corrected electron microscopy and spectroscopy to record magnetic circular dichroism (MCD) spectra at the nm scale, in combination with structural and chemical information at the atomic scale from the very same region. We study nanoscale phases in ordered Sr2[Fe][Re]O6, ordered Sr2[Fe][Fe1/5Re4/5]O6 and disordered Sr[Fe4/5Re1/5]O3 individually, in order to understand the role of cation ratio and order on local magnetic coupling. When compared with ordered Sr2[Fe][Re]O6, we find that antiferromagnetic Fe3+-O2−-Fe3+superexchange interactions arising from an excess of Fe suppress the MCD signal from Fe cations in ordered Sr2[Fe][Fe1/5Re4/5]O6, while dominant Fe3+-O2−-Fe3+antiferromagnetic coupling in disordered Sr[Fe4/5Re1/5]O3 leads to a decrease in MCD signal down to the noise level. Our work demonstrates a protocol that can be used to correlate crystallographic, electronic and magnetic information in materials such as Sr2Fe1+xRe1-xO6, in order to provide insight into structure-property relationships in double perovskite oxides at the atomic scale.

Atomic scale imaging of magnetic circular dichroism by achromatic electron microscopy.

In order to obtain a fundamental understanding of the interplay between charge, spin, orbital and lattice degrees of freedom in magnetic materials and to predict and control their physical properties1-3, experimental techniques are required that are capable of accessing local magnetic information with atomic-scale spatial resolution. Here, we show that a combination of electron energy-loss magnetic chiral dichroism 4 and chromatic-aberration-corrected transmission electron microscopy, which reduces the focal spread of inelastically scattered electrons by orders of magnitude when compared with the use of spherical aberration correction alone, can achieve atomic-scale imaging of magnetic circular dichroism and provide element-selective orbital and spin magnetic moments atomic plane by atomic plane. This unique capability, which we demonstrate for Sr2FeMoO6, opens the door to local atomic-level studies of spin configurations in a multitude of materials that exhibit different types of magnetic coupling, thereby contributing to a detailed understanding of the physical origins of magnetic properties of materials at the highest spatial resolution.

Detection of magnetic circular dichroism in amorphous materials utilizing a single-crystalline overlayer

Electron energy-loss magnetic chiral dichroism (EMCD) is a novel technique that allows magnetic information determination down to the nanoscale. However, constrained by the predefined diffraction g ...

An in-plane magnetic chiral dichroism approach for measurement of intrinsic magnetic signals using transmitted electrons

Electron energy-loss magnetic chiral dichroism is a powerful technique that allows the local magnetic properties of materials to be measured quantitatively with close-to-atomic spatial resolution and element specificity in the transmission electron microscope. Until now, the technique has been restricted to measurements of the magnetic circular dichroism signal in the electron beam direction. However, the intrinsic magnetization directions of thin samples are often oriented in the specimen plane, especially when they are examined in magnetic-field-free conditions in the transmission electron microscope. Here, we introduce an approach that allows in-plane magnetic signals to be measured using electron magnetic chiral dichroism by selecting a specific diffraction geometry. We compare experimental results recorded from a cobalt nanoplate with simulations to demonstrate that an electron magnetic chiral dichroism signal originating from in-plane magnetization can be detected successfully.

Atom size electron vortex beams with selectable orbital angular momentum

The decreasing size of modern functional magnetic materials and devices cause a steadily increasing demand for high resolution quantitative magnetic characterization. Transmission electron microscopy (TEM) based measurements of the electron energy-loss magnetic chiral dichroism (EMCD) may serve as the needed experimental tool. To this end, we present a reliable and robust electron-optical setup that generates and controls user-selectable single state electron vortex beams with defined orbital angular momenta. Our set-up is based on a standard high-resolution scanning TEM with probe aberration corrector, to which we added a vortex generating fork aperture and a miniaturized aperture for vortex selection. We demonstrate that atom size probes can be formed from these electron vortices and that they can be used for atomic resolution structural and spectroscopic imaging – both of which are prerequisites for future atomic EMCD investigations.

EMCD with an electron vortex filter: Limitations and possibilities

We discuss the feasibility of detecting spin polarized electronic transitions with a vortex filter. This approach does not rely on the principal condition of the standard electron energy-loss magnetic chiral dichroism (EMCD) technique, the precise alignment of the crystal in order to use it as a beam splitter, and thus would pave the way for the application of EMCD to new classes of materials and problems, like amorphous magnetic alloys and interface magnetism. The dichroic signal strength at the L2, 3-edge of ferromagnetic Cobalt (Co) is estimated on theoretical grounds using a single atom scattering approach. To justify this approach, multi-slice simulations were carried out in order to confirm that orbital angular momentum (OAM) is conserved in amorphous materials over an extended range of sample thickness and also in very thin crystalline specimen, which is necessary for the detection of EMCD. Also artefact sources like spot size, mask tilt and astigmatism are discussed. In addition, the achievable SNR under typical experimental conditions is assessed.

Effects of dynamic diffraction conditions on magnetic parameter determination in a double perovskite Sr2FeMoO6 using electron energy-loss magnetic chiral dichroism

Electron energy-loss magnetic chiral dichroism (EMCD) spectroscopy, which is similar to the well-established X-ray magnetic circular dichroism spectroscopy (XMCD), can determine the quantitative magnetic parameters of materials with high spatial resolution. One of the major obstacles in quantitative analysis using the EMCD technique is the relatively poor signal-to-noise ratio (SNR), compared to XMCD. Here, in the example of a double perovskite Sr2FeMoO6, we predicted the optimal dynamical diffraction conditions such as sample thickness, crystallographic orientation and detection aperture position by theoretical simulations. By using the optimized conditions, we showed that the SNR of experimental EMCD spectra can be significantly improved and the error of quantitative magnetic parameter determined by EMCD technique can be remarkably lowered. Our results demonstrate that, with enhanced SNR, the EMCD technique can be a unique tool to understand the structure-property relationship of magnetic materials particularly in the high-density magnetic recording and spintronic devices by quantitatively determining magnetic structure and properties at the nanometer scale.

Magnetic properties of single nanomagnets: Electron energy-loss magnetic chiral dichroism on FePt nanoparticles

Electron energy-loss magnetic chiral dichroism (EMCD) allows for the quantification of magnetic properties of materials at the nanometer scale. It is shown that with the support of simulations that help to identify the optimal conditions for a successful experiment and upon implementing measurement routines that effectively reduce the noise floor, EMCD measurements can be pushed towards quantitative magnetic measurements even on individual nanoparticles. With this approach, the ratio of orbital to spin magnetic moments for the Fe atoms in a single L10 ordered FePt nanoparticle is determined to be ml/ms=0.08±0.02. This finding is in good quantitative agreement with the results of XMCD ensemble measurements.

Quantitative determination of site-specific magnetic structure in TEM

Determining the magnetic structure of material on a nanometer scale is fundamental for understanding its nano-scale magnetic property and developing nano-scale magnetic devices. Site-specific electron energy-loss magnetic chiral dichroism (site-specific EMCD[1],[2]) method is come up with to get the crystallographic site-specific magnetic information of nanostructures. By constructively using the dynamical diffraction conditions in EMCD experiments, we experimentally achieve the crystallographic site-specific magnetic structure of a nanostructure of NiFe2O4 as an example in transmission electron microscope, with its site-specific magnetic circular dichroism spectra, and its site-specific spin/orbital magnetic moments extracted. The site-specific EMCD method shows its unique capability for solving the crystallographic site-specific magnetic structure on nano-scale, compared with X-ray magnetic circular dichroism and neutron diffraction. This work may benefit the research and application of magnetic materials on a nanometer scale. Acknowledgement: This work is financially supported by National 973 Project of China (2009CB623701) and Chinese National Nature Science Foundation (11374174,51390471 ). This work made use of the resources of the Beijing National Center for Electron Microscopy.

Quantitative experimental determination of site-specific magnetic structures by transmitted electrons

Understanding the magnetic structure of materials on a nanometre scale provides fundamental information in the development of novel applications. Here we show a site-specific electron energy-loss magnetic chiral dichroism method, first experimentally demonstrating that the use of transmitted electrons allows us to quantitatively determine atomic site-specific magnetic structure information on a nanometre scale. From one NiFe(2)O(4) nanograin in composite films, we extract its atomic site-specific magnetic circular dichroism spectra and achieve the quantitative magnetic structure information, such as site-specific total magnetic moments and orbital to spin magnetic moment ratios, by constructively selecting the specific dynamical diffraction conditions in electron energy-loss magnetic chiral dichroism experiments. The site-specific electron energy-loss magnetic chiral dichroism method shows its unique ability for solving the site-specific magnetic structure at nanoscale resolution, compared with X-ray magnetic circular dichroism and neutron diffraction. This work opens a door to meet the challenge of exploring the magnetic structures of magnetic materials at the nanoscale using transmitted electrons.

Simulation of magnetic circular dichroism in the electron microscope

As electron energy-loss spectroscopy (EELS) and x-ray absorption spectroscopy (XAS) probe the same transitions from core–shell states to unoccupied states above the Fermi energy, it should always be possible to apply the two techniques to the same physical phenomena, such as magnetic dichroism, and obtain the same information. Indeed, the similarity in the expression of the electron and x-ray cross-sections had been already exploited to prove the equivalence of x-ray magnetic linear dichroism and anisotropy in EELS, by noting that the polarization vector of a photon plays the same role as the momentum transfer in electron scattering. Recently, the same was proven true for x-ray magnetic circular dichroism (XMCD) by establishing a new TEM technique called EMCD (electron energy-loss magnetic chiral dichroism) (Schattschneider P et al 2006 Nature 441 486–8), which makes use of special electron scattering conditions to force the absorption of a circularly polarized virtual photon.The intrinsic advantage of EMCD over XMCD is the high spatial resolution of electron microscopes, which are readily available. Among the particular obstacles in EMCD that do not exist for synchrotron radiation, is the notoriously low signal and the very particular scattering conditions necessary to observe a chiral dichroic signal. In spite of that, impressive progress has been made in recent years. The signal strength could be considerably increased, and some innovations such as using a convergent beam have been introduced. EMCD has evolved into several techniques, which make full use of the versatility of the TEM and energy filtering, spectroscopy or STEM conditions (Rubino S 2007 Magnetic circular dichroism in the transmission electron microscope PhD Thesis Vienna University of Technology, Vienna, Austria).

Detection of magnetic circular dichroism using a transmission electron microscope

A material is said to exhibit dichroism if its photon absorption spectrum depends on the polarization of the incident radiation. In the case of X-ray magnetic circular dichroism (XMCD), the absorption cross-section of a ferromagnet or a paramagnet in a magnetic field changes when the helicity of a circularly polarized photon is reversed relative to the magnetization direction. Although similarities between X-ray absorption and electron energy-loss spectroscopy in a transmission electron microscope (TEM) have long been recognized, it has been assumed that extending such equivalence to circular dichroism would require the electron beam in the TEM to be spin-polarized. Recently, it was argued on theoretical grounds that this assumption is probably wrong. Here we report the direct experimental detection of magnetic circular dichroism in a TEM. We compare our measurements of electron energy-loss magnetic chiral dichroism (EMCD) with XMCD spectra obtained from the same specimen that, together with theoretical calculations, show that chiral atomic transitions in a specimen are accessible with inelastic electron scattering under particular scattering conditions. This finding could have important consequences for the study of magnetism on the nanometre and subnanometre scales, as EMCD offers the potential for such spatial resolution down to the nanometre scale while providing depth information--in contrast to X-ray methods, which are mainly surface-sensitive.