Both spectra are normalized to the max value of the Chiral Plus spectra and the normalization factor is provided. The difference spectrum EMCD signal is also presented. Inset is a schematic depicting the positions of the different aperture pairings in the reciprocal plane.
Figure 4a depicts the two chiral EELS spectra acquired using the scattering geometry of aperture pairing A, while Fig. All spectra in Fig. In these figures, the plural scattering has been removed 37 , the pre-edge background for the Chiral Plus and Chiral Minus spectra has been subtracted, and the signals have been shifted and aligned with respect to each other as described in the methods section. They otherwise represent the raw data. A clear difference can be seen between the two aperture pairings, indicating that the ratio of the area under the Fe L 2 and Fe L 3 edges changes between aperture pairings.
The determination of the error bars is discussed in the supplementary information. The presence of two chemically and structurally distinct layers described in the previous section offers a plausible explanation for this effect. The results of this summation for aperture pairings A and B are presented in Fig. A striking variation is visible.
This asymmetry nearly vanishes in aperture pairing B, which is additional evidence that the EMCD signal in aperture pairing B is dominated by the metallic iron signal. Such behavior would be expected if the oxide layer is magnetic and exhibits a strong orbital component yet is oriented in such a way that its contribution to the total EMCD signal at aperture pairing B is strongly reduced.
Aperture pairings A and B are presented in a , b , respectively. The EMCD signals for each chiral pair are also presented. Technical details of the computational approach are provided in the methods section. Figure 6a,b shows the calculated distribution of the magnetic signal originating from the L 3 edge of Fe atoms in the diffraction plane, displayed separately for the iron layer Fig.
This signal corresponds to the energy integral over the Fe- L 3 edge of the difference spectrum between chiral minus and chiral plus positions It shows that the magnetic signal varies with scattering angles differently for the iron and the oxide layers. Blue circles denote positions of the transmitted beam and Bragg-scattered beam G. The Thales circle is drawn with a full line, and aperture pairings A and B are shown with dashed and dotted lines, respectively.
Despite the much lower strength of the EMCD signal originating from the oxide layer, these maps depend quite strongly on the assumed orbital angular momentum of its iron atoms. Stronger variations are observed only along the lines where the EMCD signal originating from bcc Fe is negligible, thus even tiny deviations lead to substantial changes of calculated ratio.
In the area close to the Thales circle aperture position A, dashed line the value is significantly enhanced, while near the region represented by aperture position B dotted line , the value remains close to the expected 0. The range of this variation scales with the size of orbital angular momentum on oxide iron atoms, with smaller values giving rise to less variation.
The experimental design presented here provides two ways to study magnetic heterostructures that cannot be performed by any other method. First, by exploiting the angular dependency of the EMCD signal through the two different aperture pairings, it is possible to experimentally explore the different magnetic scattering contributions for both the metallic iron as well as its oxide surface layer. Second, by scanning the probe over a well-defined area from which individual datasets containing both spatial and spectral information are collected, it becomes possible to spatially segregate the EMCD signal with a spatial resolution of approximately 1.
The simplest explanation could be that this is an artifact in the analysis due to the position and width of the interval used for post-edge normalization of the spectra. However, note that the post-edge slope is very close to zero both aperture pairings over a wide energy range see Fig. Thus we are led explore the possibility that the orbital component to the net magnetization in the iron oxide layers is enhanced, as suggested by the simulations.
Such results have some precedent in the literature. For stoichiometric Fe 3 O 4 , Huang et al. However, other studies suggest that the orbital moment is quenched within the stoichiometric Fe 3 O 4 , resulting in a nearly vanishing net value 6 , 7 , 8 , and these conflicting reports have lead to some controversy 42 , Although our calculations provide strong support for the interpretation suggesting an enhanced orbital angular moment in oxide, we would like to present an alternative argument, which is independent of the simulations.
The dynamical diffraction effects 25 , 44 will mix the contributions of the three sublattices in a non-trivial way. A full disentangling of the individual contributions, as performed by Wang et al. However, in general, a linear combination of large spin moment contributions will yield a result larger than a corresponding linear combination of the small orbital moment contributions, especially considering that there is a variation of the thickness of the oxide within the studied region. But this is in contradiction with our measurements, implying enhancement of the orbital moment in the oxide layer.
The reason for the variation of orbital magnetic moments in the literature is not always evident, although a number of theories exist.
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Kallmayer et al. A modest enhancement of the orbital moment was observed at the interface between Fe 3 O 4 and Al 2 O 3. They interpret this as a consequence of the reduced crystal symmetry of the magnetite at this interface arising from the incorporation of misfit dislocations due to the large lattice mismatch. Another explanation comes from an investigation into the potential for magnetite to harbor large, hidden orbital moments by E. Goering Goering calculates an average orbital moment of 1.
Thus it appears that the observed enhancement of the orbital moment may be partially understood by examining the literature. However, it is critical to emphasize that, due to the unique nature of the EMCD technique presented here, it needs to be considered independently. For example, to the best of our knowledge, all of the quantitative magnetic information on stoichiometric Fe 3 O 4 to date comes from bulk systems or thin films where the signals are averaged over regions several hundreds of microns in diameter or more.
The results presented here, on the other hand, are a summation of individual spectra acquired from volumes of material illuminated with an electron probe having a diameter of less than 1. Thus nanoscale effects may play a greater role than for measurement techniques that probe much larger volumes of material. As an example of how this may manifest itself, we note that it is quite plausible that a series of correlated defects at the interface between Fe and magnetite could lead to a reduction in crystalline symmetry that may account for at least some enhancement of the orbital moment, and that the EMCD technique presented here would be exceptionally sensitive to this.
Moreover, although not explicitly investigated in this experiment, the preparation of the lamella with the FIB results in the presence of Gallium impurities on the exposed iron surface. This may influence the growth and magnetic behavior of the cladding oxide layers. In conclusion, we present an EMCD-based method that enables the quantitative analysis of magnetic moments in chemically and structurally distinct overlapping magnetic thin films in the TEM with nanoscale spatial resolution.
Simulations suggest that this can be understood if the orbital component of the net magnetic moment in the oxide is enhanced. Thus this method is capable of providing significant insight into the nature of nanoscale magnetism in a way not yet possible for any other technique. A thin film of pure iron was deposited by molecular beam epitaxy onto a single crystal 0 0 1 MgO substrate. The field emission gun was operated in such a way to produce a high current at the expense of energy resolution, which was close to 1.
The minicondenser lens was switched off to yield a lower convergence angle of 1. We estimate that the spatial resolution of this configuration is 1. The EELS entrance aperture physical diameter 1. The aperture was positioned using a script to excite the diffraction shift coils and the exact positions are shown in the insets of Fig.
This resulted primarily in a mass-thickness contrast mechanism, but also included some diffraction contrast. The region from which all spectrum image data cubes were acquired is shown in green in Fig. A drift correction routine carried out at regular intervals ensured that the probe position within this region could be linked to the survey image and, subsequently, related between all of the individual data cubes.
This was repeated for both aperture positions in pairing B see Fig. The low-loss region was acquired with the diffraction pattern on-axis using a dispersion of 0. Critically, the survey image was not reacquired between aperture shifts, allowing for the same region to be scanned multiple times. Following the acquisition of each individual spectral image, correlated noise was accounted for by taking the average of dark current measurements - where N is the total number of acquisitions - and subsequently subtracted from the gain normalized spectra Energy drift in the individual spectra within the spectral images was corrected for by using a cross-correlation algorithm to align the spectra to the Fe L 3 ionization edge within the regions of the film having the largest metallic iron content.
The drift correction for the remaining spectra was determined by interpolating a spline fit between the non-corrected regions. For the EMCD spectra, the energy drift correction resulted in a gain averaging over approximately 15 channels, further improving the signal to noise ratio Following this step, the effects of plural scattering were removed by deconvolving all of the core-loss spectral images with the on-axis low-loss spectral image The on-axis core-loss spectral image was used to quantify the relative amount of iron r Fe and oxygen r ox at any given pixel.
This was accomplished by fitting the deconvolved data to the differential scattering cross-sections calculated using the Hartree-Slater model as implemented in Digital Micrograph. This was used to calculate the absolute thickness t tot of the region at each pixel position by using the low-loss spectral image to first extract the relative thickness values.
An equation governing the thickness of the oxide layer t ox as a function of R and t tot was derived under the assumption of it being similar in structure to Fe 3 O 4. The justification for this assumption is provided in the supplementary information. This yields equation 1. The primary sources of systematic error for this calculation include the choice of cross-section model and the quantification routine, uncertainty in the local densities of the oxide and metal, the potential presence of an amorphous carbon coating layer, and unknown stoichiometric deviations from pure Fe 3 O 4.
Since many of these error sources are difficult to quantify, we are not able to provide systematic error bars for this calculation. Despite that, we note that the statistical error appears to be quite low due to the high signal to noise ratio. Consequently, we feel that these data provide a constructive qualitative assessment of the thicknesses of the individual metal and oxide layers. The EMCD signal was computed by first interpolating the background-removed data to a dispersion of 0.
With this, the conditions for sum rules are satisfied and can be calculated using equation 2 36 ,. The uncertainty was estimated by accumulating the errors introduced by counting statistics, background extrapolation, post-edge normalization, and taking the difference between the two chiral spectra. This cumulative error was then propagated through equation 2. More detail is provided in the supplementary information.
We note that this way of processing data, particularly the post-edge normalization step before taking the difference, significantly suppresses the effects of asymmetry of the two beam case 17 , 44 , Thus the difference of post-edge normalized spectra faithfully represents the EMCD spectrum.
Simulations of the inelastic electron scattering were performed using the classical Bloch-waves method assuming a plane-wave illumination 54 , 55 , This book covers the exciting new area of characterization of materials on the nanoscale by studying the chirality of electrons in transmission electron microscopy TEM. Schattschneider, his team in Vienna and his colleagues all around the world, edited an extremely well written book which will have its impact for the important area of advanced characterisation techniques of materials with high spatial resolution- nearly on the atomic scale.
The different techniques can be used by experienced microscopists who are able to understand the physics of the different inelastic scattering processes occurring in a specimen in TEM. This state-of-the-art textbook describes how magnetic properties of solids can be investigated by using x-ray absorption and electron energy-loss spectroscopy. The main emphasis is on the underlying theory but experimental techniques, data analysis and recent results are also well covered.
Chiral effects in anisotropic materials, multiplet and density-functional theory, magic-angle and relativistic effects, x-ray holography and the possibility of atomic-scale spin mapping are all described in detail by experts in these various fields. Peter Schattchneider has made many fundamental contributions to the theory of electron-beam imaging and spectroscopic techniques. The result is a spin-sensitive imaging method with far higher spatial resolution than similar synchrotron-based methods.
The growing interest in the miniaturization of magnetic storage media and the quest for novel spintronics applications rely on the element-specific detection of spin and orbital magnetic moments in a solid. The most sophisticated technique to reach this aim has been X-ray magnetic circular dichroism XMCD , largely used in synchrotron beam lines.
The spatial resolution limit of this technique is of the order of 20—50 nm. This presents a sensible limit for the study of nanostructured devices.
This book describes energy loss magnetic chiral dichroism EMCD , a phenomenon in energy loss spectroscopy discovered in A spatial resolution of 2 nm has been demonstrated, and the lattice-resolved mapping of atomic spins appears feasible. EMCD is, thus, a promising technique for magnetic studies on the nanometer and sub-nanometer scale, providing the technical and logistic advantages of electron microscopy, such as in situ chemical and structural information, easy access, and low cost.
The role of the crystal as an electron interferometer for the setup of chiral electronic transitions is also discussed. In addition to the appearance of retardation effects in EELS, theoretical approaches to X-ray absorption spectroscopy are covered. In the theory section, various methods of the calculation of XMCD and EMCD spectra from first principles are covered, namely the multiplet, density functional reciprocal space , and multiple scattering cluster methods. The experimental part covers a number of EMCD techniques with their particularities, as well as data treatment that is nontrivial in view of low-scattering cross sections.
Sum rules for spin and orbital moments, already touched in several chapters, are treated in a separate contribution.
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X-ray holography will benefit from the high-brightness X-ray sources now under construction. Scanning EMCD promises spin mapping on the atomic level with the generation of electron microscopes now under development. The color version of the figures in the book can be accessed here. Advanced graduate-level students in physics and material science; researchers in physics, magnetism, and nanotechnology; scientific staff in electron microscopy, nanomagnetism, and spintronics development. All rights reserved.
Magnetic linear dichroism in electron energy loss spectroscopy
The characters you copied from the image are incorrect. Please try again. A further capping layer of 2 nm of Cu was We chose Fe for the experiment because the Fe L2,3 ionization edge deposited to prevent Fe layer oxidation during the transferring of the shows a strong dichroic effect. The magnitude of the equipped with a Gatan image filter. A flat region of nm radius dichroism is represented by the difference between the two spectra. The sample is immersed in the magnetic field of the TEM previously thinned and ion milled to electron transparency and objective lens pole piece, which is approximately 2 T and oriented protected by 2.
Remanent in-plane magnetization perpendicular to the surface. The magnetization of the iron film in could be evidenced by measurements of the transverse and longi- the TEM experiment is therefore saturated in the out-of-plane tudinal magneto-optic Kerr effect: the hysteresis loops indicated a direction by a field that is large with respect to the in-plane coercive field of 80 Oe and full remanence in the in-plane easy coercitivity. This is crystallographically identical to the in-plane magnetization direction. The specimens, suitable for both X-ray magnetization used in the XMCD experiment, providing two physi- absorption spectroscopy and TEM experiments, were transferred in cally equivalent conditions.
The measured spectra are shown in Fig. The with the WIEN2k code18 —a full-potential, fully relativistic augmen- dichroic signal was obtained by scanning in energy over the Fe L2,3 ted plane wave code based on density functional theory.
EMCD edge and by reversing the photon helicity, as well as for a given X-ray spectra require evaluation of the mixed dynamic form factor. For this Figure 2 X-ray magnetic circular dichroism. Circular dichroism in the Fe Figure 3 Energy-loss magnetic chiral dichroism. Measured a and L2,3 edge of epitaxial iron on GaAs remanently magnetized along the simulated b Fe L2,3 edges for 10 nm Fe on GaAs in the two in-plane  direction.
The r. Ohldag, H. Spectroscopic identification and direct imaging of interfacial magnetic spins. Wu, Y. Details about the calculation can multilayers: a magnetic circular X-ray dichroism study. A comparison Fig. Tischer, M. Enhancement of orbital magnetism at surfaces: Co on observed dichroic signal is smaller than predicted. This can be Cu Won, C.
USTEM : Dichroism
Weller, D. The GaAs spot Vogel, J. Magnetic moments in as-deposited and annealed Ni layers on Fe : an x-ray-dichroism study. B 53, — Exploring the microscopic origin of magnetic anisotropies with X-ray quasi-elastic Bragg to inelastic scattering. Moreover, the integration magnetic circular dichroism XMCD spectroscopy. Another X-ray magnetic circular dichroism spectroscopy of transition metal prominent effect is the sensitivity of the signal to the specimen thin films. Electron Spectrosc. Related Phenom.
Linear and Chiral Dichroism in the Electron Microscope
Yuan, J. Magnetic linear dichroism in electron energy loss thickness. Hitchcock, A. Near edge electron energy loss spectroscopy: comparison to tary Fig. X-ray absorption. Kohl, H. Theory of image formation by inelastically scattered electrons in the electron microscope.