“Low-field switching of noncollinear spin texture at La0.7Sr0.3MnO3-SrRuO3interfaces”. Das S, Rata AD, Maznichenko I V, Agrestini IS, Pippel E, Gauquelin N, Verbeeck J, Chen K, Valvidares SM, Vasili HB, Herrero-Martin J, Pellegrin E, Nenkov K, Herklotz A, Ernst A, Mertig I, Hu Z, Doerr K, Physical review B 99, 024416 (2019). http://doi.org/10.1103/PHYSREVB.99.024416
Abstract: Interfaces of ferroic oxides can show complex magnetic textures which have strong impact on spintronics devices. This has been demonstrated recently for interfaces with insulating antiferromagnets such as BiFeO3. Here, noncollinear spin textures which can be switched in very low magnetic field are reported for conducting ferromagnetic bilayers of La0.7Sr0.3MnO3-SrRuO3 (LSMO-SRO). The magnetic order and switching are fundamentally different for bilayers coherently grown in reversed stacking sequence. The SRO top layer forms a persistent exchange spring which is antiferromagnetically coupled to LSMO and drives switching in low fields of a few milliteslas. Density functional theory reveals the crucial impact of the interface termination on the strength of Mn-Ru exchange coupling across the interface. The observation of an exchange spring agrees with ultrastrong coupling for the MnO2/SrO termination. Our results demonstrate low-field switching of noncollinear spin textures at an interface between conducting oxides, opening a pathway for manipulating and utilizing electron transport phenomena in controlled spin textures at oxide interfaces.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.836
Times cited: 19
DOI: 10.1103/PHYSREVB.99.024416
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“2D atomic mapping of oxidation states in transition metal oxides by scanning transmission electron microscopy and electron energy-loss spectroscopy”. Tan H, Turner S, Yücelen E, Verbeeck J, Van Tendeloo G, Physical review letters 107, 107602 (2011). http://doi.org/10.1103/PhysRevLett.107.107602
Abstract: Using a combination of high-angle annular dark-field scanning transmission electron microscopy and atomically resolved electron energy-loss spectroscopy in an aberration-corrected transmission electron microscope we demonstrate the possibility of 2D atom by atom valence mapping in the mixed valence compound Mn3O4. The Mn L2,3 energy-loss near-edge structures from Mn2+ and Mn3+ cation sites are similar to those of MnO and Mn2O3 references. Comparison with simulations shows that even though a local interpretation is valid here, intermixing of the inelastic signal plays a significant role. This type of experiment should be applicable to challenging topics in materials science, such as the investigation of charge ordering or single atom column oxidation states in, e.g., dislocations.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 115
DOI: 10.1103/PhysRevLett.107.107602
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“2D atomic mapping of oxidation states in transition metal oxides by scanning transmission electron microscopy and electron energy-loss spectroscopy : reply”. Tan H, Turner S, Yucelen E, Verbeeck J, Van Tendeloo G, Physical review letters 108, 259702 (2012). http://doi.org/10.1103/PHYSREVLETT.108.259702
Keywords: Editorial; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
DOI: 10.1103/PHYSREVLETT.108.259702
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“Novel vortex generator and mode converter for electron beams”. Schattschneider P, Stoeger-Pollach M, Verbeeck J, Physical review letters 109, 084801 (2012). http://doi.org/10.1103/PhysRevLett.109.084801
Abstract: A mode converter for electron vortex beams is described. Numerical simulations, confirmed by experiment, show that the converter transforms a vortex beam with a topological charge m = +/- 1 into beams closely resembling Hermite-Gaussian HG(10) and HG(01) modes. The converter can be used as a mode discriminator or filter for electron vortex beams. Combining the converter with a phase plate turns a plane wave into modes with topological charge m = +/- 1. This combination serves as a generator of electron vortex beams of high brilliance.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 74
DOI: 10.1103/PhysRevLett.109.084801
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“Observation of the Larmor and Gouy rotations with electron vortex beams”. Guzzinati G, Schattschneider P, Bliokh KY, Nori F, Verbeeck J, Physical review letters 110, 093601 (2013). http://doi.org/10.1103/PhysRevLett.110.093601
Abstract: Electron vortex beams carrying intrinsic orbital angular momentum (OAM) are produced in electron microscopes where they are controlled and focused by using magnetic lenses. We observe various rotational phenomena arising from the interaction between the OAM and magnetic lenses. First, the Zeeman coupling, proportional to the OAM and magnetic field strength, produces an OAM-independent Larmor rotation of a mode superposition inside the lens. Second, when passing through the focal plane, the electron beam acquires an additional Gouy phase dependent on the absolute value of the OAM. This brings about the Gouy rotation of the superposition image proportional to the sign of the OAM. A combination of the Larmor and Gouy effects can result in the addition (or subtraction) of rotations, depending on the OAM sign. This behavior is unique to electron vortex beams and has no optical counterpart, as Larmor rotation occurs only for charged particles. Our experimental results are in agreement with recent theoretical predictions.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 91
DOI: 10.1103/PhysRevLett.110.093601
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“Comment on “Quantized orbital angular momentum transfer and magnetic dichroism in the interaction of electron vortices with matter””. Schattschneider P, Löffler S, Verbeeck J, Physical review letters 110, 189501 (2013). http://doi.org/10.1103/PhysRevLett.110.189501
Keywords: Editorial; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 8
DOI: 10.1103/PhysRevLett.110.189501
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“Exploiting lens aberrations to create electron-vortex beams”. Clark L, Béché, A, Guzzinati G, Lubk A, Mazilu M, Van Boxem R, Verbeeck J, Physical review letters 111, 064801 (2013). http://doi.org/10.1103/PhysRevLett.111.064801
Abstract: A model for a new electron-vortex beam production method is proposed and experimentally demonstrated. The technique calls on the controlled manipulation of the degrees of freedom of the lens aberrations to achieve a helical phase front. These degrees of freedom are accessible by using the corrector lenses of a transmission electron microscope. The vortex beam is produced through a particular alignment of these lenses into a specifically designed astigmatic state and applying an annular aperture in the condenser plane. Experimental results are found to be in good agreement with simulations.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 66
DOI: 10.1103/PhysRevLett.111.064801
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“Experimental evidence for oxygen sublattice control in polar infinite layer SrCuO2”. Samal D, Tan H, Molegraaf H, Kuiper B, Siemons W, Bals S, Verbeeck J, Van Tendeloo G, Takamura Y, Arenholz E, Jenkins CA, Rijnders G, Koster G, Physical review letters 111, 096102 (2013). http://doi.org/10.1103/PhysRevLett.111.096102
Abstract: A recent theoretical study [ Phys. Rev. B 85 121411(R) (2012)] predicted a thickness limit below which ideal polar cuprates turn nonpolar driven by the associated electrostatic instability. Here we demonstrate this possibility by inducing a structural transformation from the bulk planar to chainlike structure upon reducing the SrCuO2 repeat thickness in SrCuO2/SrTiO3 superlattices with unit-cell precision. Our results, based on structural investigation by x-ray diffraction and high resolution scanning transmission electron microscopy, demonstrate that the oxygen sublattice can essentially be built by design. In addition, the electronic structure of the chainlike structure, as studied by x-ray absorption spectroscopy, shows the signature for preferential hole occupation in the Cu 3d3z2-r2 orbital, which is different from the planar case.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 29
DOI: 10.1103/PhysRevLett.111.096102
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“Transport of intensity phase retrieval of arbitrary wave fields including vortices”. Lubk A, Guzzinati G, Börrnert F, Verbeeck J, Physical review letters 111, 173902 (2013). http://doi.org/10.1103/PhysRevLett.111.173902
Abstract: The phase problem can be considered as one of the cornerstones of quantum mechanics intimately connected to the detection process and the uncertainty relation. The latter impose fundamental limits on the manifold phase reconstruction schemes invented to date, in particular, at small magnitudes of the quantum wave. Here, we show that a rigorous solution of the transport of intensity reconstruction (TIE) scheme in terms of a linear elliptic partial differential equation for the phase provides reconstructions even in the presence of wave zeros if particular boundary conditions are given. We furthermore discuss how partial coherence hampers phase reconstruction and show that a modified version of the TIE reconstructs the curl-free current density at arbitrary (in)coherence. Our results open the way for TIE-based phase retrieval of arbitrary wave fields, eventually containing zeros such as phase vortices.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 40
DOI: 10.1103/PhysRevLett.111.173902
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“Casting light on the darkening of colors in historical paintings”. da Pieve F, Hogan C, Lamoen D, Verbeeck J, Vanmeert F, Radepont M, Cotte M, Janssens K, Gonze X, Van Tendeloo G, Physical review letters 111, 208302 (2013). http://doi.org/10.1103/PhysRevLett.111.208302
Abstract: The degradation of colors in historical paintings affects our cultural heritage in both museums and archeological sites. Despite intensive experimental studies, the origin of darkening of one of the most ancient pigments known to humankind, vermilion (α-HgS), remains unexplained. Here, by combining many-body theoretical spectroscopy and high-resolution microscopic x-ray diffraction, we clarify the composition of the damaged paint work and demonstrate possible physicochemical processes, induced by illumination and exposure to humidity and air, that cause photoactivation of the original pigment and the degradation of the secondary minerals. The results suggest a new path for the darkening process which was never considered by previous studies and prompt a critical examination of their findings.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 8.462
Times cited: 30
DOI: 10.1103/PhysRevLett.111.208302
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“Electron Microscopy of Probability Currents at Atomic Resolution”. Lubk A, Béché, A, Verbeeck J, Physical review letters 115, 176101 (2015). http://doi.org/10.1103/PhysRevLett.115.176101
Abstract: Atomic resolution transmission electron microscopy records the spatially resolved scattered electron density to infer positions, density, and species of atoms. These data are indispensable for studying the relation between structure and properties in solids. Here, we show how this signal can be augmented by the lateral probability current of the scattered electrons in the object plane at similar resolutions and fields of view. The currents are reconstructed from a series of three atomic resolution TEM images recorded under a slight difference of perpendicular line foci. The technique does not rely on the coherence of the electron beam and can be used to reveal electric, magnetic, and strain fields with incoherent electron beams as well as correlations in inelastic transitions, such as electron magnetic chiral dichroism.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 12
DOI: 10.1103/PhysRevLett.115.176101
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“Spin-orbit semimetal SrIrO3 in the two-dimensional limit”. Groenendijk DJ, Autieri C, Girovsky J, Martinez-Velarte MC, Manca N, Mattoni G, Monteiro AMRVL, Gauquelin N, Verbeeck J, Otte AF, Gabay M, Picozzi S, Caviglia AD, Physical review letters 119, 256403 (2017). http://doi.org/10.1103/PHYSREVLETT.119.256403
Abstract: <script type='text/javascript'>document.write(unpmarked('We investigate the thickness-dependent electronic properties of ultrathin SrIrO3 and discover a transition from a semimetallic to a correlated insulating state below 4 unit cells. Low-temperature magnetoconductance measurements show that spin fluctuations in the semimetallic state are significantly enhanced while approaching the transition point. The electronic properties are further studied by scanning tunneling spectroscopy, showing that 4 unit cell SrIrO(3)d is on the verge of a gap opening. Our density functional theory calculations reproduce the critical thickness of the transition and show that the opening of a gap in ultrathin SrIrO3 requires antiferromagnetic order.'));
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 79
DOI: 10.1103/PHYSREVLETT.119.256403
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“Electrical Polarization in AlN/GaN Nanodisks Measured by Momentum-Resolved 4D Scanning Transmission Electron Microscopy”. Müller-Caspary K, Grieb T, Müßener J, Gauquelin N, Hille P, Schörmann J, Verbeeck J, Van Aert S, Eickhoff M, Rosenauer A, Physical review letters 122, 106102 (2019). http://doi.org/10.1103/PhysRevLett.122.106102
Abstract: We report the mapping of polarization-induced internal electric fields in AlN/GaN nanowire heterostructures at unit cell resolution as a key for the correlation of optical and structural phenomena in semiconductor optoelectronics. Momentum-resolved aberration-corrected scanning transmission electron microscopy is employed as a new imaging mode that simultaneously provides four-dimensional data in real and reciprocal space. We demonstrate how internal mesoscale and atomic electric fields can be separated in an experiment, which is verified by comprehensive dynamical simulations of multiple electron scattering. A mean difference of 5.3 +- 1.5 MV/cm is found for the polarization-induced electric fields in AlN and GaN, being in accordance with dedicated simulations and photoluminescence measurements in previous publications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 26
DOI: 10.1103/PhysRevLett.122.106102
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“Coupling Charge and Topological Reconstructions at Polar Oxide Interfaces”. van Thiel T c, Brzezicki W, Autieri C, Hortensius J r, Afanasiev D, Gauquelin N, Jannis D, Janssen N, Groenendijk D j, Fatermans J, Van Aert S, Verbeeck J, Cuoco M, Caviglia A d, Physical Review Letters 127, 127202 (2021). http://doi.org/10.1103/PhysRevLett.127.127202
Abstract: In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion symmetry across the heterointerfaces. A notable example is the interface between polar and nonpolar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way for the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wave functions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO3, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and
LaAlO3, a polar wide-band-gap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO2/SrO interface configuration, leading to excess charge being pinned near the LaAlO3/SrRuO3 interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction drives a reorganization of the topological charges in the band structure, thereby modifying the momentum-space Berry curvature in SrRuO3. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.462
Times cited: 17
DOI: 10.1103/PhysRevLett.127.127202
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“Co valence transformation in isopolar LaCoO3/LaTiO3 perovskite heterostructures via interfacial engineering”. Araizi-Kanoutas G, Geessinck J, Gauquelin N, Smit S, Verbeek XH, Mishra SK, Bencok P, Schlueter C, Lee T-L, Krishnan D, Fatermans J, Verbeeck J, Rijnders G, Koster G, Golden MS, Physical review materials 4, 026001 (2020). http://doi.org/10.1103/PhysRevMaterials.4.026001
Abstract: We report charge transfer up to a single electron per interfacial unit cell across nonpolar heterointerfaces from the Mott insulator LaTiO3 to the charge transfer insulator LaCoO3. In high-quality bi- and trilayer systems grown using pulsed laser deposition, soft x-ray absorption, dichroism, and scanning transmission electron microscopy-electron energy loss spectroscopy are used to probe the cobalt-3d electron count and provide an element-specific investigation of the magnetic properties. The experiments show the cobalt valence conversion is active within 3 unit cells of the heterointerface, and able to generate full conversion to 3d7 divalent Co, which displays a paramagnetic ground state. The number of LaTiO3/LaCoO3 interfaces, the thickness of an additional, electronically insulating “break” layer between the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself in trilayers provide a trio of control knobs for average charge of the cobalt ions in LaCoO3, illustrating the efficacy of O−2p band alignment as a guiding principle for property design in complex oxide heterointerfaces.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.4
Times cited: 13
DOI: 10.1103/PhysRevMaterials.4.026001
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“Two-dimensional electron systems in perovskite oxide heterostructures : role of the polarity-induced substitutional defects”. Lin S-C, Kuo C-T, Shao Y-C, Chuang Y-D, Geessinck J, Huijben M, Rueff J-P, Graff IL, Conti G, Peng Y, Bostwick A, Gullikson E, Nemsak S, Vailionis A, Gauquelin N, Verbeeck J, Ghiringhelli G, Schneider CM, Fadley CS, Physical review materials 4, 115002 (2020). http://doi.org/10.1103/PHYSREVMATERIALS.4.115002
Abstract: The discovery of a two-dimensional electron system (2DES) at the interfaces of perovskite oxides such as LaAlO3 and SrTiO3 has motivated enormous efforts in engineering interfacial functionalities with this type of oxide heterostructures. However, the fundamental origins of the 2DES are still not understood, e.g., the microscopic mechanisms of coexisting interface conductivity and magnetism. Here we report a comprehensive spectroscopic investigation on the depth profile of 2DES-relevant Ti 3d interface carriers using depthand element-specific techniques like standing-wave excited photoemission and resonant inelastic scattering. We found that one type of Ti 3d interface carriers, which give rise to the 2DES are located within three unit cells from the n-type interface in the SrTiO3 layer. Unexpectedly, another type of interface carriers, which are polarity-induced Ti-on-Al antisite defects, reside in the first three unit cells of the opposing LaAlO3 layer (similar to 10 angstrom). Our findings provide a microscopic picture of how the localized and mobile Ti 3d interface carriers distribute across the interface and suggest that the 2DES and 2D magnetism at the LaAlO3/SrTiO3 interface have disparate explanations as originating from different types of interface carriers.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.4
Times cited: 7
DOI: 10.1103/PHYSREVMATERIALS.4.115002
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“Resistance minimum in LaAlO3/Eu1-xLaxTiO3/SrTiO3 heterostructures”. Lebedev N, Huang Y, Rana A, Jannis D, Gauquelin N, Verbeeck J, Aarts J, Physical review materials 6, 075003 (2022). http://doi.org/10.1103/PHYSREVMATERIALS.6.075003
Abstract: In this paper we study LaAlO3/Eu1-xLaxTiO3/SrTiO3 structures with nominally x = 0, 0.1 and different thicknesses of the Eu1-xLaxTiO3 layer. We observe that both systems have many properties similar to previously studied LaAlO3/EuTiO3/SrTiO3 and other oxide interfaces, such as the formation of a two-dimensional electron liquid for two unit cells of Eu1-xLaxTiO3; a metal-insulator transition driven by the increase in thickness of the Eu1-xLaxTiO3 layer; the presence of an anomalous Hall effect when driving the systems above the Lifshitz point with a back-gate voltage; and a minimum in the temperature dependence of the sheet resistance below the Lifshitz point in the one-band regime, which becomes more pronounced with increasing negative gate voltage. However, and notwithstanding the likely presence of magnetism in the system, we do not attribute that minimum to the Kondo effect, but rather to the properties of the SrTiO3 crystal and the inevitable effects of charge trapping when using back gates.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.4
DOI: 10.1103/PHYSREVMATERIALS.6.075003
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“Unusual structural rearrangement and superconductivity in infinite layer cuprate superlattices”. Samal D, Gauquelin N, Takamura Y, Lobato I, Arenholz E, Van Aert S, Huijben M, Zhong Z, Verbeeck J, Van Tendeloo G, Koster G, Physical review materials 7, 054803 (2023). http://doi.org/10.1103/PhysRevMaterials.7.054803
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.4
DOI: 10.1103/PhysRevMaterials.7.054803
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“Berry phase engineering at oxide interfaces”. Groenendijk DJ, Autieri C, van Thiel TC, Brzezicki W, Hortensius JR, Afanasiev D, Gauquelin N, Barone P, van den Bos KHW, van Aert S, Verbeeck J, Filippetti A, Picozzi S, Cuoco M, Caviglia AD, 2, 023404 (2020). http://doi.org/10.1103/PhysRevResearch.2.023404
Abstract: Three-dimensional strontium ruthenate (SrRuO3) is an itinerant ferromagnet that features Weyl points acting as sources of emergent magnetic fields, anomalous Hall conductivity, and unconventional spin dynamics. Integrating SrRuO3 in oxide heterostructures is potentially a novel route to engineer emergent electrodynamics, but its electronic band topology in the two-dimensional limit remains unknown. Here we show that ultrathin SrRuO3 exhibits spin-polarized topologically nontrivial bands at the Fermi energy. Their band anticrossings show an enhanced Berry curvature and act as competing sources of emergent magnetic fields. We control their balance by designing heterostructures with symmetric (SrTiO3/SrRuO3/SrTiO3 and SrIrO3/SrRuO3/SrIrO3) and asymmetric interfaces (SrTiO3/SrRuO3/SrIrO3). Symmetric structures exhibit an interface-tunable single-channel anomalous Hall effect, while ultrathin SrRuO3 embedded in asymmetric structures shows humplike features consistent with multiple Hall contributions. The band topology of two-dimensional SrRuO3 proposed here naturally accounts for these observations and harmonizes a large body of experimental results.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 58
DOI: 10.1103/PhysRevResearch.2.023404
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“Electron vortex beams in a magnetic field : a new twist on Landau levels and Aharonov-Bohm states”. Bliokh KY, Schattschneider P, Verbeeck J, Nori F, Physical review X 2, 041011 (2012). http://doi.org/10.1103/PhysRevX.2.041011
Abstract: We examine the propagation of the recently discovered electron vortex beams in a longitudinal magnetic field. We consider both the Aharonov-Bohm configuration with a single flux line and the Landau case of a uniform magnetic field. While stationary Aharonov-Bohm modes represent Bessel beams with flux- and vortex-dependent probability distributions, stationary Landau states manifest themselves as nondiffracting Laguerre-Gaussian beams. Furthermore, the Landau-state beams possess field- and vortex-dependent phases: (i) the Zeeman phase from coupling the quantized angular momentum to the magnetic field and (ii) the Gouy phase, known from optical Laguerre-Gaussian beams. Remarkably, together these phases determine the structure of Landau energy levels. This unified Zeeman-Landau-Gouy phase manifests itself in a nontrivial evolution of images formed by various superpositions of modes. We demonstrate that, depending on the chosen superposition, the image can rotate in a magnetic field with either (i) Larmor, (ii) cyclotron (double-Larmor), or (iii) zero frequency. At the same time, its centroid always follows the classical cyclotron trajectory, in agreement with the Ehrenfest theorem. Interestingly, the nonrotating superpositions reproduce stable multivortex configurations that appear in rotating superfluids. Our results open an avenue for the direct electron-microscopy observation of fundamental properties of free quantum-electron states in magnetic fields.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 12.789
Times cited: 130
DOI: 10.1103/PhysRevX.2.041011
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“TEM and AES investigations of the natural surface nano-oxide layer of an AISI 316L stainless steel microfibre”. Ramachandran D, Egoavil R, Crabbe A, Hauffman T, Abakumov A, Verbeeck J, Vandendael I, Terryn H, Schryvers D, Journal of microscopy 264, 207 (2016). http://doi.org/10.1111/jmi.12434
Abstract: The chemical composition, nanostructure and electronic structure of nanosized oxide scales naturally formed on the surface of AISI 316L stainless steel microfibres used for strengthening of composite materials have been characterised using a combination of scanning and transmission electron microscopy with energy-dispersive X-ray, electron energy loss and Auger spectroscopy. The analysis reveals the presence of three sublayers within the total surface oxide scale of 5.0-6.7 nm thick: an outer oxide layer rich in a mixture of FeO.Fe2 O3 , an intermediate layer rich in Cr2 O3 with a mixture of FeO.Fe2 O3 and an inner oxide layer rich in nickel.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.692
Times cited: 12
DOI: 10.1111/jmi.12434
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“Induced giant piezoelectricity in centrosymmetric oxides”. Park D-s, Hadad M, Riemer LM, Ignatans R, Spirito D, Esposito V, Tileli V, Gauquelin N, Chezganov D, Jannis D, Verbeeck J, Gorfman S, Pryds N, Muralt P, Damjanovic D, Science 375, 653 (2022). http://doi.org/10.1126/science.abm7497
Abstract: Giant piezoelectricity can be induced in centrosymmetric oxides by controlling the long-range motion of oxygen vacancies.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 56.9
Times cited: 51
DOI: 10.1126/science.abm7497
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“Deeper insights into the photoluminescence properties and (photo)chemical reactivity of cadmium red (CdS1-xSex) paints in renowned twentieth century paintings by state-of-the-art investigations at multiple length scales”. Monico L, Rosi F, Vivani R, Cartechini L, Janssens K, Gauquelin N, Chezganov D, Verbeeck J, Cotte M, D'Acapito F, Barni L, Grazia C, Buemi LP, Andral J-L, Miliani C, Romani A, The European Physical Journal Plus 137, 311 (2022). http://doi.org/10.1140/EPJP/S13360-022-02447-7
Abstract: Cadmium red is the name used for denoting a class of twentieth century artists' pigments described by the general formula CdS1-xSex. For their vibrant hues and excellent covering power, a number of renowned modern and contemporary painters, including Jackson Pollock, often used cadmium reds. As direct band gap semiconductors, CdS1-xSex compounds undergo direct radiative recombination (with emissions from the green to orange region) and radiative deactivation from intragap trapping states due to crystal defects, which give rise to two peculiar red-NIR emissions, known as deep level emissions (DLEs). The positions of the DLEs mainly depend on the Se content of CdS1-xSex; thus, photoluminescence and diffuse reflectance vis-NIR spectroscopy have been profitably used for the non-invasive identification of different cadmium red varieties in artworks over the last decade. Systematic knowledge is however currently lacking on what are the parameters related to intrinsic crystal defects of CdS1-xSex and environmental factors influencing the spectral properties of DLEs as well as on the overall (photo)chemical reactivity of cadmium reds in paint matrixes. Here, we present the application of a novel multi-length scale and multi-method approach to deepen insights into the photoluminescence properties and (photo)chemical reactivity of cadmium reds in oil paintings by combining both well established and new non-invasive/non-destructive analytical techniques, including macro-scale vis-NIR and vibrational spectroscopies and micro-/nano-scale advanced electron microscopy mapping and X-ray methods employing synchrotron radiation and conventional sources. Macro-scale vis-NIR spectroscopy data obtained from the in situ non-invasive analysis of nine masterpieces by Gerardo Dottori, Jackson Pollock and Nicolas de Stael allowed classifying the CdS1-xSex-paints in three groups, according to the relative intensity of the two DLE bands. These outcomes, combined with results from micro-/nano-scale electron microscopy mapping and X-ray analysis of a set of CdS1-xSex powders and artificially aged paint mock-ups, indicated that the relative intensity of DLEs is not affected by the morphology, microstructure and local atomic environment of the pigment particles but it is influenced by the presence of moisture. Furthermore, the extensive study of artificially aged oil paint mock-ups permitted us to provide first evidence of the tendency of cadmium reds toward photo-degradation and to establish that the conversion of CdS1-xSex to CdSO4 and/or oxalates is triggered by the oil binding medium and moisture level and depends on the Se content. Based on these findings, we could interpret the localized presence of CdSO4 and cadmium oxalate as alteration products of the original cadmium red paints in two paintings by Pollock.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 3.4
Times cited: 3
DOI: 10.1140/EPJP/S13360-022-02447-7
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“Spin effects in electron vortex states”. Van Boxem R, Verbeeck J, Partoens B, Europhysics letters 102, 40010 (2013). http://doi.org/10.1209/0295-5075/102/40010
Abstract: The recent experimental realization of electron vortex beams opens up a wide research domain previously unexplored. The present paper explores the relativistic properties of these electron vortex beams, and quantifies deviations from the scalar wave theory. It is common in electron optics to use the Schrodinger equation neglecting spin. The present paper investigates the role of spin and the total angular momentum J(z) and how it pertains to the vortex states. As an application, we also investigate if it is possible to use holographic reconstruction to create novel total angular momentum eigenstates in a transmission electron microscope. It is demonstrated that relativistic spin coupling effects disappear in the paraxial limit, and spin effects in holographically created electron vortex beams can only be exploited by using specialized magnetic apertures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT)
Impact Factor: 1.957
Times cited: 11
DOI: 10.1209/0295-5075/102/40010
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“Direct structural and spectroscopic investigation of ultrathin films of tetragonal CuO: Six-fold coordinated copper”. Samal D, Tan H, Takamura Y, Siemons W, Verbeeck J, Van Tendeloo G, Arenholz E, Jenkins CA, Rijnders G, Koster G, Europhysics letters 105, 17003 (2014). http://doi.org/10.1209/0295-5075/105/17003
Abstract: Unlike other 3d transition metal monoxides (MnO, FeO, CoO, and NiO), CuO is found in a low-symmetry distorted monoclinic structure rather than the rocksalt structure. We report here of the growth of ultrathin CuO films on SrTiO3 substrates; scanning transmission electron microscopy was used to show the stabilization of a tetragonal rocksalt structure with an elongated c-axis such that c/a similar to 1.34 and the Cu-O-Cu bond angle similar to 180 degrees, pointing to metastable six-fold coordinated Cu. X-ray absorption spectroscopy demonstrates that the hole at the Cu site for the CuO is localized in 3d(x2-y2) orbital unlike the well-studied monoclinic CuO phase. The experimental confirmation of the tetragonal structure of CuO opens up new avenues to explore electronic and magnetic properties of six-fold coordinated Cu. Copyright (C) EPLA, 2014
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 1.957
Times cited: 15
DOI: 10.1209/0295-5075/105/17003
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“Linearized radially polarized light for improved precision in strain measurements using micro-Raman spectroscopy”. Prabhakara V, Nuytten T, Bender H, Vandervorst W, Bals S, Verbeeck J, Optics Express 29, 34531 (2021). http://doi.org/10.1364/OE.434726
Abstract: Strain engineering in semiconductor transistor devices has become vital in the semiconductor industry due to the ever-increasing need for performance enhancement at the nanoscale. Raman spectroscopy is a non-invasive measurement technique with high sensitivity to mechanical stress that does not require any special sample preparation procedures in comparison to characterization involving transmission electron microscopy (TEM), making it suitable for inline strain measurement in the semiconductor industry. Indeed, at present, strain measurements using Raman spectroscopy are already routinely carried out in semiconductor devices as it is cost effective, fast and non-destructive. In this paper we explore the usage of linearized radially polarized light as an excitation source, which does provide significantly enhanced accuracy and precision as compared to linearly polarized light for this application. Numerical simulations are done to quantitatively evaluate the electric field intensities that contribute to this enhanced sensitivity. We benchmark the experimental results against TEM diffraction-based techniques like nano-beam diffraction and Bessel diffraction. Differences between both approaches are assigned to strain relaxation due to sample thinning required in TEM setups, demonstrating the benefit of Raman for nondestructive inline testing.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.307
Times cited: 2
DOI: 10.1364/OE.434726
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“Preparation, structural and optical characterization of nanocrystalline ZnO doped with luminescent Ag-nanoclusters”. Kuznetsov AS, Lu Y-G, Turner S, Shestakov MV, Tikhomirov VK, Kirilenko D, Verbeeck J, Baranov AN, Moshchalkov VV, Optical materials express 2, 723 (2012). http://doi.org/10.1364/OME.2.000723
Abstract: Nanocrystalline ZnO doped with Ag-nanoclusters has been synthesized by a salt solid state reaction. Three overlapping broad emission bands due to the Ag nanoclusters have been detected at about 570, 750 and 900 nm. These emission bands are excited by an energy transfer from the exciton state of the ZnO host when pumped in the wavelength range from 250 to 400 nm. The 900 nm emission band shows characteristic orbital splitting into three components pointing out that the anisotropic crystalline wurtzite host of ZnO is responsible for this feature. Heat-treatment and temperature dependence studies confirm the origin of these emission bands. An energy level diagram for the emission process and a model for Ag nanoclusters sites are suggested. The emission of nanocrystalline ZnO doped with Ag nanoclusters may be applied for white light generation, displays driven by UV light, down-convertors for solar cells and luminescent lamps.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.591
DOI: 10.1364/OME.2.000723
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“Layered oxygen vacancy ordering in Nb-doped SrCo1-xFexO3-\delta perovskite”. Van Rompaey S, Dachraoui W, Turner S, Podyacheva OY, Tan H, Verbeeck J, Abakumov A, Hadermann J, Zeitschrift für Kristallographie 228, 28 (2013). http://doi.org/10.1524/zkri.2013.1556
Abstract: The crystal structure of SrCo0.7Fe0.2Nb0.1O2.72 was determined using a combination of precession electron diffraction (PED), high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and spatially resolved electron energy loss spectroscopy (STEM-EELS). The structure has a tetragonal P4/mmm symmetry with cell parameters a = b = a(p), c = 2a(p) (a(p) being the cell parameter of the perovskite parent structure). Octahedral BO2 layers alternate with the anion-deficient BO1.4 layers, the different B cations are randomly distributed over both layers. The specific feature of the SrCo0.7Fe0.2NB0.1O2.72 microstructure is a presence of extensive nanoscale twinning resulting in domains with alignment of the tetragonal c-axis along all three cubic direction of the perovskite subcell.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.179
Times cited: 9
DOI: 10.1524/zkri.2013.1556
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“Quantum wavefront shaping with a 48-element programmable phase plate for electrons”. Yu CP, Vega Ibañez F, Béché, A, Verbeeck J, SciPost Physics 15, 223 (2023). http://doi.org/10.21468/SciPostPhys.15.6.223
Abstract: We present a 48-element programmable phase plate for coherent electron waves produced by a combination of photolithography and focused ion beam. This brings the highly successful concept of wavefront shaping from light optics into the realm of electron optics and provides an important new degree of freedom to prepare electron quantum states. The phase plate chip is mounted on an aperture rod placed in the C2 plane of a transmission electron microscope operating in the 100-300 kV range. The phase plate's behavior is characterized by a Gerchberg-Saxton algorithm, showing a phase sensitivity of 0.075 rad/mV at 300 kV, with a phase resolution of approximately 3x10e−3π. In addition, we provide a brief overview of possible use cases and support it with both simulated and experimental results.
Keywords: A1 Journal Article; Electron Microscopy for Materials Science (EMAT)
Impact Factor: 5.5
Times cited: 1
DOI: 10.21468/SciPostPhys.15.6.223
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“Asymmetric Interfacial Intermixing Associated Magnetic Coupling in LaMnO3/LaFeO3 Heterostructures”. Chen B, Gauquelin N, Green RJ, Verbeeck J, Rijnders G, Koster G, Frontiers in physics 9 (2021). http://doi.org/10.3389/fphy.2021.698154
Abstract: The structural and magnetic properties of LaMnO<sub>3</sub>/LaFeO<sub>3</sub>(LMO/LFO) heterostructures are characterized using a combination of scanning transmission electron microscopy, electron energy-loss spectroscopy, bulk magnetometry, and resonant x-ray reflectivity. Unlike the relatively abrupt interface when LMO is deposited on top of LFO, the interface with reversed growth order shows significant cation intermixing of Mn<sup>3+</sup>and Fe<sup>3+</sup>, spreading ∼8 unit cells across the interface. The asymmetric interfacial chemical profiles result in distinct magnetic properties. The bilayer with abrupt interface shows a single magnetic hysteresis loop with strongly enhanced coercivity, as compared to the LMO plain film. However, the bilayer with intermixed interface shows a step-like hysteresis loop, associated with the separate switching of the “clean” and intermixed LMO sublayers. Our study illustrates the key role of interfacial chemical profile in determining the functional properties of oxide heterostructures.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 1
DOI: 10.3389/fphy.2021.698154
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