On stoichiometry and intermixing at the spinel/perovskite interface in CoFe2O4/BaTiO3 thin films

The performance of complex oxide heterostructures depends primarily on the interfacial coupling of the two component structures. This interface character inherently varies with the synthesis method and conditions used since even small composition variations can alter the electronic, ferroelectric, or magnetic functional properties of the system. The focus of this article is placed on the interface character of a pulsed laser deposited CoFe2O4/BaTiO3 thin film. Using a range of state-of-the-art transmission electron microscopy methodologies, the roles of substrate morphology, interface stoichiometry, and cation intermixing are determined on the atomic level. The results reveal a surprisingly uneven BaTiO3 substrate surface formed after the film deposition and Fe atom incorporation in the top few monolayers inside the unit cell of the BaTiO3 crystal. Towards the CoFe2O4 side, a disordered region extending several nanometers from the interface was revealed and both Ba and Ti from the substrate were found to diffuse into the spinel layer. The analysis also shows that within this somehow incompatible composite interface, a different phase is formed corresponding to the compound Ba2Fe3Ti5O15, which belongs to the ilmenite crystal structure of FeTiO3 type. The results suggest a chemical activity between these two oxides, which could lead to the synthesis of complex engineered interfaces

Direct measurement of the charge distribution along a biased carbon nanotube bundle using electron holography

Nanowires and nanotubes can be examined in the transmission electron microscope under an applied bias. Here we introduce a model-independent method, which allows the charge distribution along a nanowire or nanotube to be measured directly from the Laplacian of an electron holographic phase image. We present results from a biased bundle of carbon nanotubes, in which we show that the charge density increases linearly with distance from its base, reaching a value of similar to 0.8 electrons/nm near its tip. (C) 2011 American Institute of Physics. [doi:10.1063/1.3598468

Observation of thermally-induced magnetic relaxation in a magnetite grain using off-axis electron holography

A synthetic basalt comprising magnetic Fe3O4 grains (~ 50 nm to ~ 500 nm in diameter) is investigated using a range of complementary nano-characterisation techniques. Off-axis electron holography combined with in situ heating allowed for the visualisation of the thermally-induced magnetic relaxation of an Fe3O4 grain (~ 300 nm) from an irregular domain state into a vortex state at 550˚C, just below its Curie temperature, with the magnetic intensity of the vortex increasing on cooling

Eigenmode Tomography of Surface Charge Oscillations of Plasmonic Nanoparticles by Electron Energy Loss Spectroscopy

Plasmonic devices designed in three dimensions enable careful tuning of optical responses for control of complex electromagnetic interactions on the nanoscale. Probing the fundamental characteristics of the constituent nanoparticle building blocks is, however, often constrained by diffraction-limited spatial resolution in optical spectroscopy. Electron microscopy techniques, including electron energy loss spectroscopy (EELS), have recently been developed to image surface plasmon resonances qualitatively at the nanoscale in three dimensions using tomographic reconstruction techniques. Here, we present an experimental realization of a distinct method that uses direct analysis of modal surface charge distributions to reconstruct quantitatively the three-dimensional eigenmodes of a silver right bipyramid on a metal oxide substrate. This eigenmode tomography removes ambiguity in two-dimensional imaging of spatially-localized plasmonic resonances, reveals substrate-induced mode degeneracy breaking in the bipyramid, and enables EELS for the analysis not of a particular electron-induced response but of the underlying geometric modes characteristic of particle surface plasmons.S.M.C. acknowledges support of a Gates Cambridge Scholarship. E.R. acknowledges support from the Royal Society's Newton International Fellowship scheme and a Trinity Hall Research Fellowship. We thank Ben Knappet for assistance with the synthesis of the silver bipyramids. We thank F.J. de la Peña for helpful discussions on the use of HYPERSPY. The research leading to these results has received funding from the European Research Council under the European Union's Seventh Framework Program (No. FP7/2007-2013)/ERC Grant Agreement No. 291522-3DIMAGE and the European Union's Seventh Framework Program under a contract for an Integrated Infrastructure Initiative (Reference No. 312483-ESTEEM2)This is the final version of the article. It was first available from ACS via http://dx.doi.org/10.1021/acsphotonics.5b0042

In situ transmission electron microscopy of resistive switching in thin silicon oxide layers

Silicon oxide-based resistive switching devices show great potential for applications in nonvolatile random access memories. We expose a device to voltages above hard breakdown and show that hard oxide breakdown results in mixing of the SiOx layer and the TiN lower contact layers. We switch a similar device at sub-breakdown fields in situ in the transmission electron microscope (TEM) using a movable probe and study the diffusion mechanism that leads to resistance switching. By recording bright-field (BF) TEM movies while switching the device, we observe the creation of a filament that is correlated with a change in conductivity of the SiOx layer. We also examine a device prepared on a microfabricated chip and show that variations in electrostatic potential in the SiOx layer can be recorded using off-axis electron holography as the sample is switched in situ in the TEM. Taken together, the visualization of compositional changes in ex situ stressed samples and the simultaneous observation of BF TEM contrast variations, a conductivity increase, and a potential drop across the dielectric layer in in situ switched devices allow us to conclude that nucleation of the electroforming—switching process starts at the interface between the SiOx layer and the lower contact

Visualized effect of oxidation on magnetic recording fidelity in pseudo-single-domain magnetite particles

Magnetite (​Fe3O4) is an important magnetic mineral to Earth scientists, as it carries the dominant magnetic signature in rocks, and the understanding of its magnetic recording fidelity provides a critical tool in the field of palaeomagnetism. However, reliable interpretation of the recording fidelity of ​Fe3O4 particles is greatly diminished over time by progressive oxidation to less magnetic iron oxides, such as maghemite (γ-Fe2O3), with consequent alteration of remanent magnetization potentially having important geological significance. Here we use the complementary techniques of environmental transmission electron microscopy and off-axis electron holography to induce and visualize the effects of oxidation on the magnetization of individual nanoscale ​Fe3O4 particles as they transform towards γ-Fe2O3. Magnetic induction maps demonstrate a change in both strength and direction of remanent magnetization within ​Fe3O4 particles in the size range dominant in rocks, confirming that oxidation can modify the original stored magnetic information

Carrier localization in the vicinity of dislocations in InGaN

We present a multi-microscopy study of dislocations in InGaN, whereby the same threading dislocation was observed under several microscopes (atomic force microscopy, scanning electron microscopy, cathodoluminescence imaging and spectroscopy, transmission electron microscopy), and its morphological optical and structural properties directly correlated. We achieved this across an ensemble of defects large enough to be statistically significant. Our results provide evidence that carrier localization occurs in the direct vicinity of the dislocation through the enhanced formation of In-N chains and atomic condensates, thus limiting non-radiative recombination of carriers at the dislocation core. We highlight that the localization properties in the vicinity of threading dislocations arise as a consequence of the strain field of the individual dislocation and the additional strain field building between interacting neighboring dislocations. Our study therefore suggests that careful strain and dislocation distribution engineering may further improve the resilience of InGaN-based devices to threading dislocations. Besides providing a new understanding of dislocations in InGaN, this paper presents a proof-of-concept for a methodology which is relevant to many problems in materials science.This project is funded in part by the European Research Council under the European Community's Seventh Framework Programme (FP7/2007-2013)/ERC Grant Agreement No. 279361 (MACONS). The research leading to these results has received funding from the European Union Seventh Framework Programme under Grant Agreement 312483-ESTEEM2 (Integrated Infrastructure InitiativeI3). F.M. would also like to acknowledge the financial support from EPSRC Doctoral Prize Awards and Cambridge Philosophical Society. M.H. would like to acknowledge support from the Lindemann Fellowship

Alloy fluctuations at dislocations in III-Nitrides: identification and impact on optical properties

We investigated alloy fluctuations at dislocations in III-Nitride alloys (InGaN and AlGaN). We found that in both alloys, atom segregation (In segregation in InGaN and Ga segregation in AlGaN) occurs in the tensile part of dislocations with an edge component. In InGaN, In atom segregation leads to an enhanced formation of In-N chains and atomic condensates which act as carrier localization centers. This feature results in a bright spot at the position of the dislocation in the CL images, suggesting that non-radiative recombination at dislocations is impaired. On the other hand, Ga atom segregation at dislocations in AlGaN does not seem to noticeably affect the intensity recorded by CL at the dislocation. This study sheds light on why InGaN-based devices are more resilient to dislocations than AlGaN-based devices. An interesting approach to hinder non-radiative recombination at dislocations may therefore be to dope AlGaN with In.ER

The impact of trench defects in InGaN/GaN light emitting diodes and implications for the "green gap" problem

The impact of trench defects in blue InGaN/GaN light emitting diodes (LEDs) has been investigated. Two mechanisms responsible for the structural degradation of the multiple quantum well (MQW) active region were identified. It was found that during the growth of the p-type GaN capping layer, loss of part of the active region enclosed within a trench defect occurred, affecting the top-most QWs in the MQW stack. Indium platelets and voids were also found to form preferentially at the bottom of the MQW stack. The presence of high densities of trench defects in the LEDs was found to relate to a significant reduction in photoluminescence and electroluminescence emission efficiency, for a range of excitation power densities and drive currents. This reduction in emission efficiency was attributed to an increase in the density of non-radiative recombination centres within the MQW stack, believed to be associated with the stacking mismatch boundaries which form part of the sub-surface structure of the trench defects. Investigation of the surface of green-emitting QW structures found a two decade increase in the density of trench defects, compared to its blue-emitting counterpart, suggesting that the efficiency of green-emitting LEDs may be strongly affected by the presence of these defects. Our results are therefore consistent with a model that the “green gap” problem might relate to localized strain relaxation occurring through defects.This is the accepted manuscript version. The final version is available from AIP at http://scitation.aip.org/content/aip/journal/apl/105/11/10.1063/1.4896279?showFTTab=true&containerItemId=content/aip/journal/apl