Daniel Gilks

Atomic-scale structure and properties of highly stable antiphase boundary defects in Fe3O4

The complex and intriguing properties of the ferrimagnetic half metal magnetite (Fe3O4) are of continuing fundamental interest as well as being important for practical applications in spintronics, magnetism, catalysis and medicine. There is considerable speculation concerning the role of the ubiquitous antiphase boundary (APB) defects in magnetite, however, direct information on their structure and properties has remained challenging to obtain. Here we combine predictive first principles modelling with high-resolution transmission electron microscopy to unambiguously determine the three-dimensional structure of APBs in magnetite. We demonstrate that APB defects on the {110} planes are unusually stable and induce antiferromagnetic coupling between adjacent domains providing an explanation for the magnetoresistance and reduced spin polarization often observed. We also demonstrate how the high stability of the {110} APB defects is connected to the existence of a metastable bulk phase of Fe3O4, which could be stabilized by strain in films or nanostructures.

Origin of anomalous magnetite properties in crystallographic matched heterostructures: Fe3O4(111)/MgAl2O4(111)

Magnetite films grown on crystallographically matched substrates such as MgAl2O4 are not expected to show anomalous properties such as negative magnetoresistance and high saturation fields. By atomic resolution imaging using scanning transmission electron microscopy we show direct evidence of anti-phase domain boundaries (APB) present in these heterostructures. Experimentally identified 1/4<101> shifts determine the atomic structure of the observed APBs. The dominant non-bulk superexchange interactions are between 180° octahedral-Fe/O/octahedral-Fe sites which provide strong antiferromagnetic coupling across the defect interface resulting in non-bulk magnetic and magnetotransport properties.

Magnetism and magnetotransport in symmetry matched spinels: Fe3O4/MgAl2O4

In this work, we show that Fe3O4 films grown by oxygen plasma assisted molecular beam epitaxy have anomalous magnetic properties such as negative magnetoresistance and high saturation magnetic fields. The film substrate mismatch of 3% is relieved by the formation of misfit dislocations at the interface. Transmission electron microscopy results show that misfit dislocations are not the cause of antiphase domain boundary (APB). This suggests that in this system APB formation is a property of the three dimensional Fe3O4 growth.

The Effect of Cobalt-Sublattice Disorder on Spin Polarisation in Co2FexMn1−xSi Heusler Alloys

In this work we present a theoretical study of the effect of disorder on spin polarisation at the Fermi level, and the disorder formation energies for Co2FexMn1−xSi (CFMS) alloys. The electronic calculations are based on density functional theory with a Hubbard U term. Chemical disorders studied consist of swapping Co with Fe/Mn and Co with Si; in all cases we found these are detrimental for spin polarisation, i.e., the spin polarisation not only decreases in magnitude, but also can change sign depending on the particular disorder. Formation energy calculation shows that Co–Si disorder has higher energies of formation in CFMS compared to Co2MnSi and Co2FeSi, with maximum values occurring for x in the range 0.5–0.75. Cross-sectional structural studies of reference Co2MnSi, Co2Fe0.5Mn0.5Si, and Co2FeSi by Z-contrast scanning transmission electron microscopy are in qualitative agreement with total energy calculations of the disordered structures.

Structural study of Fe3O4(111) thin films with bulk like magnetic and magnetotransport behaviour

Post-annealing of Fe3O4 films in a CO/CO2 atmosphere results in a significant improvement in magnetic and magnetotransport properties with values close to the single crystal bulk of Ms ∼ 480 emu/cm3 and negative magnetoresistance of 0.05% in a field of 1 T. By using atomic resolution Z-contrast transmission electron microscopy, we show that improved magnetic properties in the annealed films are due to improved structural ordering as a result of the annealing process.

Correlations between atomic structure and giant magnetoresistance ratio in Co2(Fe,Mn)Si spin valves

We show that the magnetoresistance of Co2FexMn1?xSi-based spin valves, over 70% at low temperature, is directly related to the structural ordering in the electrodes and at the electrodes/spacer (Co2FexMn1?xSi/Ag) interfaces. Aberration-corrected atomic resolution Z-contrast scanning transmission electron microscopy of device structures reveals that annealing at 350??C and 500??C creates partial B2/L21 and fully L21 ordering of electrodes, respectively. Interface structural studies show that the Ag/Co2FexMn1?xSi interface is more ordered compared to the Co2FexMn1?xSi/Ag interface. The release of interface strain is mediated by misfit dislocations that localize the strain around the dislocation cores, and the effect of this strain is assessed by first principles electronic structure calculations. This study suggests that by improving the atomic ordering and strain at the interfaces, further enhancement of the magnetoresistance of CFMS-based current-perpendicular-to-plane spin valves is possible.

Atomic and electronic structure of twin growth defects in magnetite

We report the existence of a stable twin defect in Fe3O4 thin films. By using aberration corrected scanning transmission electron microscopy and spectroscopy the atomic structure of the twin boundary has been determined. The boundary is confined to the (111) growth plane and it is non-stoichiometric due to a missing Fe octahedral plane. By first principles calculations we show that the local atomic structural configuration of the twin boundary does not change the nature of the superexchange interactions between the two Fe sublattices across the twin grain boundary. Besides decreasing the half-metallic band gap at the boundary the altered atomic stacking at the boundary does not change the overall ferromagnetic (FM) coupling between the grains.

STEM and EELS study of the Graphene/Bi 2 Se 3 Interface

SuperSTEM Laboratory, STFC Daresbury Campus, Warrington, WA4 4AD, UK Department of Physics, University of York, Heslington, York, YO10 5DD, UK, York JEOL Nanocentre, University of York, Heslington, York, YO10 5BR, UK 4 Department of Computer Science and Engineering, Universidad de Cádiz, 11510 Puerto Real, Spain University of Wisconsin Milwaukee, Milwaukee, 53211,WI, USA 6 Institute for microelectronics and microsystems, CNR Catania, 95121 Catania CT, Sicilia, Italy

Effects of spin doping and spin injection in the luminescence and vibrational spectrum of C60

We have studied the Raman spectrum and photoemission of hybrid magneto-fullerene devices. For C60 layers on cobalt, the spin polarized electron transfer shifts the photoemission energy, reducing the zero phonon contribution. The total luminescence of hybrid devices can be controlled via spin injection from magnetic electrodes, with changes of the order of 10%–20% at room temperature. Spin polarised currents alter as well the Raman spectrum of the molecules, enhancing some modes by a factor 5 while shifting others by several wavenumbers due to a spin-dependent hopping time and/or enhanced intermolecular interactions. These results can be used to measure spin polarisation in molecules or to fabricate magneto-optic and magneto-vibrational devices.

Polar Spinel-Perovskite Interfaces: an atomistic study of Fe3O4(111)/SrTiO3(111) structure and functionality

Atomic resolution scanning transmission electron microscopy and electron energy loss spectroscopy combined with ab initio electronic calculations are used to determine the structure and properties of the Fe3O4(111)/SrTiO3(111) polar interface. The interfacial structure and chemical composition are shown to be atomically sharp and of an octahedral Fe/SrO3 nature. Band alignment across the interface pins the Fermi level in the vicinity of the conduction band of SrTiO3. Density functional theory calculations demonstrate very high spin-polarization of Fe3O4 in the interface vicinity which suggests that this system may be an excellent candidate for spintronic applications.