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Register a new userUltrathin oxides: bulk-oxide-like model surfaces or unique films?
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Added by
Christoph Freysoldt
Publication date
2007
fields
Physics
and research's language is
English
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To better understand the electronic and chemical properties of wide-gap oxide surfaces at the atomic scale, experimental work has focused on epitaxial films on metal substrates. Recent findings show that these films are considerably thinner than previously thought. This raises doubts about the transferability of the results to surface properties of thicker films and bulk crystals. By means of density-functional theory and approximate GW corrections for the electronic spectra we demonstrate for three characteristic wide-gap oxides (silica, alumina, and hafnia) the influence of the substrate and highlight critical differences between the ultrathin films and surfaces of bulk materials. Our results imply that monolayer-thin oxide films have rather unique properties.
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We present a synchrotron grazing incidence x-ray diffraction analysis of the domain structure and polar symmetry of highly strained BiFeO3 thin films grown on LaAlO3 substrate. We revealed the existence of periodic elastic nanodomains in the pure tetragonal-like BFO ultrathin films down to a thickness of 6 nm. A unique shear strain accommodation mechanism is disclosed. We further demonstrated that the periodicity of the nanodomains increases with film thickness but deviates from the classical Kittels square root law in ultrathin thickness regime (6 - 30 nm). Temperature-dependent experiments also reveal the disappearance of periodic modulation above 90C due to a MC-MA structural phase transition.
Quantum mechanical tunneling of electrons across ultrathin insulating oxide barriers has been studied extensively for decades due to its great potential in electronic device applications. In the few-nanometer-thick epitaxial oxide films, atomic-scale structural imperfections, such as the ubiquitously existed one-unit-cell-high terrace edges, can dramatically affect the tunneling probability and device performance. However, the underlying physics has not been investigated adequately. Here, taking ultrathin BaTiO3 films as a model system, we report an intrinsic tunneling conductance enhancement near the terrace edges. Scanning probe microscopy results demonstrate the existence of highly-conductive regions (tens of nanometers-wide) near the terrace edges. First-principles calculations suggest that the terrace edge geometry can trigger an electronic reconstruction, which reduces the effective tunneling barrier width locally. Furthermore, such tunneling conductance enhancement can be discovered in other transition-metal-oxides and controlled by surface termination engineering. The controllable electronic reconstruction could facilitate the implementation of oxide electronic devices and discovery of exotic low-dimensional quantum phases.
The phase immiscibility and the excellent matching between Ag(001) and Fe(001) unit cells (mismatch 0.8 %) make Fe/Ag growth attractive in the field of low dimensionality magnetic systems. Intermixing could be drastically limited at deposition temperatures as low as 140-150 K. The film structural evolution induced by post-growth annealing presents many interesting aspects involving activated atomic exchange processes and affecting magnetic properties. Previous experiments, of He and low energy ion scattering on films deposited at 150 K, indicated the formation of a segregated Ag layer upon annealing at 550 K. Higher temperatures led to the embedding of Fe into the Ag matrix. In those experiments, information on sub-surface layers was attained by techniques mainly sensitive to the topmost layer. Here, systematic PED measurements, providing chemical selectivity and structural information for a depth of several layers, have been accompanied with a few XRD rod scans, yielding a better sensitivity to the buried interface and to the film long range order. The results of this paper allow a comparison with recent models enlightening the dissolution paths of an ultra thin metal film into a different metal, when both subsurface migration of the deposit and phase separation between substrate and deposit are favoured. The occurrence of a surfactant-like stage, in which a single layer of Ag covers the Fe film is demonstrated for films of 4-6 ML heated at 500-550 K. Evidence of a stage characterized by the formation of two Ag capping layers is also reported. As the annealing temperature was increased beyond 700 K, the surface layers closely resembled the structure of bare Ag(001) with the residual presence of subsurface Fe aggregates.
The structural and magnetic properties of ultrathin FeO(111) films on Pt(111) with thicknesses from 1 to 16 monolayers (ML) were studied using the nuclear inelastic scattering (NIS) of synchrotron radiation. Distinct evolution of vibrational characteristics with thickness that is revealed in the phonon density of states (PDOS) witnesses a textbook transition from 2D to 3D lattice dynamics. For the thinnest films of 1 and 2 ML, the low energy part of the PDOS followed a linear dependence in energy that is characteristic for 2-dimensional systems. This dependence gradually transforms with thickness to the bulk ~E-square relation. Density functional theory phonon calculations perfectly reproduced the measured 1 ML PDOS within a simple model of a pseudomorphic FeO/Pt(111) interface. The calculations show that the 2D PDOS character is due to a weak coupling of the FeO film to the Pt(111) substrate. The evolution of the vibrational properties with an increasing thickness is closely related to a transient long range magnetic order and stabilization of an unusual structural phase.
Nitrogen-vacancy magnetic microscopy is employed in quenching mode as a non-invasive, high resolution tool to investigate the morphology of isolated skyrmions in ultrathin magnetic films. The skyrmion size and shape are found to be strongly affected by local pinning effects and magnetic field history. Micromagnetic simulations including static disorder, based on a physical model of grain-to-grain thickness variations, reproduce all experimental observations and reveal the key role of disorder and magnetic history in the stabilization of skyrmions in ultrathin magnetic films. This work opens the way to an in-depth understanding of skyrmion dynamics in real, disordered media.
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