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  1. Amorphous BaTiO3 layers deposited on SrTiO3 (001) substrates at room temperature were subsequently crystallized using solid phase epitaxy (SPE). Heating an initially amorphous BaTiO3 layer in air at 650 °C for 3 h resulted in crystallization with components in two distinct crystallographic orientation relationships with respect to the substrate. Part of the volume of the BaTiO3 layer crystallized in a cube-on-cube relationship with the substrate. Other volumes crystallized in four variants of a 70.5° rotation about ⟨110⟩, resulting in a ⟨221⟩ surface normal in each case. Each of these four variants forms a Σ = 3 coincident site lattice with respect to the SrTiO3 substrate and the cube-on-cube oriented BaTiO3. Heating for the same duration and temperature in a reducing gas atmosphere resulted in the formation of polycrystalline BaTiO3 with no preferred crystallographic orientation. The dependence on the gas atmosphere indicates that it may be possible to tune the annealing time, temperature, and atmosphere to produce a single crystalline BTO on STO by SPE or produce a desired distribution of orientations.

     
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    Free, publicly-accessible full text available August 1, 2024
  2. Abstract

    The drive toward non‐von Neumann device architectures has led to an intense focus on insulator‐to‐metal (IMT) and the converse metal‐to‐insulator (MIT) transitions. Studies of electric field‐driven IMT in the prototypical VO2thin‐film channel devices are largely focused on the electrical and elastic responses of the films, but the response of the corresponding TiO2substrate is often overlooked, since it is nominally expected to be electrically passive and elastically rigid. Here, in‐operando spatiotemporal imaging of the coupled elastodynamics using X‐ray diffraction microscopy of a VO2film channel device on TiO2substrate reveals two new surprises. First, the film channel bulges during the IMT, the opposite of the expected shrinking in the film undergoing IMT. Second, a microns thick proximal layer in the substrate also coherently bulges accompanying the IMT in the film, which is completely unexpected. Phase‐field simulations of coupled IMT, oxygen vacancy electronic dynamics, and electronic carrier diffusion incorporating thermal and strain effects suggest that the observed elastodynamics can be explained by the known naturally occurring oxygen vacancies that rapidly ionize (and deionize) in concert with the IMT (MIT). Fast electrical‐triggering of the IMT via ionizing defects and an active “IMT‐like” substrate layer are critical aspects to consider in device applications.

     
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  3. null (Ed.)
    Hard X-ray nanodiffraction provides a unique nondestructive technique to quantify local strain and structural inhomogeneities at nanometer length scales. However, sample mosaicity and phase separation can result in a complex diffraction pattern that can make it challenging to quantify nanoscale structural distortions. In this work, a k -means clustering algorithm was utilized to identify local maxima of intensity by partitioning diffraction data in a three-dimensional feature space of detector coordinates and intensity. This technique has been applied to X-ray nanodiffraction measurements of a patterned ferroelectric PbZr 0.2 Ti 0.8 O 3 sample. The analysis reveals the presence of two phases in the sample with different lattice parameters. A highly heterogeneous distribution of lattice parameters with a variation of 0.02 Å was also observed within one ferroelectric domain. This approach provides a nanoscale survey of subtle structural distortions as well as phase separation in ferroelectric domains in a patterned sample. 
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