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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.

 

A multistep phase sequence following the crystallization of amorphous Al2O3 via solid-phase epitaxy (SPE) points to methods to create low-defect-density thin films of the metastable cubic γ-Al2O3 polymorph. An amorphous Al2O3 thin film on a (0001) α-Al2O3 sapphire substrate initially transforms upon heating to form epitaxial γ-Al2O3, followed by a transformation to monoclinic θ-Al2O3, and eventually to α-Al2O3. Epitaxial γ-Al2O3 layers with low mosaic widths in X-ray rocking curves can be formed via SPE by crystallizing the γ-Al2O3 phase from amorphous Al2O3 and avoiding the microstructural inhomogeneity arising from the spatially inhomogeneous transformation to θ-Al2O3. A complementary molecular dynamics (MD) simulation indicates that the amorphous layer and γ-Al2O3 have similar Al coordination geometry, suggesting that γ-Al2O3 forms in part because it involves the minimum rearrangement of the initially amorphous configuration. The lattice parameters of γ-Al2O3 are consistent with a structure in which the majority of the Al vacancies in the spinel structure occupy sites with tetrahedral coordination, consistent with the MD results. The formation of Al vacancies at tetrahedral spinel sites in epitaxial γ-Al2O3 can minimize the epitaxial elastic deformation of γ-Al2O3 during crystallization. 

Chemical vapor deposition of CH 4 on Ge(001) can enable anisotropic growth of narrow, semiconducting graphene nanoribbons with predominately smooth armchair edges and high-performance charge transport properties. However, such nanoribbons are not aligned in one direction but instead grow perpendicularly, which is not optimal for integration into high-performance electronics. Here, it is demonstrated that vicinal Ge(001) substrates can be used to synthesize armchair nanoribbons, of which ∼90% are aligned within ±1.5° perpendicular to the miscut. When the growth rate is slow, graphene crystals evolve as nanoribbons. However, as the growth rate increases, the uphill and downhill crystal edges evolve asymmetrically. This asymmetry is consistent with stronger binding between the downhill edge and the Ge surface, for example due to different edge termination as shown by density functional theory calculations. By tailoring growth rate and time, nanoribbons with sub-10 nm widths that exhibit excellent charge transport characteristics, including simultaneous high on-state conductance of 8.0 μS and a high on/off conductance ratio of 570 in field-effect transistors, are achieved. Large-area alignment of semiconducting ribbons with promising charge transport properties is an important step towards understanding the anisotropic nanoribbon growth and integrating these materials into scalable, future semiconductor technologies. 

Reconfiguration of amorphous complex oxides provides a readily controllable source of stress that can be leveraged in nanoscale assembly to access a broad range of 3D geometries and hybrid materials. An amorphous SrTiO₃layer on a Si:B/Si_1−xGe_x:B heterostructure is reconfigured at the atomic scale upon heating, exhibiting a change in volume of ≈2% and accompanying biaxial stress. The Si:B/Si_1−xGe_x:B bilayer is fabricated by molecular beam epitaxy, followed by sputter deposition of SrTiO₃at room temperature. The processes yield a hybrid oxide/semiconductor nanomembrane. Upon release from the substrate, the nanomembrane rolls up and has a curvature determined by the stress in the epitaxially grown Si:B/Si_1−xGe_x:B heterostructure. Heating to 600 °C leads to a decrease of the radius of curvature consistent with the development of a large compressive biaxial stress during the reconfiguration of SrTiO₃. The control of stresses via post‐deposition processing provides a new route to the assembly of complex‐oxide‐based heterostructures in 3D geometry. The reconfiguration of metastable mechanical stressors enables i) synthesis of various types of strained superlattice structures that cannot be fabricated by direct growth and ii) technologies based on strain engineering of complex oxides via highly scalable lithographic processes and on large‐area semiconductor substrates.