Miri Choi

Strain relaxation in single crystal SrTiO3 grown on Si (001) by molecular beam epitaxy

An epitaxial layer of SrTiO3 grown directly on Si may be used as a pseudo-substrate for the integration of perovskite oxides onto silicon. When SrTiO3 is initially grown on Si (001), it is nominally compressively strained. However, by subsequent annealing in oxygen at elevated temperature, an SiOx interlayer can be formed which alters the strain state of SrTiO3. We report a study of strain relaxation in SrTiO3 films grown on Si by molecular beam epitaxy as a function of annealing time and oxygen partial pressure. Using a combination of x-ray diffraction, reflection high energy electron diffraction, and transmission electron microscopy, we describe the process of interfacial oxidation and strain relaxation of SrTiO3 on Si (001). Understanding the process of strain relaxation of SrTiO3 on silicon will be useful for controlling the SrTiO3 lattice constant for lattice matching with functional oxide overlayers.

Structural, optical, and electrical properties of strained La-doped SrTiO3 films

The structural, optical, and room-temperature electrical properties of strained La-doped SrTiO3 epitaxial thin films are investigated. Conductive La-doped SrTiO3 thin films with concentration varying from 5 to 25% are grown by molecular beam epitaxy on four different substrates: LaAlO3, (LaAlO3)0.3(Sr2AlTaO6)0.7, SrTiO3, and DyScO3, which result in lattice mismatch strain ranging from −2.9% to +1.1%. We compare the effect of La concentration and strain on the structural and optical properties, and measure their effect on the electrical resistivity and mobility at room temperature. Room temperature resistivities ranging from ∼10−2 to 10−5 Ω cm are obtained depending on strain and La concentration. The room temperature mobility decreases with increasing strain regardless of the sign of the strain. The observed Drude peak and Burstein-Moss shift from spectroscopic ellipsometry clearly confirm that the La addition creates a high density of free carriers in SrTiO3. First principles calculations were performed to help understand the effect of La-doping on the density of states effective mass as well as the conductivity and DC relaxation time.

Surface electronic structure for various surface preparations of Nb-doped SrTiO3 (001)

High-resolution angle-resolved photoemission spectroscopy (ARPES) was used to study the surface electronic structure of Nb-doped SrTiO3 (STO) single crystals prepared using a variety of surface preparations. ARPES measurements show that simple degreasing with subsequent anneal in vacuum is not an adequate surface preparation of STO, rather, preparations consisting of etching with buffered HF or HCl, and to a lesser extent, simple water leaching resulted in surfaces with much less disorder. A non-dispersing, mid-gap state was found ∼800 meV above the top of the valence band for samples which underwent etching. This mid-gap state is not present for vacuum-annealed and water-leached samples, as well as for STO thin films grown using molecular beam epitaxy. Theoretical modeling using density functional theory suggests that this mid-gap state is not related to the SrO- and TiO2-terminated surfaces, but rather, is due to a partial hydrogenation of the STO surface that occurs during etching.

Charge transfer in Sr Zintl template on Si(001)

The formation of the half monolayer (ML) Sr Zintl template layer on Si(001) is investigated in a combined experimental and theoretical work consisting of in situ reflection high energy electron diffraction, in situ x-ray photoelectron spectroscopy (XPS), and density functional theory. Starting with clean 2 × 1 reconstructed Si(001), we demonstrate that Sr deposition leads to a charge transfer from the metal to the Si substrate resulting in the disappearance of the asymmetry of Si dimers—an essential structural change that enables direct perovskite epitaxy on Si, and likely, other semiconductors. XPS reveals an unexpected shift to higher binding energy of the Si 2p core-level components, including the bulk. This unusual behavior is attributed to final state effects using first principles calculations. As measured by ultraviolet photoelectron spectroscopy, the deposition of 0.5 ML of Sr lowers the work function of the system by 1.35 eV, and is in good agreement with our theoretical calculations.

Comparison of acid- and non-acid-based surface preparations of Nb-doped SrTiO3 (001)

High-resolution angle-resolved photoemission spectroscopy (ARPES) and x-ray photoelectron spectroscopy (XPS) were used to study the relative effectiveness of acid- and non-acid-based surface preparations of Nb-doped SrTiO3 (STO) single crystals. ARPES measurements show that boiling STO in deionized water produces surfaces of similar quality to those etched with buffered HF (Kawasaki method), or HCl/HNO3 (Arkansas method). XPS measurements indicate this water-based surface preparation is more effective than acid-based methods at removing SrOx crystallites and leaving the surface TiO2-terminated.

Tunable electrical properties of TaNx thin films grown by ionized physical vapor deposition

Tantalum nitride (TaNx) amorphous thin films with varying nitrogen content were grown on SiO2/Si using ionized physical vapor deposition. The composition of the films was examined by Rutherford back scattering spectrometry. The carrier density and the resistivity of TaNx films were measured by Hall effect and Van Der Pauws method. TaNx thin films showed increased electrical resistivity and reduced carrier density as the amount of nitrogen was increased. By controlling the nitrogen content, the carrier density can be tuned within a large range of 1019–1022 cm−3 for 3 and 15 nm thick TaNx films. The metallicity of the films was confirmed using ultraviolet photoemission spectroscopy. For 3 nm thick TaNx films, carrier densities of ∼1021 cm−3 were obtained with the N2 flow rate in the range of 10–15 sccm. Such films have potential application in a quantum metal field effect transistor.

Optical properties of transition metal oxide quantum wells

Fabrication of a quantum well, a structure that confines the electron motion along one or more spatial directions, is a powerful method of controlling the electronic structure and corresponding optical response of a material. For example, semiconductor quantum wells are used to enhance optical properties of laser diodes. The ability to control the growth of transition metal oxide films to atomic precision opens an exciting opportunity of engineering quantum wells in these materials. The wide range of transition metal oxide band gaps offers unprecedented control of confinement while the strong correlation of d-electrons allows for various cooperative phenomena to come into play. Here, we combine density functional theory and tight-binding model Hamiltonian analysis to provide a simple physical picture of transition metal oxide quantum well states using a SrO/SrTiO3/SrO heterostructure as an example. The optical properties of the well are investigated by computing the frequency-dependent dielectric functions. The effect of an external electric field, which is essential for electro-optical devices, is also considered.

Quantum confinement in transition metal oxide quantum wells

We report on the quantum confinement in SrTiO3 (STO) quantum wells (QWs) grown by molecular beam epitaxy. The QW structure consists of LaAlO3 (LAO) and STO layers grown on LAO substrate. Structures with different QW thicknesses ranging from two to ten unit cells were grown and characterized. Optical properties (complex dielectric function) were measured by spectroscopic ellipsometry in the range of 1.0 eV–6.0 eV at room temperature. We observed that the absorption edge was blue-shifted by approximately 0.39 eV as the STO quantum well thickness was reduced to two unit cells. This demonstrates that the energy level of the first sub-band can be controlled by the QW thickness in a complex oxide material.

Combined in-situ photoemission spectroscopy and density functional theory of the Sr Zintl template for oxide heteroepitaxy on Si(001)

Half-monolayer Sr on Si(001) is a Zintl template necessary for epitaxial growth of SrTiO3 on Si(001). The authors investigate the reconstruction in the atomic and electronic structure of Si(001) induced by sub-monolayer Sr deposition using in-situ x-ray/ultraviolet photoemission spectroscopy and density functional theory. Sub-monolayer Sr is deposited on Si(001) using molecular beam epitaxy and the structural evolution of the surface is monitored using reflection high-energy electron diffraction. Experimentally, the authors find that the ionization energy of Si(001) decreases as a function of Sr coverage from 4.82 eV for pure Si(001) to 3.97 eV for half-monolayer Sr on Si(001) due to charge transfer from Sr to Si. They calculate the ionization energy for sub-monolayer Sr on Si(001) by considering several atomistic models and find good agreement with experiment. The authors clearly establish the Zintl character of the template by measuring the surface core level shifts of Si(001) and half-monolayer Sr/Si(0...

Formation of single-orientation epitaxial islands of TiSi2 on Si(001) using Sr passivation

Epitaxial islands of C49-phase TiSi2 of up to 100 nm in size, and with a single crystallographic orientation, have been fabricated on Si(001) substrates. The growth process involves passivation of the Si surface using Sr, followed by deposition of Ti in the form of SrTiO3, which prevents the reaction between Ti and Si. Decomposition of SrTiO3 at temperatures above 800 °C drives off Sr and O completely, leaving epitaxial islands of TiSi2 dispersed on the Si surface. The TiSi2 islands have (010) orientation and an in-plane epitaxial relationship of Si[110]∥TiSi2[100]. Density functional calculations of the surface and interface energies show that the island sizes and contact angles are consistent with surface energy minimization.