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Hybrid molecular beam epitaxy (MBE) growth of Sn-modified BaTiO 3 films was realized with varying domain structures and crystal symmetries across the entire composition space. Macroscopic and microscopic structures and the crystal symmetry of these thin films were determined using a combination of optical second harmonic generation (SHG) polarimetry and scanning transmission electron microscopy (STEM). SHG polarimetry revealed a variation in the global crystal symmetry of the films from tetragonal ( P4 mm) to cubic [Formula: see text] across the composition range, x = 0 to 1 in BaTi 1− x Sn x O 3 (BTSO). STEM imaging shows that the long-range polar order observed when the Sn content is low ( x = 0.09) transformed to a short-range polar order as the Sn content increased ( x = 0.48). Consistent with atomic displacement measurements from STEM, the largest polarization was obtained at the lowest Sn content of x = 0.09 in Sn-modified BaTiO 3 as determined by SHG. These results agree with recent bulk ceramic reports and further identify this material system as a potential replacement for Pb-containing relaxor-based thin film devices.

Abstract Materials that blend physical properties that are usually mutually exclusive could facilitate devices with novel functionalities. For example, the doped perovskite alkaline earth stannates BaSnO 3 and SrSnO 3 show the intriguing combination of high light transparency and high electrical conductivity. Understanding such emergent physics requires deep insight into the materials’ electronic structures. Moreover, the band structure at the surfaces of those materials can deviate significantly from their bulk counterparts, thereby unlocking novel physical phenomena. Employing angle-resolved photoemission spectroscopy and ab initio calculations, we reveal the existence of a 2-dimensional metallic state at the SnO 2 -terminated surface of 1% La-doped BaSnO 3 thin films. The observed surface state is characterized by a distinct carrier density and a lower effective mass compared to the bulk conduction band, of about 0.12 m e . These particular surface state properties place BaSnO 3 among the materials suitable for engineering highly conductive transition metal oxide heterostructures.

Abstract Germanium-based oxides such as rutile GeO 2 are garnering attention owing to their wide band gaps and the prospects of ambipolar doping for application in high-power devices. Here, we present the use of germanium tetraisopropoxide (GTIP), a metal-organic chemical precursor, as a source of germanium for the demonstration of hybrid molecular beam epitaxy for germanium-containing compounds. We use Sn 1- x Ge x O 2 and SrSn 1- x Ge x O 3 as model systems to demonstrate our synthesis method. A combination of high-resolution X-ray diffraction, scanning transmission electron microscopy, and X-ray photoelectron spectroscopy confirms the successful growth of epitaxial rutile Sn 1- x Ge x O 2 on TiO 2 (001) substrates up to x  = 0.54 and coherent perovskite SrSn 1- x Ge x O 3 on GdScO 3 (110) substrates up to x  = 0.16. Characterization and first-principles calculations corroborate that germanium occupies the tin site, as opposed to the strontium site. These findings confirm the viability of the GTIP precursor for the growth of germanium-containing oxides by hybrid molecular beam epitaxy, thus providing a promising route to high-quality perovskite germanate films.

Perovskite SrIrO 3 films and its heterostructures are very promising, yet less researched, avenues to explore interesting physics originating from the interplay between strong spin–orbit coupling and electron correlations. Elemental iridium is a commonly used source for molecular beam epitaxy (MBE) synthesis of SrIrO 3 films. However, elemental iridium is extremely difficult to oxidize and evaporate while maintaining an ultra-high vacuum and a long mean free path. Here, we calculated a thermodynamic phase diagram to highlight these synthesis challenges for phase-pure SrIrO 3 and other iridium-based oxides. We addressed these challenges using a novel solid-source metal-organic MBE approach that rests on the idea of modifying the metal-source chemistry. Phase-pure, single-crystalline, coherent, epitaxial (001) pc SrIrO 3 films on (001) SrTiO 3 substrate were grown. Films demonstrated semi-metallic behavior, Kondo scattering, and weak antilocalization. Our synthesis approach has the potential to facilitate research involving iridate heterostructures by enabling their atomically precise syntheses.

This work reports the quantification of rise in channel temperature due to self-heating in two-terminal SrSnO 3 thin film devices under electrical bias. Using pulsed current–voltage (I–V) measurements, thermal resistances of the thin films were determined by extracting the relationship between the channel temperature and the dissipated power. For a 26-nm-thick n-doped SrSnO 3 channel with an area of 200 μm 2 , a thermal resistance of 260.1 ± 24.5 K mm/W was obtained. For a modest dissipated power of 0.5 W/mm, the channel temperature rose to ∼176 °C, a value which increases further at higher power levels. Electro-thermal simulations were performed which showed close agreement between the simulated and experimental I–V characteristics both in the absence and presence of self-heating. The work presented is critical for the development of perovskite-based high-power electronic devices.

Hybrid MBE produces epitaxial SrTiO 3 free-standing nanomembranes using remote epitaxy in an adsorption-controlled manner.

SrTiO 3 (STO) is an incipient ferroelectric perovskite oxide for which the onset of ferroelectric order is suppressed by quantum fluctuations. This property results in a very large increase in static dielectric constant from ∼300 at room temperature to ∼20,000 at liquid He temperature in bulk single crystals. However, the low-temperature dielectric constant of epitaxial STO films is typically a few hundred to a few thousand. Here, we use all-epitaxial capacitors of the form n -STO/undoped STO/ n -STO (001) prepared by hybrid molecular beam epitaxy, to demonstrate intrinsic dielectric constants of an unstrained STO (001) film exceeding 25,000. We show that the n -STO/undoped STO interface plays a critically important role not previously considered in determining the dielectric properties that must be properly accounted for to determine the intrinsic dielectric constant.

We investigate the surface electronic structure of SrTiO 3 (STO) films grown by a hybrid molecular beam epitaxy that are both stoichiometric and nonstoichiometric by means of x-ray photoelectron spectroscopy and electron energy loss spectroscopy. Increasing the fraction of the surface that is terminated with an SrO layer is correlated with a decrease in the chemical potential whereby the valence band maximum moves closer to the Fermi level, but without a significant change in the bandgap. Inasmuch as SrO-terminated STO (001) has previously been shown to act as an electron scavenger in which carriers from the bulk are trapped, we argue that the high fraction of SrO in the terminal layer is what lowers the chemical potential in Sr-rich STO. Our experimental results provide important insights into various physical phenomena that can occur on STO (001) surfaces and their effect on bulk electronic properties.