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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Mechanisms of Three-Dimensional Solid-Phase Epitaxial Crystallization of Strontium Titanate

Strontium titanate (SrTiO 3 , STO) is a complex metal oxide with a cubic perovskite crystal structure. Due to its easily described and understood crystal structure in the cubic phase, STO is an ideal model system for exploring the mechanistic details of solid-phase epitaxy (SPE) in complex oxides. SPE is a crystallization approach that aims to guide crystal growth at low homologous temperatures to achieve targeted microstructures. Beyond planar thin films, SPE can also exploit the addition of a chemically inert, noncrystallizing, amorphous obstacle in the path of crystallization to generate complex three-dimensional structures. The introduction of this mask fundamentally alters the SPE process, inducing a transition from two- to three-dimensional geometries and from vertical to lateral crystal growth under the influence of the crystal/mask/amorphous boundary. Using a combination of molecular dynamics simulations and experiments, we identify several unique phenomena in the nanoscale growth behaviors in both conventional (unmasked) and masked SPE. Examining conventional SPE of STO, we find that crystallization at the interface is strongly correlated to, and potentially driven by, density fluctuations in the region of the amorphous STO near the crystalline/amorphous interface with a strong facet dependence. In the masked case, we find that the crystalline growth front becomes nonplanar near contact with the mask. We also observe a minimum vertical growth requirement prior to lateral crystallization. Both phenomena depend on the relative bulk and interfacial free energies of the three-phase (crystal/mask/amorphous) system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

All Roads Lead to TiO 2 : TiO 2 -Rich Surfaces of Barium and Strontium Titanate Prepared by Hydrothermal Synthesis

Through high-resolution electron microscopy, the surface structure of barium titanate and strontium titanate nanoparticles are found to be terminated by a TiO 2 double layer. These results confirm prior observations of TiO 2 -rich surface reconstructions on strontium titanate nanoparticles made hydrothermally at high pH and single crystals prepared with wet chemical etching. Of all the reconstructions observed on single crystals for these two materials, we report for first time the √13 × √13R33.7° structure on the {001} facets of hydrothermally prepared barium titanate and strontium titanate nanocrystals. The aqueous environment common to the two preparation methods preferentially leaves strontium and barium depleted from the A-sites near the surface and leads to TiO 2 -terminated surfaces for both materials. Analysis indicates that the observed structures are the thermodynamic lowest energy structures in aqueous conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2015

P-type conductivity in annealed strontium titanate

Hall-effect measurements indicate p-type conductivity in bulk, single-crystal strontium titanate (SrTiO{sub 3}, or STO) samples that were annealed at 1200°C. Room-temperature mobilities above 100 cm{sup 2}/V s were measured, an order of magnitude higher than those for electrons (5-10 cm{sup 2}/V s). Average hole densities were in the 10{sup 9}-10{sup 10} cm{sup −3} range, consistent with a deep acceptor.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Probing the thermal Hall effect using miniature capacitive strontium titanate thermometry

The thermal Hall effect is the thermal analog of the electrical Hall effect. Rarely observed in normal metals, thermal Hall signals have been argued to be a key property for a number of strongly correlated materials, such as high temperature superconductors, correlated topological insulators, and quantum magnets. The observation of the thermal Hall effect requires precise measurement of temperature in intense magnetic fields. Particularly at low temperature, resistive thermometers have a strong dependence on field, which makes them unsuitable for this purpose. We have created capacitive thermometers which instead measure the dielectric constant of strontium titanate (SrTiO 3 ). SrTiO 3 approaches a ferroelectric transition, causing its dielectric constant to increase by a few orders of magnitude at low temperature. As a result, these thermometers are very sensitive at low temperature while having very little dependence on the applied magnetic field, making them ideal for thermal Hall measurements. Here, we demonstrate this method by making measurements of the thermal Hall effect in Bismuth in magnetic fields of up to 10 T.

47 OTHER INSTRUMENTATION↗
DOE OSTI2016

Superconductivity at very low density: The case of strontium titanate

Doped strontium titanate becomes superconducting at a density as low as n = 5 × 10 17 cm -3 , where the Fermi energy is orders of magnitude smaller than the longitudinal-optical-phonon frequencies. In this limit, the only optical mode with a frequency which is smaller than the Fermi energy is the plasmon. In contrast to metals, the interaction strength is weak due to screening by the crystal, which allows the construction of a controllable theory of plasmon superconductivity. We show that plasma mediated pairing alone can account for the observed transition temperatures only if the dielectric screening by the crystal is reduced in the slightly doped samples compared with the insulating ones. We also discuss unique features of the plasmon mechanism, which appear in the tunneling density of states above the gap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Phonon thermal transport through tilt grain boundaries in strontium titanate

In this work, we perform nonequilibrium molecular dynamics simulations to study phonon scattering at two tilt grain boundaries (GBs) in SrTiO{sub 3}. Mode-wise energy transmission coefficients are obtained based on phonon wave-packet dynamics simulations. The Kapitza conductance is then quantified using a lattice dynamics approach. The obtained results of the Kapitza conductance of both GBs compare well with those obtained by the direct method, except for the temperature dependence. Contrary to common belief, the results of this work show that the optical modes in SrTiO{sub 3} contribute significantly to phonon thermal transport, accounting for over 50% of the Kapitza conductance. To understand the effect of the GB structural disorder on phonon transport, we compare the local phonon density of states of the atoms in the GB region with that in the single crystalline grain region. Our results show that the excess vibrational modes introduced by the structural disorder do not have a significant effect on phonon scattering at the GBs, but the absence of certain modes in the GB region appears to be responsible for phonon reflections at GBs. This work has also demonstrated phonon mode conversion and simultaneous generation of new modes. Some of the new modes have the same frequency as the initial wave packet, while some have the same wave vector but lower frequencies.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A clean ballistic quantum point contact in strontium titanate

The perovskite oxide strontium titanate (SrTiO 3 ) combines electrostatic tunability, superconductivity and spin–orbit coupling, and is of potential use in the development of quantum devices. However, exploring quantum effects in SrTiO 3 nanostructures is challenging because of the presence of disorder. Here, in this work, we report high-mobility, gate-tunable devices in SrTiO 3 that have ballistic constrictions and clean normal-state conductance quantization. Our devices are based on SrTiO 3 two-dimensional electron gas channels that have a thin hafnium oxide barrier layer between the channel and an ionic liquid gate. Conductance plateaus show twofold degeneracy that persists for magnetic fields of at least 5 T. This is above what is expected from the g factors extracted at high fields and could be a signature of electron pairing extending outside the superconducting regime.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Correlation between Cr 3+ Luminescence and Oxygen Vacancy Disorder in Strontium Titanate under MeV Ion Irradiation

Strontium titanate (SrTiO 3 ), a model system with a strongly correlated electronic structure, has attracted much attention recently because of its outstanding physicochemical properties and considerable potentials for technological applications. The capability to control oxygen vacancy profiles and their effect on valence states of cations will increase significantly the functionality of devices based on transition metal oxides. This work presents new insights into the near-infrared luminescence emission of Cr 3+ centers in stoichiometric SrTiO 3 induced using 3 MeV protons at temperatures of 100 K, 170 K, and room temperature. The study covers a wide spectral range, including near-infrared, visible, and near-UV regions. Our main purpose is to investigate the role of the oxygen vacancies introduced by energetic charged particles on the shape and yield of induced luminescence spectra, in particular to explore the interplay between the Cr 3+ luminescence at 1.55 eV and oxygen disorder. A clear correlation is found between the decay of the Cr luminescence yield during irradiation and the growth of a band at 2.0 eV, well-resolved below 170 K, which has been very recently attributed to d–d transitions of electrons self-trapped as Ti 3+ in the close vicinity of oxygen vacancies. This correlation suggests irradiation-induced oxidation of the Cr 3+ (Cr 3+ → Cr n+ , n > 3) via trapping of irradiation-induced holes, while the partner electrons are self-trapped as Ti 3+ . Here, these new results provide effective guidelines for further understanding the electronic and photocatalytic behavior of STO:Cr 3+ .

36 MATERIALS SCIENCE↗
DOE OSTI2014

On the sol-gel synthesis of strontium-titanate thin films and the prospects of their use in electronics

Strontium-titanate films obtained by the sol-gel technique are deposited onto silicon and silicon/oxide titanium/platinum substrates. The strontium-titanate phase is detected by the method of X-ray diffraction analysis after heat treatment at temperatures of 750 and 800°C. The thickness of the films obtained by the spin-on method increases from 50 to 250 nm as the number of deposited layers is increased and is accompanied with an increase in the grain size in the films. Prospects of the development of the sol-gel technique for the formation of film components of electronic devices based on SrTiO{sub 3} xerogels are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Enhanced flexoelectricity through residual ferroelectricity in barium strontium titanate

Residual ferroelectricity is observed in barium strontium titanate ceramics over 30 °C above the global phase transition temperature, in the same temperature range in which anomalously large flexoelectric coefficients are reported. The application of a strain gradient leads to strain gradient-induced poling or flexoelectric poling. This was observed by the development of a remanent polarization in flexoelectric measurements, an induced d{sub 33} piezoelectric response even after the strain gradient was removed, and the production of an internal bias of 9 kV m{sup −1}. It is concluded that residual ferroelectric response considerably enhances the observed flexoelectric response.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Low-temperature state in strontium titanate microcrystals using in situ multireflection Bragg coherent x-ray diffraction imaging

Strontium titanate is a classic quantum paraelectric oxide material that has been widely studied in bulk and thin films. It exhibits a well-known cubic-to-tetragonal antiferrodistortive phase transition at 105 K, characterized by the rotation of oxygen octahedra. A possible second phase transition at lower temperature is suppressed by quantum fluctuations, preventing the onset of ferroelectric order. However, recent studies have shown that ferroelectric order can be established at low temperatures by inducing strain and other means. Here, we used in situ multireflection Bragg coherent x-ray diffraction imaging to measure the strain and rotation tensors for two strontium titanate microcrystals at low temperature. We observe strains induced by dislocations and inclusion-like impurities in the microcrystals. Based on radial magnitude plots, these strains increase in magnitude and spread as the temperature decreases. Pearson's correlation heat maps show a structural transition at 50 K, which could possibly be the formation of a low-temperature ferroelectric phase in the presence of strain. We do not observe any change in local strains associated with the tetragonal phase transition at 105 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Blocking effect of crystal–glass interface in lanthanum doped barium strontium titanate glass–ceramics

Graphical abstract: The blocking effect of the crystal–glass interface on the carrier transport behavior in the lanthanum doped barium strontium titanate glass–ceramics: preparation and characterization. - Highlights: • La{sub 2}O{sub 3} addition promotes the crystallization of the major crystalline phase. • The Z″ and M″ peaks exist a significant mismatch for 0.5 mol% La{sub 2}O{sub 3} addition. • The Z″ and M″ peaks separate obviously for 1.0 mol% La{sub 2}O{sub 3} addition. • Crystallite impedance decreases while crystal–glass interface impedance increases. • La{sub 2}O{sub 3} addition increases blocking factor of the crystal–glass interface. - Abstract: The microstructures and dielectric properties in La{sub 2}O{sub 3}-doped barium strontium titanate glass–ceramics have been investigated by scanning electron microscopy (SEM) and impedance spectroscopy. SEM analysis indicated that La{sub 2}O{sub 3} additive decreases the average crystallite size. Impedance spectroscopy revealed that the positions of Z″ and M″ peaks are close for undoped samples. When La{sub 2}O{sub 3} concentration is 0.5 mol%, the Z″ and M″ peaks show a significant mismatch. Furthermore, these peaks separate obviously for 1.0 mol% La{sub 2}O{sub 3} addition. With increasing La{sub 2}O{sub 3} concentration, the contribution of the crystallite impedance becomes smaller, while the contribution of the crystal–glass interface impedance becomes larger. More interestingly, it was found that La{sub 2}O{sub 3} additive increases blocking factor of the crystal–glass interface in the temperature range of 250–450 °C. This may be attributed to a decrease of activation energy of the crystallite and an increase of the crystal–glass interface area.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Tuned sensitivity towards H{sub 2}S and NH{sub 3} with Cu doped barium strontium titanate materials

The different amount of Cu-doped Barium Strontium Titanate (BST) thick film materials have been tested for their gas-sensing performances towards NH{sub 3} and H{sub 2}S under dry and 50% relative humidity (RH) background conditions. The optimum NH{sub 3} sensitivity was attained with 0.1mol% Cu-doped BST whereas the selective detection of H{sub 2}S was highlighted using 5mol% Cu-doped BST material. No cross-sensitivity effects to CO, NO{sub 2}, CH{sub 4} and SO{sub 2} were observed for all tested materials operated at their optimum temperature (200°C) under humid conditions (50% RH). The presence of humidity clearly enhances the gas sensitivity to NH{sub 3} and H{sub 2}S detection.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Effect of thermochemical treatments on laser-induced luminescence spectra from strontium titanate: comparison with swift ion-beam irradiation experiments

Results recently reported on the effect of thermochemical treatments on the (He-Cd) laser-excited emission spectra of strontium titanate (STO) are re-analyzed here and compared with results obtained under ion-beam irradiation. Contributing bands centered at 2.4 eV and 2.8 eV, which appear under laser excitation, present intensities dependent upon previous thermal treatments in oxidizing (O 2 ) or reducing atmosphere (H 2 ). As a key result, the emission band centered at 2.8 eV is clearly enhanced in samples exposed to a reducing atmosphere. From a comparison with the ionoluminescence data, it is concluded that the laser-excited experiments can be rationalized within a framework developed from ion-beam excitation studies. In particular, the band at 2.8 eV, sometimes attributed to oxygen vacancies, behaves as expected for optical transitions from conduction-band (CB) states to the ground state level of the self-trapped exciton center. The band at 2.0 eV reported in ion-beam irradiated STO, and attributed to oxygen vacancies, is not observed in laser-excited crystals. As a consequence of our analysis, a consistent scheme of electronic energy levels and optical transitions can now be reliably offered for strontium titanate.

74 ATOMIC AND MOLECULAR PHYSICS↗