Bharat Jalan

Epitaxial SrTiO3 films with electron mobilities exceeding 30,000 cm2 V(-1) s(-1).

The study of quantum phenomena in semiconductors requires epitaxial structures with exceptionally high charge-carrier mobilities. Furthermore, low-temperature mobilities are highly sensitive probes of the quality of epitaxial layers, because they are limited by impurity and defect scattering. Unlike many other complex oxides, electron-doped SrTiO(3) single crystals show high (approximately 10(4) cm(2) V(-1) s(-1)) electron mobilities at low temperatures. High-mobility, epitaxial heterostructures with SrTiO(3) have recently attracted attention for thermoelectric applications, field-induced superconductivity and two-dimensional (2D) interface conductivity. Epitaxial SrTiO(3) thin films are often deposited by energetic techniques, such as pulsed laser deposition. Electron mobilities in such films are lower than those of single crystals. In semiconductor physics, molecular beam epitaxy (MBE) is widely established as the deposition method that produces the highest mobility structures. It is a low-energetic, high-purity technique that allows for low defect densities and precise control over doping concentrations and location. Here, we demonstrate controlled doping of epitaxial SrTiO(3) layers grown by MBE. Electron mobilities in these films exceed those of single crystals. At low temperatures, the films show Shubnikov-de Haas oscillations. These high-mobility SrTiO(3) films allow for the study of the intrinsic physics of SrTiO(3) and can serve as building blocks for high-mobility oxide heterostructures.

Growth of high-quality SrTiO3 films using a hybrid molecular beam epitaxy approach

A hybrid molecular beam epitaxy approach for atomic-layer controlled growth of high-quality SrTiO3 films with scalable growth rates was developed. The approach uses an effusion cell for Sr, a plasma source for oxygen, and a metal-organic source (titanium tetra isopropoxide) for Ti. SrTiO3 films were investigated as a function of cation flux ratio on (001) SrTiO3 and (LaAlO3)0.3(Sr2AlTaO6)0.7 (LSAT) substrates. Growth conditions for stoichiometric insulating films were identified. Persistent (>180 oscillations) reflection high-energy electron diffraction oscillation characteristic of layer-by-layer growth were observed. The full widths at half maximum of x-ray diffraction rocking curves were similar to those of the substrates, i.e., 34 arc sec on LSAT. The film surfaces were nearly ideal with root mean square surface roughness values of less than 0.1 nm. The relationship between surface reconstructions, growth modes, and stoichiometry is discussed.

Molecular beam epitaxy of SrTiO3 with a growth window

Many complex oxides with only nonvolatile constituents do not have a wide growth window in conventional molecular beam epitaxy (MBE) approaches, which makes it difficult to obtain stoichiometric films. Here it is shown that a growth window in which the stoichiometry is self-regulating can be achieved for SrTiO3 films by using a hybrid MBE approach that uses a volatile metal-organic source for Ti, titanium tetra isopropoxide (TTIP). The growth window widens and shifts to higher TTIP/Sr flux ratios with increasing temperature, showing that it is related to the desorption of the volatile TTIP. We demonstrate stoichiometric, highly perfect, insulating SrTiO3 films. The approach can be adapted for the growth of other complex oxides that previously were believed to have no wide MBE growth window.

Large Seebeck coefficients and thermoelectric power factor of La-doped SrTiO3 thin films

Seebeck coefficients and conductivity of La-doped SrTiO3 thin films grown by molecular beam epitaxy were measured as a function of carrier concentration. At low carrier concentrations, thin films show very high Seebeck coefficients (up to 980 μV K−1). The maximum thermoelectric power factor was 39 μWcm−1 K−2 at a carrier concentration of 7×1020 cm−3. La-delta-doped superlattices were also characterized and exhibited Seebeck coefficients of ∼500 μV K−1. The results are discussed in the context of reports of enhanced Seebeck coefficients in delta-doped SrTiO3 superlattices.

Thermal conductivity as a metric for the crystalline quality of SrTiO3 epitaxial layers

Measurements of thermal conductivity Λ by time-domain thermoreflectance in the temperature range 100<T<300 K are used to characterize the crystalline quality of epitaxial layers of a prototypical oxide, SrTiO3. Twenty samples from five institutions using two growth techniques, molecular beam epitaxy and pulsed laser deposition (PLD), were analyzed. Optimized growth conditions produce layers with Λ comparable to bulk single crystals. Many PLD layers, particularly those that use ceramics as the target material, show surprisingly low Λ. For homoepitaxial layers, the decrease in Λ created by point defects correlates well with the expansion of the lattice parameter in the direction normal to the surface.

Transport in ferromagnetic GdTiO3 / SrTiO3 heterostructures

Epitaxial GdTiO3/SrTiO3 structures with different SrTiO3 layer thicknesses are grown on (001) (LaAlO3)0.3(Sr2AlTaO6)0.7 substrate surfaces by hybrid molecular beam epitaxy. It is shown that the formation of the pyrochlore (Gd2Ti2O7) phase can be avoided if GdTiO3 is grown by shuttered growth, supplying alternating monolayer doses of Gd and of the metalorganic precursor that supplies both Ti and O. Phase-pure GdTiO3 films grown by this approach exhibit magnetic ordering with a Curie temperature of 30 K. The electrical transport characteristics can be understood as being dominated by a conductive interface layer within the SrTiO3.

Structure and transport in high pressure oxygen sputter-deposited BaSnO3−δ

BaSnO3 has recently been identified as a high mobility wide gap semiconductor with significant potential for room temperature oxide electronics. Here, a detailed study of the high pressure oxygen sputter-deposition, microstructure, morphology, and stoichiometry of epitaxial BaSnO3 on SrTiO3(001) and MgO(001) is reported, optimized conditions resulting in single-phase, relaxed, close to stoichiometric films. Most significantly, vacuum annealing is established as a facile route to n-doped BaSnO3−δ, leading to electron densities above 1019 cm−3, 5 mΩ cm resistivities, and room temperature mobility of 20 cm2 V−1 s−1 in 300-A-thick films on MgO(001). Mobility limiting factors, and the substantial scope for their improvement, are discussed.

Enhancing the electron mobility of SrTiO3 with strain

We demonstrate, using high-mobility SrTiO3 thin films grown by molecular beam epitaxy, that stress has a pronounced influence on the electron mobility in this prototype complex oxide. Moderate strains result in more than 300% increases in the electron mobilities with values exceeding 120 000 cm2/V s and no apparent saturation in the mobility gains. The results point to a range of opportunities to tailor high-mobility oxide heterostructure properties and open up ways to explore oxide physics.

Effects of hydrogen anneals on oxygen deficient SrTio3-x single crystals

The influence of hydrogen gas anneals on the electrical properties of nominally undoped, oxygen-deficient SrTiO3−x single crystals was investigated. Titanium getter layers and vacuum anneals were used to obtain oxygen-deficient SrTiO3−x with a low electrical resistivity. These crystals showed an optical absorption peak at 2.92 eV and strong midinfrared absorption. Subsequent anneals at 800 °C in forming gas, which contained 10% hydrogen, returned the crystals into the insulating, transparent state. The mechanisms by which hydrogen anneals can compensate for the effects of oxygen vacancies in SrTiO3−x are discussed. The results show that forming gas anneals of stoichiometric SrTiO3 can lead to complex electrical conduction behavior.

Band alignment at epitaxial BaSnO3/SrTiO3(001) and BaSnO3/LaAlO3(001) heterojunctions

We have spectroscopically determined the optical bandgaps and band offsets at epitaxial interfaces of BaSnO3 with SrTiO3(001) and LaAlO3(001). 28 u.c. BaSnO3 epitaxial films exhibit direct and indirect bandgaps of 3.56 ± 0.05 eV and 2.93 ± 0.05 eV, respectively. The lack of a significant Burstein-Moss shift corroborates the highly insulating, defect-free nature of the BaSnO3 films. The conduction band minimum is lower in electron energy in 5 u.c. films of BaSnO3 than in SrTiO3 and LaAlO3 by 0.4 ± 0.2 eV and 3.7 ± 0.2 eV, respectively. This result bodes well for the realization of oxide-based, high-mobility, two-dimensional electron systems that can operate at ambient temperature, since electrons generated in the SrTiO3 by modulation doping, or at the BaSnO3/LaAlO3 interface by polarization doping, can be transferred to and at least partially confined in the BaSnO3 film.