Woong-Jhae Lee

High Mobility in a Stable Transparent Perovskite Oxide

We discovered that La-doped BaSnO3 with the perovskite structure has an unprecedentedly high mobility at room temperature while retaining its optical transparency. In single crystals, the mobility reached 320 cm2 V-1 s-1 at a doping level of 8×1019 cm-3, constituting the highest value among wide-band-gap semiconductors. In epitaxial films, the maximum mobility was 70 cm2 V-1 s-1 at a doping level of 4.4×1020 cm-3. We also show that resistance of (Ba,La)SnO3 changes little even after a thermal cycle to 530 °C in air, pointing to an unusual stability of oxygen atoms and great potential for realizing transparent high-frequency, high-power functional devices.

Physical properties of transparent perovskite oxides (Ba,La)SnO3with high electrical mobility at room temperature

Transparent electronic materials are increasingly in demand for a variety of optoelectronic applications. BaSnO3 is a semiconducting oxide with a large band gap of more than 3.1 eV. Recently, we discovered that La doped BaSnO3 exhibits unusually high electrical mobility of 320 cm^2(Vs)^-1 at room temperature and superior thermal stability at high temperatures [H. J. Kim et al. Appl. Phys. Express. 5, 061102 (2012)]. Following that work, we report various physical properties of (Ba,La)SnO3 single crystals and films including temperature-dependent transport and phonon properties, optical properties and first-principles calculations. We find that almost doping-independent mobility of 200-300 cm^2(Vs)^-1 is realized in the single crystals in a broad doping range from 1.0x10^19 to 4.0x10^20 cm^-3. Moreover, the conductivity of ~10^4 ohm^-1cm^-1 reached at the latter carrier density is comparable to the highest value. We attribute the high mobility to several physical properties of (Ba,La)SnO3: a small effective mass coming from the ideal Sn-O-Sn bonding, small disorder effects due to the doping away from the SnO2 conduction channel, and reduced carrier scattering due to the high dielectric constant. The observation of a reduced mobility of ~70 cm^2(Vs)^-1 in the film is mainly attributed to additional carrier-scatterings which are presumably created by the lattice mismatch between the substrate SrTiO3 and (Ba,La)SnO3. The main optical gap of (Ba,La)SnO3 single crystals remained at about 3.33 eV and the in-gap states only slightly increased, thus maintaining optical transparency in the visible region. Based on these, we suggest that the doped BaSnO3 system holds great potential for realizing all perovskite-based, transparent high-frequency high-power functional devices as well as highly mobile two-dimensional electron gas via interface control of heterostructured films.

Enhanced electron mobility in epitaxial (Ba,La)SnO3 films on BaSnO3(001) substrates

We report the growth of Ba1−xLaxSnO3 (x = 0.00, 0.005, 0.01, 0.02, and 0.04) thin films on the insulating BaSnO3(001) substrate by pulsed laser deposition. The insulating BaSnO3 substrates were grown by the Cu2O-CuO flux, in which the molar fraction of KClO4 was systematically increased to reduce electron carriers and thus induce a doping induced metal-insulator transition, exhibiting a resistivity increase from ∼10−3 to ∼1012 Ω cm at room temperature. We find that all the Ba1−xLaxSnO3 films are epitaxial, showing good in-plane lattice matching with the substrate as confirmed by X-ray reciprocal space mappings and transmission electron microscopy studies. The Ba1−xLaxSnO3 (x = 0.005–0.04) films showed degenerate semiconducting behavior, and the electron mobility at room temperature reached 100 and 85 cm2 V−1 s−1 at doping levels 1.3 × 1020 and 6.8 × 1019 cm−3, respectively. This work demonstrates that thin perovskite stannate films of high quality can be grown on the BaSnO3(001) substrates for potential a...

Transparent Perovskite Barium Stannate with High Electron Mobility and Thermal Stability

Transparent conducting oxides (TCOs) and transparent oxide semiconductors (TOSs) have become necessary materials for a variety of applications in the information and energy technologies, ranging from transparent electrodes to active electronics components. Perovskite barium stannate (BaSnO3), a new TCO or TOS system, is a potential platform for realizing optoelectronic devices and observing novel electronic quantum states due to its high electron mobility, excellent thermal stability, high transparency, structural versatility, and flexible doping controllability. This article reviews recent progress in the doped BaSnO3 system, discussing the wide range of physical properties, electron-scattering mechanism, and demonstration of key semiconducting devices such as pn diodes and field-effect transistors. Moreover, we discuss the pathways to achieving two-dimensional electron gases at the interface between BaSnO3 and other perovskite oxides and describe remaining challenges for observing novel quantum phenomen...

Transparent p-CuI/n-BaSnO3−δ heterojunctions with a high rectification ratio

Transparent p-CuI/n-BaSnO3-δ heterojunction diodes were successfully fabricated by the thermal evaporation of a (1 1 1) oriented γ-phase CuI film on top of an epitaxial BaSnO3-δ (0 0 1) film grown by the pulsed laser deposition. Upon the thickness of the CuI film being increased from 30 to 400 nm, the hole carrier density was systematically reduced from 6.0  ×  1019 to 1.0  ×  1019 cm-3 and the corresponding rectification ratio of the pn diode was proportionally enhanced from ~10 to ~106. An energy band diagram exhibiting the type-II band alignment is proposed to describe the behavior of the heterojunction diode. A shift of a built-in potential caused by the hole carrier density change in the CuI film is attributed to the thickness-dependent rectification ratio. The best performing p-CuI/n-BaSnO3-δ diode exhibited a high current rectification ratio of 6.75  ×  105 at  ±2 V and an ideality factor of ~1.5.

Single crystal growth and optical properties of a transparent perovskite oxide LaInO3

Transparent LaInO3 single crystals have been grown using the optical floating zone method. Optimal growth, resulting in the highest optical transparency and best crystallinity, has been found at a growth speed of 15 mm/h and an O2 gas pressure of 10 bar. Under these conditions, single crystals as large as ∼4 × 4 mm2 have been obtained. Chemical compositions and structural analyses reveal that the resulting LaInO3 single crystal is stoichiometric without any impurity phase and forms an orthorhombic perovskite structure. Optical transmission spectra exhibit multiple optical transitions in a wide spectral range (0.5–4.2 eV). Although the main optical absorption occurs at ∼4.13 eV, weak absorption starts to develop from ∼1.4 eV, in agreement with an activation energy of ∼0.7 eV derived from electrical resistivity measurements. The dielectric constant e is found to be 23.7 at room temperature. This LaInO3 single crystal can be used as a transparent perovskite substrate for growing oxide semiconductors with lat...

Post-annealing effect on the electronic structure of Mn atoms in Ga1−xMnxAs probed by resonant inelastic x-ray scattering

The electronic structure of as-grown and post-annealed Ga(₁-x)Mn(x)As epilayers (x≈0.055) has been investigated using resonant inelastic x-ray scattering. Mn L₂,₃ x-ray emission spectra show that the integral intensity ratio of Mn L₂ to L₃ emission lines increases with annealing temperature and comes close to that of manganese oxide. The oxygen K-emission/absorption spectra of post-annealed Ga₀.₉₄₅Mn₀.₀₅₅As show 1.5-3.0 times higher degree of oxidation on the film surface than that of the as-grown sample. These experimental findings are attributed to the diffusion of Mn impurity atoms from interstitial positions in the GaAs host lattice to the surface where they are passivated by oxygen.

Realization of an atomically flat BaSnO3(001) substrate with SnO2 termination

Atomically flat terraces terminated by mostly single layer SnO2 are realized on the surface of a BaSnO3(001) substrate with a lateral dimension of about 3 × 3 mm2 by deionized water leaching and thermal annealing. Surface topography studies reveal that by controlling the annealing time and temperature, the topmost surface evolves from having chemically mixed termination to atomically flat terraces with a step height of one unit cell. The step bunching and kinked steps also depend sensitively on the out-of-plane and in-plane miscut angles. X-ray photoemission spectroscopy near the Ba3d5/2 and Sn3d5/2 states with variation in the electron emission angle confirmed that the topmost atomic layer of the BaSnO3−δ(001) surface mostly consisted of SnO2 rather than BaO. The present findings will facilitate the preparation of atomically flat BaSnO3(001) substrates, which will be useful in the studies of exploring possible two-dimensional electron gases at the interface between BaSnO3(001) and other oxides.