Akimasa Yamada

Uniaxial locked epitaxy of ZnO on the a face of sapphire

High-quality, c-oriented ZnO epitaxial films have been grown on the a surface using molecular-beam epitaxy. The use of a-oriented sapphire eliminates rotational domains and related structural defects which have limited the use of ZnO in electronic applications. The ZnO epitaxial layers are uniquely oriented with the ZnO/sapphire orientational relationship [0001]‖[1120] and 〈1120〉‖[0001]. This unique orientation is a consequence of the anisotropy of the a-sapphire surface in conjunction with a strong correlation along a single direction leading to the term uniaxial locked epitaxy. High-resolution x-ray diffraction measurements show an increase in x-ray lateral coherence length from several tens of nanometers to >0.7 μm for growth of c-oriented ZnO on the a surface as opposed to the c surface of sapphire.

Interactions between gallium and nitrogen dopants in ZnO films grown by radical-source molecular-beam epitaxy

It has been recently predicted that the co-doping of an acceptor (nitrogen) and a donor (aluminum, gallium, indium) in a 2:1 ratio will dope ZnO p-type due to a reduction in the Madelung energy making the nitrogen acceptor energy level more shallow. We have been growing gallium and nitrogen co-doped ZnO films by radical-source molecular-beam epitaxy by use of oxygen and nitrogen radicals supplied via rf radical source cells. Diode-like current–voltage characteristics and donor acceptor pair-like photoluminescence emission were observed for a Ga and N doped ZnO film grown on an undoped ZnO buffer layer. However, Hall measurements revealed that the conductivity was n-type. Formation of a non-ZnO phase in the sample was confirmed by secondary ion mass spectroscopy and x-ray diffraction measurements. Zn and Zn+O secondary ion intensities fell sharply by two orders of magnitude in going from the undoped ZnO layer to the highly co-doped ZnO. X-ray diffraction measurements indicated the formation of ZnGa2O4.

Na-induced variations in the structural, optical, and electrical properties of Cu(In,Ga)Se2 thin films

The systematic variations in the structural, optical, and electrical properties of polycrystalline Cu(In,Ga)Se2 (CIGS) thin films with Na doping level were investigated. Precise control of the Na concentration in CIGS films was demonstrated using alkali-silicate glass thin layers of various thicknesses deposited on substrates prior to CIGS growth. The CIGS grain size was observed to decrease with increasing Na concentration, although the surface morphology became smoother and exhibited a stronger (112) texture, which has been demonstrated consequence of larger grain size. The Ga composition gradient in the CIGS films was found to become large due to the presence of Na during growth, which in turn led to a decrease in the nominal band gap energy. Variations in the photoluminescence spectra and electrical properties suggested that the formation of an acceptor energy state, which may originate from OSe point defects, was enhanced in the presence of Na. This result suggests that not only Na, but also the pres...

Band-gap modified Al-doped Zn1−xMgxO transparent conducting films deposited by pulsed laser deposition

Al-doped Zn1−xMgxO films have been deposited on glass substrates at a substrate temperature of 200°C by a pulsed laser deposition system. A resistivity of 3×10−4Ωcm was obtained at x=0.06. Film resistivity was found to increase with further increases in Mg composition. The maximum band gap of films with a resistivity ρ⩽1×10−3Ωcm was found to be 3.97eV, demonstrating band-gap engineering possibilities in the range of Eg=3.5–3.97eV with a resistivity ρ⩽1×10−3Ωcm. The average transmittance of the films was higher than 90% in the wavelength region λ=400–800nm, a range suitable for transparent conducting film applications.

Band gap energies of bulk, thin-film, and epitaxial layers of CuInSe2 and CuGaSe2

Band gap and excitonic resonance energies of high-quality bulk single crystals, polycrystalline thin films, and epitaxial layers of CuInSe2 and CuGaSe2 were determined as a function of temperature by means of photoreflectance, optical absorption (OA), and photoluminescence measurements. OA spectra were fit including excitonic absorption from low temperature up to room temperature (RT). The band gap energy of 1.032 eV and free exciton (FE) resonance energy of 1.024 eV were obtained at RT for strain-free CuInSe2 giving an exciton binding energy of 7.5 meV. The band gap energy of both CuInSe2 and CuGaSe2 was found to be essentially independent of the molar ratio of Cu to group-III atom (Cu/III) for near-stoichiometric and Cu-rich samples. The disappearance of the FE absorption in the In-rich (Cu/In<0.88) CuInSe2 thin films was explained by plasma screening of Coulomb interactions. A slight decrease in the band gap energy of the In-rich films was attributed to a degradation of film quality such as high-densit...

Polarization-induced two-dimensional electron gases in ZnMgO/ZnO heterostructures

Both the formation mechanism and the origin of the two-dimensional electron gas (2DEG) in ZnMgO/ZnO heterostructures have been investigated. The 2DEG in the heterostructures was confirmed to originate from polarization-induced charge and was found to be dominant for transport at low temperatures as well as room temperature (RT) by transport measurements. The origin of 2DEG was concluded to be the surface of the ZnMgO layer based on both capacitance-voltage measurements and the dependence of the carrier concentration on the ZnMgO layer thickness. The largest sheet carrier concentration was 1.1×1013 cm−2 and the highest mobility for the heterostructure was obtained for a Mg composition of 0.61 at RT.

Two-dimensional electron gas in Zn polar ZnMgO∕ZnO heterostructures grown by radical source molecular beam epitaxy

A two-dimensional electron gas was observed in Zn polar ZnMgO∕ZnO (ZnMgO on ZnO) heterostructures grown by radical source molecular beam epitaxy. The electron mobility of the ZnMgO∕ZnO heterostructures dramatically increased with increasing Mg composition and the electron mobility (μ∼250cm2∕Vs) at RT reached a value more than twice that of an undoped ZnO layer (μ∼100cm2∕Vs). The carrier concentration in turn reached values as high as ∼1×1013cm−2 and remained nearly constant regardless of Mg composition. Strong confinement of electrons at the ZnMgO∕ZnO interface was confirmed by C-V measurements with a concentration of over 4×1019cm−3. Temperature-dependent Hall measurements of ZnMgO∕ZnO heterostructures also exhibited properties associated with well defined heterostructures. The Hall mobility increased monotonically with decreasing temperature, reaching a value of 2750cm2∕Vs at 4K. Zn polar “ZnMgO on ZnO” structures are easy to adapt to a top-gate device. These results open new possibilities for high elec...

Improved External Efficiency InGaN-Based Light-Emitting Diodes with Transparent Conductive Ga-Doped ZnO as p-Electrodes

Transparent conductive Ga-doped ZnO (ZnO:Ga) was fabricated to serve as p-contacts of InGaN-based light-emitting diodes (LEDs) using molecular-beam epitaxy. As-grown ZnO:Ga films typically have resistivities of ?=2-4?10-4 ??cm, and over 80% transparency in the near UV and visible wavelength ranges. The current-voltage characteristics between as-grown ZnO:Ga contacts and p-GaN layers were ohmic. The brightness of LEDs fabricated with ZnO:Ga p-contacts was nearly double compared to LEDs with conventional Ni/Au p-contacts. We obtained the external efficiency as high as 20.8% in the case of the near UV LED. The forward voltage at 20 mA was found not to increase even after the lamp LED with ZnO:Ga were kept for 80 h in high humidity and high temperature environments.

Growth of Undoped ZnO Films with Improved Electrical Properties by Radical Source Molecular Beam Epitaxy

High-quality undoped ZnO epitaxial films with mobilities as high as 120 cm2V-1s-1 and carrier concentrations as low as 7.6 ×1016 cm-3 have been grown on (1120) a-sapphire substrates using low-temperature buffer layers, a slow substrate cooling process and a modified oxygen radical cell. Pole figure measurements reveal that a-plane sapphire substrates are effective for the elimination of 30° rotation domains, which usually appear in the case of ZnO growth on c-sapphire. The low-temperature buffer layers allow high-temperature growth, because initial ZnO growth does not occur with high initial growth temperature. The use of slow substrate cooling prevents the deterioration of the electrical properties of the ZnO films. Use of quartz insulators in the oxygen radical cell eliminates aluminum contamination, which is a serious problem when using conventional alumina insulators.

Alkali incorporation control in Cu(In,Ga)Se2 thin films using silicate thin layers and applications in enhancing flexible solar cell efficiency

Control of the alkali doping level in Cu(In,Ga)Se2 (CIGS) films was demonstrated using alkali-silicate thin layers of various thickness deposited on substrates prior to the sputtering of the Mo back contact layer. Not only the alkali density in the CIGS film, but also the Ga composition distribution in CIGS films, CIGS grain size, and consequent photovoltaic performance showed variations with the silicate layer thickness. Using alkali-silicate thin layers as an alkali source material, 17.4% and 17.7% efficiency flexible CIGS solar cells have been demonstrated on Ti and zirconia substrates, respectively.