Makoto Otani

Transport properties of d-electron-based transparent conducting oxide: Anatase Ti1−xNbxO2

The transport properties of a d-electron-based transparent conducting oxide, Nb-doped anatase Ti1−xNbxO2, were investigated as a function of the Nb content x. From optical resistivity spectra, the static effective mass was evaluated to be ∼0.4m0 in the low-carrier-concentration (ne) regime, which is approximately the same as those of conventional transparent conducting oxides (TCOs), and two orders of magnitude smaller than that reported for rutile TiO2. The Hall mobility at room temperature, which is maximized at around x=0.01 (ne∼1021cm−3), was found to be mainly dominated by optical phonon scattering unlike that of other TCOs.The transport properties of a d-electron-based transparent conducting oxide, Nb-doped anatase Ti1−xNbxO2, were investigated as a function of the Nb content x. From optical resistivity spectra, the static effective mass was evaluated to be ∼0.4m0 in the low-carrier-concentration (ne) regime, which is approximately the same as those of conventional transparent conducting oxides (TCOs), and two orders of magnitude smaller than that reported for rutile TiO2. The Hall mobility at room temperature, which is maximized at around x=0.01 (ne∼1021cm−3), was found to be mainly dominated by optical phonon scattering unlike that of other TCOs.

A high-throughput thermoelectric power-factor screening tool for rapid construction of thermoelectric property diagrams

The authors have developed a high-throughput screening tool that maps out thermoelectric power factors of combinatorial composition-spread film libraries. The screening tool allows one to measure the electrical conductivity and Seebeck coefficient of over 1000 sample points within 6h. Seebeck coefficients of standard films measured with the screening tool are in good agreement with those measured by traditional thermoelectric measurement apparatus. The rapid construction of thermoelectric property diagrams is illustrated for two systems: (Zn, Al)–O binary composition-spread film on Al2O3 (0001) and (Ca,Sr,La)3Co4O9 ternary composition-spread film on Si (100).

Texture and phase analysis of a Ca3Co4O9∕Si (100) thermoelectric film

This paper reports the texture analysis as well as the identification of two crystalline phases between a thin film of monoclinic Ca3Co4O9 and a cubic (100) Si substrate, using a diffractometer equipped with a two-dimensional area detector. No reflections other than 00l were observed in the symmetric configuration using an x-ray powder diffraction scan (Bragg-Brentano geometry). Pole figures collected for six reflections using asymmetric configurations did not show ab-plane epitaxial relationships between the film and the substrate. These results establish the Ca3Co4O9 fiber texture of the film with the (001) pole parallel to the surface normal. Single-crystal-like second phases, CaCoSi2O6 and CoO, presumably the interface reaction products of Ca3Co4O9 with the substrate Si, were identified. The near four-fold symmetry and the similar intensity displayed by the 220 reflection from the CaCoSi2O6 structure indicated an epitaxial relation between CaCoSi2O6 and Si, with four symmetry-induced variants being ge...

Model, prediction, and experimental verification of composition and thickness in continuous spread thin film combinatorial libraries grown by pulsed laser deposition

Pulsed laser deposition was used to grow continuous spread thin film libraries of continuously varying composition as a function of position on a substrate. The thickness of each component that contributes to a library can be empirically modeled to a bimodal cosine power distribution. We deposited ternary continuous spread thin film libraries from Al(2)O(3), HfO(2), and Y(2)O(3) targets, at two different background pressures of O(2): 1.3 and 13.3 Pa. Prior to library deposition, we deposited single component calibration films at both pressures in order to measure and fit the thickness distribution. Following the deposition and fitting of the single component films, we predict both the compositional coverage and the thickness of the libraries. Then, we map the thickness of the continuous spread libraries using spectroscopic reflectometry and measure the composition of the libraries as a function of position using mapping wavelength-dispersive spectrometry (WDS). We then compare the compositional coverage of the libraries and observe that compositional coverage is enhanced in the case of 13.3 Pa library. Our models demonstrate linear correlation coefficients of 0.98 for 1.3 Pa and 0.98 for 13.3 Pa with the WDS.

Statistical Analysis of a Round-Robin Measurement Survey of Two Candidate Materials for a Seebeck Coefficient Standard Reference Material.

In an effort to develop a Standard Reference Material (SRM™) for Seebeck coefficient, we have conducted a round-robin measurement survey of two candidate materials—undoped Bi2Te3 and Constantan (55 % Cu and 45 % Ni alloy). Measurements were performed in two rounds by twelve laboratories involved in active thermoelectric research using a number of different commercial and custom-built measurement systems and techniques. In this paper we report the detailed statistical analyses on the interlaboratory measurement results and the statistical methodology for analysis of irregularly sampled measurement curves in the interlaboratory study setting. Based on these results, we have selected Bi2Te3 as the prototype standard material. Once available, this SRM will be useful for future interlaboratory data comparison and instrument calibrations.

A High-Throughput Screening System for Thermoelectric Material Exploration Based on a Combinatorial Film Approach

A high-throughput system that consists of a combinatorial tool (a sputtering deposition tool and a pulsed laser deposition tool) and two developed property screening devices was used for thermoelectric material exploration. The thermoelectric power factor (S2?, S = Seebeck coefficient, ? = electrical conductivity) screening device allows us to measure electrical conductivity and Seebeck coefficient of over 1000 sample-points within 6 h. The thermal effusivity measurement system using the frequency domain thermoreflectance technique allows us to screen thermal conductivity of combinatorial/conventional films. Illustrations of these applications are provided with a Co?Sn?Ce/Si(100) film for power factor determination and with a Ba2YCu3O7/SrTiO3(100) film for thermal conductivity derivation.

High Throughput Screening Tools for Thermoelectric Materials

A suite of complementary high-throughput screening systems for combinatorial films was developed at National Institute of Standards and Technology to facilitate the search for efficient thermoelectric materials. These custom-designed capabilities include a facility for combinatorial thin film synthesis and a suite of tools for screening the Seebeck coefficient, electrical resistance (electrical resistivity), and thermal effusivity (thermal conductivity) of these films. The Seebeck coefficient and resistance are measured via custom-built automated apparatus at both ambient and high temperatures. Thermal effusivity is measured using a frequency domain thermoreflectance technique. This paper will discuss applications using these tools on representative thermoelectric materials, including combinatorial composition-spread films, conventional films, single crystals, and ribbons.

A phase relation study of Ba–Y–Cu–O coated-conductor films using the combinatorial approach

Phase relationships in bulk and thin film Ba–Y–Cu–O high-Tc superconductor system were determined at processing conditions relevant for industrial production of coated conductors. Our results demonstrated that the absence of BaY2CuO5 (which has a critical effect on flux pinning) at 735 °C—a typical temperature employed in production of coated conductors—in thin films processed in situ from the BaF2 precursor is caused by the sluggish reaction kinetics rather than by the presence of fluorine in the system. Thermodynamic calculations combined with annealing experiments confirmed that BaY2CuO5 is thermodynamically stable but forms at temperatures higher than 735 °C.

Phase relations in the Ba–Y–Cu–O films on SrTiO3 for the ex situ BaF2 process

In situ x-ray diffraction was used to establish the phase relations in high-Tc superconductor Ba–Y–Cu–O films grown on SrTiO3 through the ex situ BaF2 process. These relations differ from bulk equilibrium phase assemblages in the BaO–Y2O3–CuOx system. In particular, BaY2CuO5 (the “green phase”), a common impurity phase in bulk processing, is absent in the films. Because of the absence of this green phase, the compositional stability field of Ba2YCu3O6+x expands considerably as compared to that of the bulk system, resulting in the tie lines Ba2YCu3O6+x–Y2O3 and Ba2YCu3O6+x–Y2Cu2O5.

Thermoelectric and Structural Characterization of Ba2Ho(Cu3-xCox)O6+y

The search for thermoelectric materials for power generation and for solid-state cooling has led to increased interest of layered cobalt-containing oxides because of their thermal stability at high temperature and their desirable thermoelectric properties. This paper examines the effect of substitution of Co in the layered pervoskite Ba2Ho(Cu3−xCox)O6+y (x=0.3, 0.4, 0.5, 0.6, and 1.0). Structural analysis using the neutron Rietveld refinement technique reveals that when x≤0.4, Co substitutes mainly for Cu in the “chain sites” of the Ba2Ho(Cu3−xCox)O6+y structure. As x>0.4, Co also enters in the Cu-O “plane sites” as well. The thermoelectric properties of polycrystalline Ba2Ho(Cu3−xCox)O6+y samples were studied in the temperature range of 10–390 K. In general, as the cobalt content x increases, the resistivity and Seebeck coefficient of these samples increase while the thermal conductivity decreases. Among the five Ba2Ho(Cu3−xCox)O6+y compositions, the x=0.4 member gives the highest figure of merit ZT of ≈...