Series of CuxO thin-films in the entire range of compositions 1≤x≤2 were obtained by varying the oxygen flux in an rf-sputter deposition process. Growth windows for three crystalline phases, i.e., the thermodynamically stable cuprous oxide Cu2O and cupric oxide CuO as well as the metastable paramelaconite Cu4O3, were observed. The crystalline phases persist non-stoichiometrically over a wide range of compositions. These flux-range windows are separated by ranges where highly disordered, almost amorphous material is obtained. All samples were analysed with respect to their thermoelectric properties, i.e., Seebeck coefficient, electrical, and thermal conductivity. Clear trends of these transport parameters were found and used to determine the thermoelectric figure of merit ZT. The ZT-values at room temperature are highest for the two thermodynamically stable crystalline phases CuO and Cu2O.
Multilayer samples of alternating n-type ZnO and insulating ZnS layers were deposited by radiofrequency (RF) magnetron sputtering on glass substrates. The number of ZnO/ZnS periods was varied throughout the series to increase the number of interfaces, whilst keeping the ratio of total thicknesses of ZnO and ZnS constant. Scanning electron microscopy (SEM) revealed the individual layers, but also a columnar structure. The in-plane Seebeck coefficient S and electric conductivity r were measured between 50 K and 300 K. The dependence of S and r on thickness d of the individual ZnO layers can be modeled by introducing a narrow interface layer of high conductivity for d > 100 nm. At lower d, fluctuations of the interfaces lead to additional effects on S and r which arise due to percolation and can be explained qualitatively in the framework of a network model.
We use a network model to calculate the influence of the mesoscopic interface structure on the thermoelectric properties of superlattice structures consisting of alternating layers of materials A and B. The thermoelectric figure of merit of such a composite material depends on the layer thickness, if interface resistances are accounted for, and can be increased by proper interface design. In general, interface roughness reduces the figure of merit, again compared to the case of ideal interfaces. However, the strength of this reduction depends strongly on the type of interface roughness. Smooth atomic surface diffusion leading to alloying of materials A and B causes the largest reduction of the figure of merit. Consequently, in real structures, it is important not only to minimize interface roughness, but also to control the type of roughness. Although the microscopic effects of interfaces are only empirically accounted for, using a network model can yield useful information about the dependence of the macroscopic transport coefficients on the mesoscopic disorder in structured thermoelectric materials.
A series of samples consisting of alternating stripes of ZnO grown by molecular-beam epitaxy (MBE) and radio-frequency (rf) sputtered Ga-doped ZnO stripes was laterally microstructured with a self-aligned pattern transfer method. We measured as a function of temperature the Seebeck coefficient S and the electrical resistivity r in-plane of the samples with the transport direction perpendicular to the stripe direction. Throughout the series the bar width and hence the number of interfaces was kept constant, but the interface profile was varied yielding different interface lengths and geometries. The dependence of S, r and the power factor S 2 /r on the interface length at room temperature were simulated using an empirical network model and it was demonstrated that the macroscopic transport coefficients are very sensitive to the interface region and that even this rather simple modelling yields useful information about the interface region.
A series of bar-shaped samples consisting of lateral arrangements of alternating ZnO:Al and ZnO stripes was fabricated by radiofrequency (RF)-sputtering and microfabrication techniques on glass substrates. Throughout the series, the number of interfaces between ZnO and ZnO:Al was varied whilst the material fractions of ZnO:Al and ZnO within the bars were not altered. Lateral thermoelectric transport parameters, i.e., Seebeck effect and electrical resistivity, were measured as a function of temperature for all microstructured samples and two reference samples of ZnO:Al and undoped ZnO. The transport direction through the bar was perpendicular to the stripe direction, such that the electrons and phonons have to pass all interfaces. The transport coefficients of the microstructured samples show clear dependence on the number of interfaces between ZnO and ZnO:Al. Thermoelectric measurements, photoluminescence, and Raman measurements indicate that this is due to diffusion of Al donors along the grain boundaries into the undoped ZnO stripes, which takes place during the fabrication process. Modeling of the dependence of the Seebeck coefficient and the resistivity of the series of samples on the basis of a network model accounting for donor diffusion supports these findings.
The thermal conductivity κ of ZnO can be significantly suppressed by alloying with a few percent of S offering the possibility of enhancing the thermoelectric figure of merit ZT. κ of radio-frequency sputtered wurtzite ZnO1–xSx thin-films was measured in the entire composition range x employing the 3ω-method. Both, incorporation of low amounts of S in ZnO and of O in ZnS reduce κ of the ZnO1–xSx-samples compared to the two binary compounds. The origin of the reduction of κ in the alloys is the formation of localized vibrational modes of S in ZnO and O in ZnS.
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