Pawel Ziolkowski

Potential-Seebeck-microprobe (PSM): measuring the spatial resolution of the Seebeck coefficient and the electric potential

Thermoelectric power generators are typically operating in a large temperature difference; indeed the properties of thermoelectric semiconductors vary with temperature. Thus the overall conversion efficiency is strongly dependent on spatial variations of the material properties according to the temperature profile along the entire thermoelectric generator element. Similarly, a functionally graded module is capable of accomplishing thermal sensors with linearised characteristics over a wide temperature range. The Seebeck-coefficient S is a measure of the electrically active components in a material. Different components in a single unit become visible by measuring the local S with a scanning thermoprobe. This applies accordingly for the electrical conductivity and therefore the behaviour of the material in a certain temperature gradient becomes predictable. A scanning Seebeck microprobe has been combined with the measurement of the electric potential along the surface of semiconducting or metallic material. A heated probe tip is placed onto the surface of the sample under investigation, measuring the Seebeck coefficient. Using a specially designed sample holder, an AC current can be applied to the specimen, allowing for the detection of the voltage drop between one current contact and the travelling probe tip. This voltage is proportional to the electrical conductivity at the tip position. With this technique a spatially resolved imaging of the Seebeck coefficient as well as the electrical conductivity can be performed. Furthermore the electrical contact resistance between different materials becomes visible, e.g., in segmented thermoelectric or other devices.

Simulations for the Development of Thermoelectric Measurements

In thermoelectricity, continuum theoretical equations are usually used for the calculation of the characteristics and performance of thermoelectric elements, modules or devices as a function of external parameters (material, geometry, temperatures, current, flow, load, etc.). An increasing number of commercial software packages aimed at applications, such as COMSOL and ANSYS, contain vkernels using direct thermoelectric coupling. Application of these numerical tools also allows analysis of physical measurement conditions and can lead to specifically adapted methods for developing special test equipment required for the determination of TE material and module properties. System-theoretical and simulation-based considerations of favorable geometries are taken into account to create draft sketches in the development of such measurement systems. Particular consideration is given to the development of transient measurement methods, which have great advantages compared with the conventional static methods in terms of the measurement duration required. In this paper the benefits of using numerical tools in designing measurement facilities are shown using two examples. The first is the determination of geometric correction factors in four-point probe measurement of electrical conductivity, whereas the second example is focused on the so-called combined thermoelectric measurement (CTEM) system, where all thermoelectric material properties (Seebeck coefficient, electrical and thermal conductivity, and Harman measurement of zT) are measured in a combined way. Here, we want to highlight especially the measurement of thermal conductivity in a transient mode. Factors influencing the measurement results such as coupling to the environment due to radiation, heat losses via the mounting of the probe head, as well as contact resistance between the sample and sample holder are illustrated, analyzed, and discussed. By employing the results of the simulations, we have developed an improved sample head that allows for measurements over a larger temperature interval with enhanced accuracy.

A sintered nanoparticle p-n junction observed by a Seebeck microscan

A nanoparticular p-n junction was realized by a field-assisted sintering process, using p-type and n-type doped silicon nanoparticles. A spatially resolved Seebeck microscan showed a broad transition from the positively doped to the negatively doped range. Overshoots on both sides are characteristic for the transition. Despite the tip size being much larger than the mean particle size, information about the dopant distribution between the particles is deduced from modeling the measured data under different assumptions, including the limited spatial resolution of the tip. The best match between measured and modeled data is achieved by the idea of doping compensation, due to the sintering process. Due to a short time at high temperature during the field-assisted sintering process, solid state diffusion is too slow to be solely responsible for the observed compensation of donors and acceptors over a wide range. Therefore, these measurements support a densification mechanism based on (partial) melting and rec...

Application Overview of the Potential Seebeck Microscope

The scanning Potential Seebeck Microscope (PSM) turned out to be a suitable tool to investigate material properties not only for thermoelectrics. Numerous cooperation and projects which were successfully accomplished by DLR and Panco and their national and international partners have shown the wide spectrum of application for this measurement instrument. The continuing extension of applications and further developments on this instrument were documented within several publications [Platzek, et al., 2005, Platzek, et al., 2005, Chen, et al., 2005, Ziolkowski, et al., 2006, Platzek, et al., 2003] showing the scientific output achieved by applying the PSM. With regard to the further developments which have been made and the results obtained so far, this work will give an overview of the possible applications of the PSM. This multiplexed informations will mark the present status of development and will give an outlook for further goals to reach

High-throughput characterization of the Seebeck coefficient of a-(Cr1 − xSix)1 − yOy thin film materials libraries as verification of the extended thermopower formula

In a previous paper (Sonntag 2010 J. Phys.: Condens. Matter 22 235501) the classical thermopower formula has been argued to be incomplete, because it only takes into account the scattering properties of the carriers, but not the temperature dependence of the electrochemical potential μ caused by variation of the carrier density and/or band edge shift with temperature T. This argument is now checked experimentally by high-throughput measurements of the thermopower (Seebeck coefficient) S of a-(Cr(1-x)Si(x))(1-y)O(y) thin film materials libraries. The concentration dependences of S differ depending on whether the measurements are done with the complete film (where x ranges continuously from x≈0.3 to 0.8; y≈0.1-0.2) or with the separated pieces (each piece with another average value of x). These differences are especially large if, in addition, an oxygen gradient is present.

Thermal conductivity, electrical resistivity, and dimensionless figure of merit (ZT) determination of thermoelectric materials by impedance spectroscopy up to 250 °C

Impedance spectroscopy has been shown as a promising method to characterize thermoelectric (TE) materials and devices. In particular, the possibility to determine the thermal conductivity λ, electrical conductivity σ, and the dimensionless figure of merit ZT of a TE element, if the Seebeck coefficient S is known, has been reported, although so far for a high-performance TE material (Bi2Te3) at room temperature. Here, we demonstrate the capability of this approach at temperatures up to 250 °C and for a material with modest TE properties. Moreover, we compare the results obtained with values from commercial equipment and quantify the precision and accuracy of the method. This is achieved by measuring the impedance response of a skutterudite material contacted by Cu contacts. The method shows excellent precision (random errors < 4.5% for all properties) and very good agreement with the results from commercial equipment (<4% for λ, between 4% and 6% for σ, and <8% for ZT), which proves its suitability to accurately characterize bulk TE materials. Especially, the capability to provide λ with good accuracy represents a useful alternative to the laser flash method, which typically exhibits higher errors and requires the measurement of additional properties (density and specific heat), which are not necessarily needed to obtain the ZT.

Application of High-Throughput Seebeck Microprobe Measurements on Thermoelectric Half-Heusler Thin Film Combinatorial Material Libraries

In view of the variety and complexity of thermoelectric (TE) material systems, combinatorial approaches to materials development come to the fore for identifying new promising compounds. The success of this approach is related to the availability and reliability of high-throughput characterization methods for identifying interrelations between materials structures and properties within the composition spread libraries. A meaningful characterization starts with determination of the Seebeck coefficient as a major feature of TE materials. Its measurement, and hence the accuracy and detectability of promising material compositions, may be strongly affected by thermal and electrical measurement conditions. This work illustrates the interrelated effects of the substrate material, the layer thickness, and spatial property distributions of thin film composition spread libraries, which are studied experimentally by local thermopower scans by means of the Potential and Seebeck Microprobe (PSM). The study is complemented by numerical evaluation. Material libraries of the half-Heusler compound system Ti-Ni-Sn were deposited on selected substrates (Si, AlN, Al2O3) by magnetron sputtering. Assuming homogeneous properties of a film, significant decrease of the detected thermopower Sm can be expected on substrates with higher thermal conductivity, yielding an underestimation of materials thermopower between 15% and 50%, according to FEM (finite element methods) simulations. Thermally poor conducting substrates provide a better accuracy with thermopower underestimates lower than 8%, but suffer from a lower spatial resolution. According to FEM simulations, local scanning of sharp thermopower peaks on lowly conductive substrates is linked to an additional deviation of the measured thermopower of up to 70% compared to homogeneous films, which is 66% higher than for corresponding cases on substrates with higher thermal conductivity of this study.