The relation of the thermoelectric figure of merit and the nanocomposite morphology is studied for thermoelectric thin films consisting of poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) with different amounts of silicon nanoparticles (Si‐NPs). An increase in the figure of merit of up to 150% is found for an Si‐NP concentration of 0.5 wt% as compared to pristine PEDOT:PSS films. The improvement originates from a disruption in the molecular ordering and therefore reduced electrical conductivity, which leads to an increased Seebeck coefficient, while also reducing thermal conductivity for higher concentrations through phonon scattering. The thermal conductivity is measured with steady‐state IR thermography on free‐standing PEDOT:PSS/Si‐NP composite films, enabling a full determination of the figure of merit. The morphology is investigated with grazing incidence resonant tender X‐ray scattering (GIR‐TeXS) around the sulfur K‐absorption edge. Without need for extrinsic labeling, GIR‐TeXS measurements have varying scattering contrast conditions for the components of the ternary system. By comparing the scattered intensities at different photon energies with the corresponding scattering contrast, the Si‐NPs are found to be preferentially dispersed in the large and medium‐sized PEDOT‐rich domains. The changes in size for the PEDOT‐rich domains as function of Si‐NP concentration cause improvement of the thermoelectric properties of the films.
We review the Raman shift method as a non-destructive optical tool to investigate the thermal conductivity and demonstrate the possibility to map this quantity with a micrometer resolution by studying thin film and bulk materials for thermoelectric applications. In this method, a focused laser beam both thermally excites a sample and undergoes Raman scattering at the excitation spot. The temperature dependence of the phonon energies measured is used as a local thermometer. We discuss that the temperature measured is an effective one and describe how the thermal conductivity is deduced from single temperature measurements to full temperature maps, with the help of analytical or numerical treatments of heat diffusion. We validate the method and its analysis on 3-and 2-dimensional single crystalline samples before applying it to more complex Si-based materials. A suspended thin mesoporous film of phosphorus-doped laser-sintered Si 78 Ge 22 nanoparticles is investigated to extract the in-plane thermal conductivity from the effective temperatures, measured as a function of the distance to the heat sink. Using an iterative multigrid Gauss-Seidel algorithm the experimental data can be modelled yielding a thermal conductivity of 0.1 W/m K after normalizing by the porosity. As a second application we map the surface of a phosphorus-doped 3-dimensional bulknanocrystalline Si sample which exhibits anisotropic and oxygen-rich precipitates. Thermal conductivities as low as 11 W/m K are found in the regions of the precipitates, significantly lower than the 17 W/m K in the surrounding matrix. The present work serves as a basis to more routinely use the Raman shift method as a versatile tool for thermal conductivity investigations, both for samples with high and low thermal conductivity and in a variety of geometries.
We demonstrate a simple and quick method for the measurement of the in-plane thermal conductance of thin films via steady-state IR thermography. The films are suspended above a hole in an opaque substrate and heated by a homogeneous visible light source. The temperature distribution of the thin films is captured via infrared microscopy and fitted to the analytical expression obtained for the specific hole geometry in order to obtain the in-plane thermal conductivity. For thin films of poly(3,4-ethylenedioxythiophene):polystyrene sulfonate post-treated with ethylene glycol and of polyimide, we find conductivities of 1.0 W m K and 0.4 W m K at room temperature, respectively. These results are in very good agreement with literature values, validating the method developed.
Here we present the realization of efficient and sustainable silicon‐based thermoelectric materials from nanoparticles. We employ a gas phase synthesis for the nanoparticles which is capable of producing doped silicon (Si) nanoparticles, doped alloy nanoparticles of silicon and germanium (Ge), SixGe1–x, and doped composites of Si nanoparticles with embedded metal silicide precipitation phases. Hence, the so‐called “nanoparticle in alloy” approach, theoretically proposed in the literature, forms a guideline for the material development. For bulk samples, a current‐activated pressure‐assisted densification process of the nanoparticles was optimized in order to obtain the desired microstructure. For thin films, a laser annealing process was developed. Thermoelectric transport properties were characterized on nanocrystalline bulk samples and laser‐sintered‐thin films. Devices were produced from nanocrystalline bulk silicon in the form of p–n junction thermoelectric generators, and their electrical output data were measured up to hot side temperatures of 750 °C. In order to get a deeper insight into thermoelectric properties and structure forming processes, a 3D‐Onsager network model was developed. This model was extended further to study the p–n junction thermoelectric generator and understand the fundamental working principle of this novel device architecture. Gas phase synthesis of composite nanoparticles; nanocrystalline bulk with optimized composite microstructure; laser‐annealed thin film.
Doped thin films of group‐IV semiconductors can be fabricated using the adsorption of dopant species from a liquid source to a precursor nanoparticle film, followed by laser‐sintering to incorporate and activate the dopants in the sintered thin film. A detailed study of the doping of germanium films with arsenic reveals diffusion of dopants into the film and their adsorption to the nanoparticle surface as kinetically governing steps, benefiting from the large internal surface area of the nanoparticle film. The resulting charge carrier concentration can be adjusted by the internal surface area via the nanoparticle diameter, by controlling the dopant concentration in the liquid, and by the immersion time and temperature. It is shown that the method can be successfully transferred to silicon and silicon–germanium alloy films using group‐III and ‐V elements, which lead to p‐ and n‐type conductivity, respectively. Atomic dopant concentrations above 1020 cm−3 can be realized by laser‐sintering, which are electrically active to a high extent and lead to effective conductivities well above 10 S cm–1 in the mesoporous films is investigated here. The method allows flexible printing of devices using inks for the nanoparticles and the dopant and avoids toxic substances for the doping of nanoparticles in the gas phase.
We extend the infrared thermography of thin materials for measurements of the full time response to homogeneous heating via illumination. We demonstrate that the thermal conductivity, the heat capacity, as well as the thermal diffusivity can be determined comparing the experimental data to finite difference simulations using a variety of test materials such as thin doped and undoped silicon wafers, sheets of steel, as well as gold and polymer films. We show how radiative cooling during calibration and measurement can be accounted for and that the effective emissivity of the material investigated can also be measured by the setup developed.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
334 Leonard St
Brooklyn, NY 11211
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.