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  • 1.
    Paul, Biplab
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Khranovskyy, Volodymyr
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Yakimova, Rositsa
    Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Donor-doped ZnO thin films on mica for fully-inorganic flexible thermoelectrics2019In: MATERIALS RESEARCH LETTERS, ISSN 2166-3831, Vol. 7, no 6, p. 239-243Article in journal (Refereed)
    Abstract [en]

    The development of fully-inorganic thin flexible materials is important for flexible thermoelectric applications in a wide temperature range, such as harvesting power from hot curved surfaces (e.g. hot pipes). Here, we investigate the thermoelectric properties of a series of ZnO:Ga,Al thin films with varying dopant concentration deposited on flexible mica substrate by atmospheric pressure metalorganic chemical vapor deposition. The films are bendable, while sustaining the high power factor, above 1 x 10(-4)Wm(-1)K(-2) for singly doped Zn0.99Ga0.01O film in a wide temperature range, from room temperature to 400 degrees C. IMPACT STATEMENTFor the first time we demonstrate here that ZnO-film-on-mica can be a promising n-type candidate for fully-inorganic flexible thermoelectrics, especially, for applications at elevated temperatures [GRAPHICS]

  • 2.
    Ekström, Erik
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Le Febvrier, Arnaud
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Fournier, Daniele
    Sorbonne Univ, France.
    Lu, Jun
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Ene, Vladimir-Lucian
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Univ Politehn Bucuresti, Romania.
    Van Nong, Ngo
    Tech Univ Denmark, Denmark.
    Eriksson, Fredrik
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Formation mechanism and thermoelectric properties of CaMnO3 thin films synthesized by annealing of Ca0.5Mn0.5O films2019In: Journal of Materials Science, ISSN 0022-2461, E-ISSN 1573-4803, Vol. 54, no 11, p. 8482-8491Article in journal (Refereed)
    Abstract [en]

    A two-step synthesis approach was utilized to grow CaMnO3 on M-, R- and C-plane sapphire substrates. Radio-frequency reactive magnetron sputtering was used to grow rock-salt-structured (Ca, Mn)O followed by a 3-h annealing step at 800 degrees C in oxygen flow to form the distorted perovskite phase CaMnO3. The effect of temperature in the post-annealing step was investigated using x-ray diffraction. The phase transformation to CaMnO3 started at 450 degrees C and was completed at 550 degrees C. Films grown on R- and C-plane sapphire showed similar structure with a mixed orientation, whereas the film grown on M-plane sapphire was epitaxially grown with an out-of-plane orientation in the [202] direction. The thermoelectric characterization showed that the film grown on M-plane sapphire has about 3.5 times lower resistivity compared to the other films with a resistivity of 0.077cm at 500 degrees C. The difference in resistivity is a result from difference in crystal structure, single orientation for M-plane sapphire compared to mixed for R- and C-plane sapphire. The highest absolute Seebeck coefficient value is -350 mu VK-1 for all films and is decreasing with temperature.

  • 3.
    Paul, Biplab
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Lu, Jun
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Growth of CaxCoO2 Thin Films by A Two-Stage Phase Transformation from CaO-CoO Thin Films Deposited by Rf-Magnetron Reactive Cosputtering2019In: NANOMATERIALS, ISSN 2079-4991, Vol. 9, no 3, article id 443Article in journal (Refereed)
    Abstract [en]

    The layered cobaltates A(x)CoO(2) (A: alkali metals and alkaline earth metals) are of interest in the area of energy harvesting and electronic applications, due to their good electronic and thermoelectric properties. However, their future widespread applicability depends on the simplicity and cost of the growth technique. Here, we have investigated the sputtering/annealing technique for the growth of CaxCoO2 (x = 0.33) thin films. In this approach, CaO-CoO film is first deposited by rf-magnetron reactive cosputtering from metallic targets of Ca and Co. Second, the as-deposited film is reactively annealed under O-2 gas flow to form the final phase of CaxCoO2. The advantage of the present technique is that, unlike conventional sputtering from oxide targets, the sputtering is done from the metallic targets of Ca and Co; thus, the deposition rate is high. Furthermore, the composition of the film is controllable by controlling the power at the targets.

  • 4.
    Ali, Sharafat
    et al.
    Linnaeus Univ, Sweden.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Magnusson, Roger
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Ekström, Erik
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Pallier, Camille
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. RISE IVF, S-58188 Linkoping, Sweden.
    Jonson, Bo
    Linnaeus Univ, Sweden.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Birch, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Optical and mechanical properties of amorphous Mg-Si-O-N thin films deposited by reactive magnetron sputtering2019In: Surface & Coatings Technology, ISSN 0257-8972, E-ISSN 1879-3347, Vol. 372, p. 9-15Article in journal (Refereed)
    Abstract [en]

    In this work, amorphous thin films in Mg-Si-O-N system typically containing amp;gt; 15 at.% Mg and 35 at.% N were prepared in order to investigate especially the dependence of optical and mechanical properties on Mg composition. Reactive RF magnetron co-sputtering from magnesium and silicon targets were used for the deposition of Mg-Si-O-N thin films. Films were deposited on float glass, silica wafers and sapphire substrates in an Ar, N-2 and O-2 gas mixture. X-ray photoelectron spectroscopy, atomic force microscopy, scanning electron microscopy, spectroscopic ellipsometry, and nanoindentation were employed to characterize the composition, surface morphology, and properties of the films. The films consist of N and Mg contents up to 40 at.% and 28 at.%, respectively and have good adhesion to substrates and are chemically inert. The thickness and roughness of the films increased with increasing content of Mg. Both hardness (16-21 GPa) and reduced elastic modulus (120-176 GPa) are strongly correlated with the amount of Mg content. The refractive index up to 2.01 and extinction coefficient up to 0.18 were found to increase with Mg content. The optical band gap (3.1-4.3) decreases with increasing the Mg content. Thin film deposited at substrate temperature of 100 degrees C shows a lower value of hardness (10 GPa), refractive index (1.75), and higher values of reduced elastic modulus (124 GPa) as compared to the thin film deposited at 310 degrees C and 510 degrees C respectively, under identical synthesis parameters.

  • 5.
    Sinha, Tridib Kumar
    et al.
    Indian Inst Technol, India; Gyeongsang Natl Univ, South Korea.
    Lee, Jinho
    Gyeongsang Natl Univ, South Korea.
    Kim, Jin Kuk
    Gyeongsang Natl Univ, South Korea.
    Ray, Samit K.
    Indian Inst Technol, India; SN Bose Natl Ctr Basic Sci, India.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rapid growth of fully-inorganic flexible CaxCoO2 thin films from a ligand free aqueous precursor ink for thermoelectric applications2019In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 55, no 54, p. 7784-7787Article in journal (Refereed)
    Abstract [en]

    We demonstrate a ligand-free green chemical method for the rapid growth of nanoporous Ca0.35CoO2 thin films on sapphire and mica substrates from a water-based precursor ink, formulated by dissolving the precursor solid, composed of in situ prepared Ca2+-DMF and Co2+-DMF complexes. Mica serves as the flexible substrate as well as the sacrificial layer for the film transfer. Despite the presence of nanopores, the power factor of the flexible film Ca0.35CoO2-on-mica is above 0.50 x 10(-4) W m(-1) K-2 at around room temperature. The present technique is simple and cost-effective.

  • 6.
    Du, Yong
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Shanghai Inst Technol, Peoples R China.
    Chen, Jiageng
    Shanghai Inst Technol, Peoples R China.
    Liu, Xin
    Shanghai Inst Technol, Peoples R China.
    Lu, Chun
    Shenyang Aerosp Univ, Peoples R China.
    Xu, Jiayue
    Shanghai Inst Technol, Peoples R China.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Flexible n-Type Tungsten Carbide/Polylactic Acid Thermoelectric Composites Fabricated by Additive Manufacturing2018In: Coatings, ISSN 2079-6412, Vol. 8, no 1, article id 25Article in journal (Refereed)
    Abstract [en]

    Flexible n-type tungsten carbide/polylactic acid (WC/PLA) composites were fabricated by additive manufacturing and their thermoelectric properties were investigated. The preparation of an n-type polymer-based thermoelectric composite with good stability in air atmosphere via additive manufacturing holds promise for application in flexible thermoelectric devices. For WC/PLA volume ratios varying from similar to 33% to 60%, the electrical conductivity of the composites increased from 10.6 to 42.2 S/cm, while the Seebeck coefficients were in the range -11 to -12.3 V/K. The thermal conductivities of the composites varied from similar to 0.2 to similar to 0.28 Wamp;lt;boldamp;gt;mamp;lt;/boldamp;gt;-1amp;lt;boldamp;gt;Kamp;lt;/boldamp;gt;-1 at similar to 300 K.

  • 7.
    Du, Yong
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Shanghai Inst Technol, Peoples R China.
    Xu, Jiayue
    Shanghai Inst Technol, Peoples R China.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Flexible thermoelectric materials and devices2018In: APPLIED MATERIALS TODAY, ISSN 2352-9407, Vol. 12, p. 366-388Article, review/survey (Refereed)
    Abstract [en]

    Thermoelectric generators (TEGs) can directly convert waste heat into electrical power. In the last few decades, most research on thermoelectrics has focused on inorganic bulk thermoelectric materials and corresponding devices, and their thermoelectric properties have been significantly improved. An emerging topic is flexible devices, where the use of bulk inorganic materials is precluded by their inherent rigidity. The purpose of this paper is to review the research progress on flexible thermoelectric materials and generators, including theoretical principles for TEGs, conducting polymer TE materials, nanocomposites comprised of inorganic nanostructures in polymer matrices and fully inorganic flexible TE materials in nanostructured thin films. Approaches for flexible TEGs and components are reviewed, and remaining challenges discussed. (C) 2018 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).

  • 8.
    Paul, Biplab
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Björk, Emma M.
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Kumar, Aparabal
    Materials Science Centre, Indian Institute of Technology, Kharagpur 721302, India.
    Lu, Jun
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Nanoporous Ca3Co4O9 Thin Films for Transferable Thermoelectrics2018In: ACS applied energy materials, ISSN 2574-0962, Vol. 1, no 5, p. 2261-2268Article in journal (Refereed)
    Abstract [en]

    The development of high-performance and transferable thin-film thermoelectric materials is important for low-power applications, e.g., to power wearable electronics, and for on-chip cooling. Nanoporous films offer an opportunity to improve thermoelectric performance by selectively scattering phonons without affecting electronic transport. Here, we report the growth of nanoporous Ca3Co4O9 thin films by a sequential sputtering-annealing method. Ca3Co4O9 is promising for its high Seebeck coefficient and good electrical conductivity and important for its nontoxicity, low cost, and abundance of its constituent raw materials. To grow nanoporous films, multilayered CaO/CoO films were deposited on sapphire and mica substrates by rf-magnetron reactive sputtering from elemental Ca and Co targets, followed by annealing at 700 C to form the final phase of Ca3Co4O9. This phase transformation is accompanied by a volume contraction causing formation of nanopores in the film. The thermoelectric propoperties of the nanoporous Ca3Co4O9 films can be altered by controlling the porosity. The lowest electrical resistivity is ~7 mO cm, yielding a power factor of 2.32 × 10-4 Wm-1K-2 near room temperature. Furthermore, the films are transferable from the primary mica substrates to other arbitrary polymer platforms by simple dry transfer, which opens an opportunity of low-temperature use these materials.

  • 9.
    Paul, Biplab
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Lu, Jun
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Nanostructural Tailoring to Induce Flexibility in Thermoelectric Ca3Co4O9 Thin Films2017In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 30, p. 25308-25316Article in journal (Refereed)
    Abstract [en]

    Because of their inherent rigidity and brittleness, inorganic materials have seen limited use in flexible thermoelectric applications. On the other hand, for high output power density and stability, the use of inorganic materials is required. Here, we demonstrate a concept of fully inorganic flexible thermoelectric thin films with Ca3Co4O9-on-mica. Ca3Co4O9 is promising not only because of its high Seebeck coefficient and good electrical conductivity but also because of the abundance, low cost, and nontoxicity of its constituent raw materials. We show a promising nanostructural tailoring approach to induce flexibility in inorganic thin-film materials, achieving flexibility in nanostructured Ca3Co4O9 thin films. The films were grown by thermally induced phase transformation from CaO-CoO thin films deposited by reactive rf-magnetron cosputtering from metallic targets of Ca and Co to the final phase of Ca3Co4O9 on a mica substrate. The pattern of nanostructural evolution during the solid-state phase transformation is determined by the surface energy and strain energy contributions, whereas different distributions of CaO and CoO phases in the as-deposited films promote different nanostructuring during the phase transformation. Another interesting fact is that the Ca3Co4O9 film is transferable onto an arbitrary flexible platform from the parent mica substrate by etch-free dry transfer. The highest thermoelectric power factor obtained is above 1 x 10(-4) W m(-1) K-2 in a wide temperature range, thus showing low-temperature applicability of this class of materials.

  • 10.
    Ali, Sharafat
    et al.
    Linnaeus University, Sweden; Corning Inc, NY 14831 USA.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Magnusson, Roger
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Broitman, Esteban
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Jonson, Bo
    Linnaeus University, Sweden.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Birch, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Synthesis and characterization of the mechanical and optical properties of Ca-Si-O-N thin films deposited by RF magnetron sputtering2017In: Surface & Coatings Technology, ISSN 0257-8972, E-ISSN 1879-3347, Vol. 315, p. 88-94Article in journal (Refereed)
    Abstract [en]

    Ca-Si-O-N thin films were deposited on commercial soda-lime silicate float glass, silica wafers and sapphire substrates by RF magnetron co-sputtering from Ca and Si targets in an Ar/N-2/O-2 gas mixture. Chemical composition, surface morphology, hardness, reduced elastic modulus and optical properties of the films were investigated using X-ray photoelectron spectroscopy, scanning electron microscopy, nanoindentation, and spectroscopic ellipsometry. It was found that the composition of the films can be controlled by the Ca target power, predominantly, and by the reactive gas flow. Thin films in the Ca-Si-O-N system are composed of N and Ca contents up to 31 eq. % and 60 eq. %, respectively. The films thickness ranges from 600 to 3000 nm and increases with increasing Ca target power. The films surface roughness varied between 2 and 12 nm, and approximately decreases with increasing power of Ca target. The hardness (4-12 GPa) and reduced elastic modulus (65-145 GPa) of the films increase and decrease with the N and Ca contents respectively. The refractive index (1.56-1.82) is primarily dictated by the N content. The properties are compared with findings for bulk glasses in the Ca-Si-(Al)-O-N systems, and it is concluded that Ca-Si-O-N thin films have higher values of hardness, elastic modulus and refractive index than bulk glasses of similar composition. (C) 2017 Elsevier B.V. All rights reserved.

  • 11.
    Ali, Sharafat
    et al.
    Linnaeus University, Sweden.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Magnusson, Roger
    Linköping University, Department of Physics, Chemistry and Biology, Applied Optics . Linköping University, Faculty of Science & Engineering.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Broitman, Esteban
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering.
    Jonson, Bo
    Linnaeus University, Sweden.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Birch, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Novel transparent Mg-Si-O-N thin films with high hardness and refractive index2016In: Vacuum, ISSN 0042-207X, E-ISSN 1879-2715, Vol. 131Article in journal (Refereed)
    Abstract [en]

    There is an increasing demand for glass materials with better mechanical and optical properties for display and electronic applications. This paper describes the deposition of novel thin films of Mg-circle divide-Si-O-N onto float glass substrates. Amorphous thin films in the Mg-Si-O-N system with high nitrogen and magnesium contents were deposited by reactive RF magnetron co-sputtering from Mg and Si targets in Ar/N-2/O-2 gas mixtures. The thin films studied span an unprecedented range of compositions up to 45 at% Mg and 80 at% N out of cations and anions respectively. Thin films in the Mg-Si-O-N system were found to be homogeneous and transparent in the visible region. Mechanical properties like hardness (H) and reduced elastic modulus (Er) show high values, up to 21 GPa and 166 GPa respectively. The refractive index (1.87-2.00) increases with increasing magnesium and nitrogen contents. (C) 2016 Elsevier Ltd. All rights reserved.

  • 12.
    Rawat, Pankaj K.
    et al.
    Indian Institute Technology, India; Science and Engn Research Board, India.
    Paul, Biplab
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Simple design for Seebeck measurement of bulk sample by 2-probe method concurrently with electrical resistivity by 4-probe method in the temperature range 300-1000 K2016In: Measurement, ISSN 0263-2241, E-ISSN 1873-412X, Vol. 91, p. 613-619Article in journal (Refereed)
    Abstract [en]

    The 4-probe method has so far been the most popular method for concurrent measurement of Seebeck coefficient and electrical resistivity of bulk samples. However, for Seebeck measurement with higher accuracy, the 2-probe method is becoming preferred over 4-probe method. The problem with the previous apparatus designs is that they do not allow 2-probe arrangement for Seebeck measurement simultaneously with linear 4-probe arrangement for electrical resistivity measurement. So, the challenge is find a design where two different probe arrangements become possible at the same time in a single measurement run. Here, we report design and fabrication of an apparatus that allows Seebeck measurement by 2-probe method concurrently with electrical resistivity by 4-probe method of bar and disc samples in the temperature range from 300 to 1000 K. The uniqueness of the present design is that it does not require heating the entire sample chamber for temperature dependent measurements. This is because a small cylindrical furnace inside the sample chamber is used to control the sample background temperature. This internal furnace arrangement results in readily achievable set temperature with desired uniformity. Thus, it allows faster thermoelectric evaluation of samples. The design includes several preventive steps to negate the effect of off-axial heat flows on the measurement accuracy. The measurement error in Seebeck coefficient and electrical resistivity of PbTe sample is estimated to be smaller than 5%. (C) 2016 Elsevier Ltd. All rights reserved.

  • 13.
    Paul, Biplab
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Schroeder, Jeremy Leroy
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Kerdsongpanya, Sit
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    van Nong, Ngo
    Risö-DTU, Denmark.
    Schell, Norbert
    Helmholtz-Zentrum Geestacht, Germany.
    Ostach, Daniel
    Helmholtz-Zentrum Geestacht, Germany.
    Lu, Jun
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Birch, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
    Mechanism of Formation of the Thermoelectric Layered Cobaltate Ca3Co4O9 by Annealing of CaO-CoO Thin Films2015In: Advanced Electronic Materials, ISSN 2199-160X, Vol. 1, no 3, article id 1400022Article in journal (Refereed)
    Abstract [en]

    The layered cobaltate Ca3Co4O9 is of interest for energy-harvesting and heat-conversion applications because of its good thermoelectric properties and the fact that the raw materials Ca and Co are nontoxic, abundantly available, and inexpensive. While single-crystalline Ca3Co4O9 exhibits high Seebeck coefficient and low resistivity, its widespread use is hampered by the fact that single crystals are too small and expensive. A promising alternative approach is the growth of highly textured and/or epitaxial Ca3Co4O9 thin films with correspondingly anisotropic properties. Here, we present a two-step sputtering/annealing method for the formation of highly textured virtually phase-pure Ca3Co4O9 thin films by reactive cosputtering from Ca and Co targets followed by an annealing process at 730 °C under O2-gas flow. The thermally induced phase transformation mechanism is investigated by in situ time-resolved annealing experiments using synchrotron-based 2D X-ray diffraction (XRD) as well as ex situ annealing experiments and standard lab-based XRD. By tuning the proportion of initial CaO and CoO phases during film deposition, the method enables synthesis of Ca3Co4O9 thin films as well as CaxCoO2. With this method, we demonstrate production of epitaxial Ca3Co4O9 thin films with in-plane electrical resistivity of 6.44 mΩ cm and a Seebeck coefficient of 118 μV K−1 at 300 K.

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