Project F – Room Temperature Aerosol Deposition of Lead-Free Ferroelectric Films for Energy Conversion Systems

The focus of this project is the investigation of lead-free ferroelectrics films for energy conversion applications using aerosol deposition (AD). During deposition, micron-sized particles are accelerated through a nozzle by a carrier gas into a vacuum chamber. The particles impact a substrate, breaking apart and forming a dense (>96 %) ceramic film at room temperature with an exceptionally high deposition rate. Because AD is a room temperature process, deposition of metallic, ceramic, semi-conductor, glass, or plastic particles on various substrates is possible. This is not achievable with other film deposition techniques requiring high temperature densification. Multi-layer composite structures consisting of alternating layers of different materials (2-2 connectivity) (Figure 1a) or mixed composite structures (0-3 connectivity) as well as porous films structures can also be produced, which could be used to optimize electromechanical properties or build-in additional functionalities.

Figure 1. (a) BaTiO₃/SrTiO₃ composite on Pt-electroded Si-wafer and a (b) porous BaTiO₃ film on a steel substrate.

The primary research goal is the improved understanding of the deposition of lead-free ferroelectric films for energy conversion applications using AD. Methods to thermally, chemically, and microstructurally tune the residual stress in the films will also be investigated, in addition to enhancement in electromechanical coupling using ceramic/ceramic composites and novel 3D film structures. In this project, novel high throughput ceramics processing methods will be used to investigate the role of stoichiometry on the deposition of photo-electro-mechancial materials.

Principal Investigators

	Prof. Dr. Kyle G. Webber Institute of Glass and Ceramics Materials Science Department Friedrich-Alexander-Universität Erlangen-Nürnberg kyle.g.webber@fau.de
	Prof. Dr. Ken-ichi Kakimoto Life Science and Applied Chemistry Department Frontier Research Institute for Materials Science Nagoya Institute of Technology kakimoto.kenichi@nitech.ac.jp
	Dr. Alexander Martin Biochemistry and Applied Chemistry Department Environmental Ceramics Division Nagoya Institute of Technology martin.alexander@nitech.ac.jp

Doctoral Researchers

	Michel Kuhfuß, M.Sc. Institute of Glass and Ceramics Materials Science Department Friedrich-Alexander-Universität Erlangen-Nürnberg michel.kuhfuss@fau.de
	Takumi Nozaki, M.Sc. Joint Degree Program in Energy Conversion Systems Nagoya Institute of Technology, Japan t.nozaki.974@stn.nitech.ac.jp

Junior/Co-Professors:

Prof. Dr. Daisuke Urushihara (NITech)

Publications Project F

2024

Darwish E., Elia J., Fehn D., Köllner D., Pourjafar A., Christiansen S., Meyer K., Webber KG., Brabec C., Batentschuk M., Osvet A.:
Brightly Luminescent and Color-Tunable CsPbBr3 Nanocrystals with Enhanced Stability and Room Temperature Cubic Structure through Codoping with MnCl2
In: Advanced Engineering Materials (2024)
ISSN: 1438-1656
DOI: 10.1002/adem.202302213
Dobesh D., Gadelmawla A., Miyazaki H., Hinterstein M., Kimura K., Maier J., Banerjee S., Zeair O., Mehta S., da Silva LL., Khansur NH., Hayashi K., de Ligny D., Webber KG., Cicconi MR.:
The role of Ca/Zr ratio on the local structure and phase transitions in lead-free (Ba,Ca)(Zr,Ti)O3
In: Journal of the European Ceramic Society (2024)
ISSN: 0955-2219
DOI: 10.1016/j.jeurceramsoc.2024.03.003
Kuhfuß M., Maier J., Hall DA., Xie B., Kleppe AK., Martin A., Kakimoto Ki., Khansur NH., Webber KG.:
In situ electric field-dependent structural changes in (Ba,Ca)(Zr,Ti)O3 with varying grain size
In: Journal of Applied Physics 135 (2024), Art.Nr.: 174101
ISSN: 0021-8979
DOI: 10.1063/5.0203652
Maier J., Fuggerer T., Urushihara D., Martin A., Khansur NH., Kakimoto Ki., Webber KG.:
The Impact of Grain Growth on the Functional Properties in Room-Temperature Powder Aerosol Deposited Free-Standing (Ba,Ca)(Zr,Ti)O3 Thick Films
In: Crystals 14 (2024), Art.Nr.: 296
ISSN: 2073-4352
DOI: 10.3390/cryst14040296
Maier J., Kuhfuß M., Urushihara D., Gadelmawla A., Khansur NH., Hall D., Algueró M., Martin A., Kakimoto Ki., Webber KG.:
Influence of grain size on electromechanical properties of (Ba,Ca)(Zr,Ti)O3: A multiscale analysis using spark plasma sintering and aerosol deposition
In: Ceramics International 50 (2024), S. 26780-26791
ISSN: 0272-8842
DOI: 10.1016/j.ceramint.2024.04.406
Marques LS., Weichelt M., Kuhfuß M., Rambo CR., Fey T.:
Novel Sol-Gel Synthesis Route for Ce- and V-Doped Ba0.85Ca0.15Ti0.9Zr0.1O3 Piezoceramics
In: Materials 17 (2024), Art.Nr.: 3228
ISSN: 1996-1944
DOI: 10.3390/ma17133228
Martin A., Kato N., Fey T., Webber KG., Kakimoto Ki.:
Increased thermal stability by the addition of ZrO2 into a 0.48Ba(Zr0.2Ti0.8)O3-0.52(Ba0.7Ca0.3)TiO3 matrix material
In: Japanese Journal of Applied Physics 63 (2024), Art.Nr.: 09SP02
ISSN: 0021-4922
DOI: 10.35848/1347-4065/ad6c58
Martin A., Maier J., Kakimoto Ki., Kamlah M., Webber KG.:
Observation of the local electromechanical response in 2-2 ceramic-ceramic lead-free ferroelectric composites via digital image correlation
In: Journal of Applied Physics 135 (2024), Art.Nr.: 044102
ISSN: 0021-8979
DOI: 10.1063/5.0184763
Urushihara D., Kobayashi R., Martin A., Asaka T., Webber KG., Kakimoto Ki.:
Microscopic evaluation of charged domain wall structure in niobium-based piezoceramics
In: Applied Physics Letters 125 (2024), Art.Nr.: 192904
ISSN: 0003-6951
DOI: 10.1063/5.0228587
Webber KG., Clemens O., Buscaglia V., Malič B., Bordia RK., Fey T., Eckstein U.:
Review of the opportunities and limitations for powder-based high-throughput solid-state processing of advanced functional ceramics
In: Journal of the European Ceramic Society 44 (2024), Art.Nr.: 116780
ISSN: 0955-2219
DOI: 10.1016/j.jeurceramsoc.2024.116780

2023

Maier J., Gadelmawla A., Khansur NH., Webber KG.:
Stress-induced tailoring of energy storage properties in lead-free Ba0.85Ca0.15Zr0.1Ti0.9O3 ferroelectric bulk ceramics
In: Journal of Materiomics 9 (2023), S. 673-682
ISSN: 2352-8478
DOI: 10.1016/j.jmat.2022.12.010
Martin A., Webber KG., Kakimoto Ki.:
Influence of Oxygen Vacancies on the Impedance Spectrum of Al2O3-Na0.5K0.5NbO3 Composites
In: Crystals 13 (2023)
ISSN: 2073-4352
DOI: 10.3390/cryst13030463
Tanaka H., Nozaki T., Martin A., Webber KG., Kakimoto Ki.:
Stress dependent impedance spectroscopy of niobium based ceramics
In: Japanese Journal of Applied Physics 62 (2023), Art.Nr.: SM1026
ISSN: 0021-4922
DOI: 10.35848/1347-4065/acedb8

2022

Eckstein U., Exner J., Bencan Golob A., Ziberna K., Drazic G., Ursic H., Wittkämper H., Papp C., Kita J., Moos R., Webber KG., Khansur NH.:
Temperature-dependent dielectric anomalies in powder aerosol deposited ferroelectric ceramic films
In: Journal of Materiomics 8 (2022), S. 1239-1250
ISSN: 2352-8478
DOI: 10.1016/j.jmat.2022.05.001
Eckstein U., Khansur NH., Bergler M., Urushihara D., Asaka T., Kakimoto KI., Sadl M., Dragomir M., Ursic H., de Ligny D., Webber KG.:
Room temperature deposition of freestanding BaTiO3 films: temperature-induced irreversible structural and chemical relaxation
In: Journal of Materials Science (2022)
ISSN: 0022-2461
DOI: 10.1007/s10853-022-07467-3
Eckstein U., Khansur NH., Urushihara D., Asaka T., Kakimoto Ki., Fey T., Webber KG.:
Defect modulated dielectric properties in powder aerosol deposited ceramic thick films
In: Ceramics International 48 (2022), S. 33082-33091
ISSN: 0272-8842
DOI: 10.1016/j.ceramint.2022.07.241
Martin A., Maier J., Streich F., Kamlah M., Webber KG.:
Investigating the importance of strain-coupling in lead-free 2-2 relaxor/ferroelectric composites with digital image correlation
In: Smart Materials & Structures 31 (2022)
ISSN: 0964-1726
DOI: 10.1088/1361-665X/ac6fa0
Shi X., Eckstein U., Lang S., Cicconi MR., Khansur NH.:
Temperature-dependent ferroelastic behaviour of antiferroelectric AgNbO3
In: Acta Materialia 232 (2022)
ISSN: 1359-6454
DOI: 10.1016/j.actamat.2022.117931
Wahl L., Maier J., Schmiedeke S., The-An Pham ., Fey T., Webber KG., Travitzky N., Khansur NH.:
Electromechanical properties of paper-derived potassium sodium niobate piezoelectric ceramics
In: Journal of the American Ceramic Society (2022)
ISSN: 0002-7820
DOI: 10.1111/jace.18655
Zhuo F., Eckstein U., Khansur NH., Dietz C., Urushihara D., Asaka T., Kakimoto KI., Webber KG., Fang X., Roedel J.:
Temperature-induced changes of the electrical and mechanical properties of aerosol-deposited BaTiO3 thick films for energy storage applications
In: Journal of the American Ceramic Society (2022)
ISSN: 0002-7820
DOI: 10.1111/jace.18377

2021

Khansur NH., Eckstein U., Ursic H., Sadl M., Brehl M., Martin A., Rieß K., de Ligny D., Webber KG.:
Enhanced Electromechanical Response and Thermal Stability of 0.93(Na1/2Bi1/2)TiO3-0.07BaTiO3 Through Aerosol Deposition of Base Metal Electrodes
In: Advanced Materials Interfaces (2021)
ISSN: 2196-7350
DOI: 10.1002/admi.202100309
Rieß K., Khansur NH., Martin A., Benčan A., Uršič H., Webber KG.:
Stress- And frequency-dependent properties of relaxor-like sodium bismuth titanate
In: Physical Review B 103 (2021), Art.Nr.: 094113
ISSN: 0163-1829
DOI: 10.1103/PhysRevB.103.094113
Sadl M., Condurache O., Bencan A., Dragomir M., Prah U., Malic B., Deluca M., Eckstein U., Hausmann D., Khansur NH., Webber KG., Ursic H.:
Energy-storage-efficient 0.9Pb(Mg1/3Nb2/3)O3–0.1PbTiO3 thick films integrated directly onto stainless steel
In: Acta Materialia 221 (2021), Art.Nr.: 117403
ISSN: 1359-6454
DOI: 10.1016/j.actamat.2021.117403
These A., Khansur NH., Almora O., Luer L., Matt G., Eckstein U., Barabash A., Osvet A., Webber KG., Brabec C.:
Characterization of Aerosol Deposited Cesium Lead Tribromide Perovskite Films on Interdigited ITO Electrodes
In: Advanced Electronic Materials (2021)
ISSN: 2199-160X
DOI: 10.1002/aelm.202001165

2020

Cicconi MR., Khansur NH., Eckstein U., Werr F., Webber KG., de Ligny D.:
Determining the local pressure during aerosol deposition using glass memory
In: Journal of the American Ceramic Society 103 (2020), S. 2443-2452
ISSN: 0002-7820
DOI: 10.1111/jace.16947
Martin A., Khansur NH., Eckstein U., Rieß K., Kakimoto Ki., Webber KG.:
High temperature piezoelectric response of polycrystalline Li-doped (K,Na)NbO3 ceramics under compressive stress
In: Journal of Applied Physics 127 (2020), Art.Nr.: 114101
ISSN: 0021-8979
DOI: 10.1063/1.5134554
Mashkov O., Körfer J., Eigen A., Yousefi Amin AA., Killilea NA., Barabash A., Sytnyk M., Khansur NH., Halik M., Webber KG., Heiß W.:
Effect of Ligand Treatment on the Tuning of Infrared Plasmonic Indium Tin Oxide Nanocrystal Electrochromic Devices
In: Advanced Engineering Materials (2020)
ISSN: 1438-1656
DOI: 10.1002/adem.202000112