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Volume 12
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10.3390/nano12061012
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Article

Widely Tuneable Composition and Crystallinity of Graded Na1+xTaO3±δ Thin Films Fabricated by Chemical Beam Vapor Deposition

by
Corrado Garlisi
1,*,
Petru Lunca Popa
1,
Kevin Menguelti
1,
Vincent Rogé
1,
Marc Michel
1,
Christèle Vergne
1,
Jérôme Guillot
1,
Estelle Wagner
2,
William Maudez
2,
Giacomo Benvenuti
2,
Bianca Rita Pistillo
1 and
Emanuele Barborini
1
1
Materials Research and Technology (MRT) Department, Luxembourg Institute of Science and Technology (LIST), L-4422 Belvaux, Luxembourg
2
3D-Oxides, F-01630 Saint Genis Pouilly, France
*
Author to whom correspondence should be addressed.
Nanomaterials 2022, 12(6), 1012; https://doi.org/10.3390/nano12061012
Submission received: 24 February 2022 / Revised: 15 March 2022 / Accepted: 16 March 2022 / Published: 19 March 2022
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Abstract

Combinatorial approach has been widely recognized as a powerful strategy to develop new-higher performance materials and shed the light on the stoichiometry-dependent properties of known systems. Herein, we take advantage of the unique features of chemical beam vapor deposition to fabricate compositionally graded Na1+xTaO3±δ thin films with −0.6 < x < 0.5. Such a varied composition was enabled by the ability of the employed technique to deliver and combine an extensive range of precursors flows over the same deposition area. The film growth occurred in a complex process, where precursor absolute flows, flow ratios, and substrate temperature played a role. The deviation of the measured Na/Ta ratios from those predicted by flow simulations suggests that a chemical-reaction limited regime underlies the growth mechanism and highlights the importance of the Ta precursor in assisting the decomposition of the Na one. The crystallinity was observed to be strongly dependent on its stoichiometry. High under-stoichiometries (e.g., Na0.5TaO3−δ) compared to NaTaO3 were detrimental for the formation of a perovskite framework, owing to the excessive amount of sodium vacancies and oxygen vacancies. Conversely, a well-crystallized orthorhombic perovskite structure peculiar of NaTaO3 was observed from mildly under-stoichiometric (e.g., Na0.9TaO3−δ) to highly over-stoichiometric (e.g., Na1.5TaO3+δ) compositions.
Keywords: chemical beam vapor deposition; compositionally graded Na1+xTaO3±δ; crystallinity spread; chemical reaction limited regime; sodium tantalate; perovskite chemical beam vapor deposition; compositionally graded Na1+xTaO3±δ; crystallinity spread; chemical reaction limited regime; sodium tantalate; perovskite

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MDPI and ACS Style

Garlisi, C.; Lunca Popa, P.; Menguelti, K.; Rogé, V.; Michel, M.; Vergne, C.; Guillot, J.; Wagner, E.; Maudez, W.; Benvenuti, G.; et al. Widely Tuneable Composition and Crystallinity of Graded Na1+xTaO3±δ Thin Films Fabricated by Chemical Beam Vapor Deposition. Nanomaterials 2022, 12, 1012. https://doi.org/10.3390/nano12061012

AMA Style

Garlisi C, Lunca Popa P, Menguelti K, Rogé V, Michel M, Vergne C, Guillot J, Wagner E, Maudez W, Benvenuti G, et al. Widely Tuneable Composition and Crystallinity of Graded Na1+xTaO3±δ Thin Films Fabricated by Chemical Beam Vapor Deposition. Nanomaterials. 2022; 12(6):1012. https://doi.org/10.3390/nano12061012

Chicago/Turabian Style

Garlisi, Corrado, Petru Lunca Popa, Kevin Menguelti, Vincent Rogé, Marc Michel, Christèle Vergne, Jérôme Guillot, Estelle Wagner, William Maudez, Giacomo Benvenuti, and et al. 2022. "Widely Tuneable Composition and Crystallinity of Graded Na1+xTaO3±δ Thin Films Fabricated by Chemical Beam Vapor Deposition" Nanomaterials 12, no. 6: 1012. https://doi.org/10.3390/nano12061012

APA Style

Garlisi, C., Lunca Popa, P., Menguelti, K., Rogé, V., Michel, M., Vergne, C., Guillot, J., Wagner, E., Maudez, W., Benvenuti, G., Pistillo, B. R., & Barborini, E. (2022). Widely Tuneable Composition and Crystallinity of Graded Na1+xTaO3±δ Thin Films Fabricated by Chemical Beam Vapor Deposition. Nanomaterials, 12(6), 1012. https://doi.org/10.3390/nano12061012

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