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Tailoring of an unusual oxidation state in a lanthanum tantalum(IV) oxynitride via precursor microstructure design

Bubeck, Cora and Widenmeyer, Marc and Richter, Gunther and Coduri, Mauro and Goering, Eberhard and Yoon, Songhak and Weidenkaff, Anke (2019):
Tailoring of an unusual oxidation state in a lanthanum tantalum(IV) oxynitride via precursor microstructure design.
In: Communications Chemistry, 2 (1), ISSN 2399-3669,
DOI: 10.1038/s42004-019-0237-x,
[Article]

Abstract

Perovskite-type oxynitrides hold great potential for optical applications due to their excellent visible light absorption properties. However, only a limited number of such oxynitrides with modulated physical properties are available to date and therefore alternative fabrication strategies are needed to be developed. Here, we introduce such an alternative strategy involving a precursor microstructure controlled ammonolysis. This leads to the perovskite family member LaTa(IV)O2N containing unusual Ta4+ cations. The adjusted precursor microstructures as well as the ammonia concentration are the key parameters to precisely control the oxidation state and O:N ratio in LaTa(O,N)3. LaTa(IV)O2N has a bright red colour, an optical bandgap of 1.9 eV and a low (optically active) defect concentration. These unique characteristics make this material suitable for visible light-driven applications and the identified key parameters will set the terms for the targeted development of further promising perovskite family members.

Item Type: Article
Erschienen: 2019
Creators: Bubeck, Cora and Widenmeyer, Marc and Richter, Gunther and Coduri, Mauro and Goering, Eberhard and Yoon, Songhak and Weidenkaff, Anke
Title: Tailoring of an unusual oxidation state in a lanthanum tantalum(IV) oxynitride via precursor microstructure design
Language: English
Abstract:

Perovskite-type oxynitrides hold great potential for optical applications due to their excellent visible light absorption properties. However, only a limited number of such oxynitrides with modulated physical properties are available to date and therefore alternative fabrication strategies are needed to be developed. Here, we introduce such an alternative strategy involving a precursor microstructure controlled ammonolysis. This leads to the perovskite family member LaTa(IV)O2N containing unusual Ta4+ cations. The adjusted precursor microstructures as well as the ammonia concentration are the key parameters to precisely control the oxidation state and O:N ratio in LaTa(O,N)3. LaTa(IV)O2N has a bright red colour, an optical bandgap of 1.9 eV and a low (optically active) defect concentration. These unique characteristics make this material suitable for visible light-driven applications and the identified key parameters will set the terms for the targeted development of further promising perovskite family members.

Journal or Publication Title: Communications Chemistry
Journal volume: 2
Number: 1
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Materials and Resources
Date Deposited: 20 May 2020 07:09
DOI: 10.1038/s42004-019-0237-x
Official URL: https://doi.org/10.1038/s42004-019-0237-x
Projects: We acknowledge the financial support of the European Synchrotron Radiation Facility, Grenoble, France and the synchrotron radiation beam time., This work was supported by the Deutsche Forschungsgemeinschaft within the priority program SPP 1613 "Solar H<INF>2</INF>" (WE 2803/7-1).
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