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Title: Creation and Ordering of Oxygen Vacancies at WO 3-δ and Perovskite Interfaces

Abstract

Changes in structure and composition resulting from oxygen deficiency can strongly impact the physical and chemical properties of transition metal oxides, which may lead to new functionalities for novel electronic devices. Oxygen vacancies (V o) can be readily formed to accomodate the lattice mismatch during epitixial thin film growth. In this paper, the effects of substrate strain and oxidizing power on the creation and distribution of V o in WO 3-δ thin films are investigated in detail. An 18O 2 isotope labeled time-of-flight secondary ion mass spectrometry study reveals that WO 3-δ films grown on SrTiO 3 substrates display a significantly larger oxygen vacancy gradient along the growth direction compared to those grown on LaAlO 3 substrates. This result is corroborated by scanning transmission electron microscopy imaging which reveals a large number of defects close to the interface to accommodate interfacial tensile strain, leading to the ordering of V o and the formation of semi-aligned Magnéli phases. The strain is gradually released and tetragonal phase with much better crystallinity is observed at the film/vacuum interface. The changes in structure resulting from oxygen defect creation are shown to have a direct impact on the electronic and optical properties of the films.

Authors:
ORCiD logo [1];  [2]; ORCiD logo; ;  [3];  [4];  [5]; ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo
  1. College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P. R. China
  2. Key Laboratory of Photovoltaic Materials of Henan Province, School of Physics &, Electronics, Henan University, Kaifeng 475004, P. R. China
  3. Institute of Microstructure and Properties of Advanced Materials, Beijing University of Technolgoy, Beijing 100124, P. R. China
  4. Department of Chemistry, Beijing Key Laboratory of Microanalytical Methods and Instrumentation, Tsinghua University, Beijing 100084, P. R. China
  5. Department of Materials Science and Engineering, Southern Unviersity of Science and Technology, Shenzhen, Guangdong 518055, P. R. China
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1455307
Report Number(s):
PNNL-SA-132665
Journal ID: ISSN 1944-8244; 50084; KC0203020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Applied Materials and Interfaces; Journal Volume: 10; Journal Issue: 20
Country of Publication:
United States
Language:
English
Subject:
WO3; epitaxy; oxygen defects; reduction; SrTiO3; Environmental Molecular Sciences Laboratory

Citation Formats

Zhang, Kelvin H. L., Li, Guoqiang, Spurgeon, Steven R., Wang, Le, Yan, Pengfei, Wang, Zhaoying, Gu, Meng, Varga, Tamas, Bowden, Mark E., Zhu, Zihua, Wang, Chongmin, and Du, Yingge. Creation and Ordering of Oxygen Vacancies at WO3-δ and Perovskite Interfaces. United States: N. p., 2018. Web. doi:10.1021/acsami.8b03278.
Zhang, Kelvin H. L., Li, Guoqiang, Spurgeon, Steven R., Wang, Le, Yan, Pengfei, Wang, Zhaoying, Gu, Meng, Varga, Tamas, Bowden, Mark E., Zhu, Zihua, Wang, Chongmin, & Du, Yingge. Creation and Ordering of Oxygen Vacancies at WO3-δ and Perovskite Interfaces. United States. doi:10.1021/acsami.8b03278.
Zhang, Kelvin H. L., Li, Guoqiang, Spurgeon, Steven R., Wang, Le, Yan, Pengfei, Wang, Zhaoying, Gu, Meng, Varga, Tamas, Bowden, Mark E., Zhu, Zihua, Wang, Chongmin, and Du, Yingge. Wed . "Creation and Ordering of Oxygen Vacancies at WO3-δ and Perovskite Interfaces". United States. doi:10.1021/acsami.8b03278.
@article{osti_1455307,
title = {Creation and Ordering of Oxygen Vacancies at WO3-δ and Perovskite Interfaces},
author = {Zhang, Kelvin H. L. and Li, Guoqiang and Spurgeon, Steven R. and Wang, Le and Yan, Pengfei and Wang, Zhaoying and Gu, Meng and Varga, Tamas and Bowden, Mark E. and Zhu, Zihua and Wang, Chongmin and Du, Yingge},
abstractNote = {Changes in structure and composition resulting from oxygen deficiency can strongly impact the physical and chemical properties of transition metal oxides, which may lead to new functionalities for novel electronic devices. Oxygen vacancies (Vo) can be readily formed to accomodate the lattice mismatch during epitixial thin film growth. In this paper, the effects of substrate strain and oxidizing power on the creation and distribution of Vo in WO3-δ thin films are investigated in detail. An 18O2 isotope labeled time-of-flight secondary ion mass spectrometry study reveals that WO3-δ films grown on SrTiO3 substrates display a significantly larger oxygen vacancy gradient along the growth direction compared to those grown on LaAlO3 substrates. This result is corroborated by scanning transmission electron microscopy imaging which reveals a large number of defects close to the interface to accommodate interfacial tensile strain, leading to the ordering of Vo and the formation of semi-aligned Magnéli phases. The strain is gradually released and tetragonal phase with much better crystallinity is observed at the film/vacuum interface. The changes in structure resulting from oxygen defect creation are shown to have a direct impact on the electronic and optical properties of the films.},
doi = {10.1021/acsami.8b03278},
journal = {ACS Applied Materials and Interfaces},
number = 20,
volume = 10,
place = {United States},
year = {Wed Apr 25 00:00:00 EDT 2018},
month = {Wed Apr 25 00:00:00 EDT 2018}
}