Modification of Band Structure by Oxygen Filling in Epitaxial La0.88Sr0.12MnO3−x Thin Films

Sangkyun Ryu; Jaejin Hwang; Jinhyung Cho; Younghak Kim; Ambrose Seo; Jaekwang Lee; Hyoungjeen Jeen

doi:10.1021/acsaelm.3c01380

Modification of Band Structure by Oxygen Filling in Epitaxial La_0.88Sr_0.12MnO_3−x Thin Films

Sangkyun Ryu, Jaejin Hwang, Jinhyung Cho, Younghak Kim, Ambrose Seo, Jaekwang Lee, Hyoungjeen Jeen

Research output: Contribution to journal › Article › peer-review

Abstract

Oxygen stoichiometry is a critical factor in transition-metal oxides, such as manganites, as it has a substantial influence on their electronic and magnetic properties through the generation of oxygen vacancies. However, the significance of oxygen stoichiometry is often underestimated in manganite thin films. In this study, we explore the formation of oxygen vacancies within La_0.88Sr_0.12MnO₃ (LSMO) under standard thin-film deposition conditions and elucidate how these vacancies can be effectively filled through exposure to high oxygen partial pressure (PO₂) on the order of several hundreds of Torr during the cooling phase. The oxygen replenishment process has a profound impact on the electronic band structure, resulting in alterations in electron occupancy near the Fermi level. This phenomenon is observed by optical spectroscopy and analyzed by density functional theory calculations. These findings underscore the indispensable nature of postdeposition oxygen annealing steps to attain stoichiometric LSMO thin films.

Original language	English
Pages (from-to)	370-375
Number of pages	6
Journal	ACS Applied Electronic Materials
Volume	6
Issue number	1
DOIs	https://doi.org/10.1021/acsaelm.3c01380
State	Published - 2024

Bibliographical note

Publisher Copyright:
© 2023 American Chemical Society.

Funding

This research was supported by NRF-Korea (NRF-2018R1D1A1B07045462). J.L. and H.J. acknowledge the support of the Korea Basic Science Institute (National Research Facilities and Equipment Center) through a grant funded by the Ministry of Education (No . 2021R1A6C101A429) for spectroscopic ellipsometry, X-ray diffraction, and DFT calculation. A.S. was supported by the National Science Foundation (Grant No. DMR-2104296). S.R. was supported by PNU-RENovation (2021\u22122022). This research was supported by NRF-Korea (NRF-2018R1D1A1B07045462). J.L. and H.J. acknowledge the support of the Korea Basic Science Institute (National Research Facilities and Equipment Center) through a grant funded by the Ministry of Education (No. 2021R1A6C101A429) for spectroscopic ellipsometry, X-ray diffraction, and DFT calculation. A.S. was supported by the National Science Foundation (Grant No. DMR-2104296). S.R. was supported by PNU-RENovation (2021\u20132022).

Funders	Funder number
NRF-Korea	NRF-2018R1D1A1B07045462
National Research Facilities and Equipment Center
PNU-RENovation
National Science Foundation Arctic Social Science Program	DMR-2104296
National Science Foundation Arctic Social Science Program
Ministry of Education China	2021R1A6C101A429
Ministry of Education China
Korea Basic Science Institute

Keywords

X-ray absorption spectroscopy
band structure
manganite thin film
oxygen vacancy
pulsed laser deposition

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Materials Chemistry
Electrochemistry

Access to Document

10.1021/acsaelm.3c01380

Cite this

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title = "Modification of Band Structure by Oxygen Filling in Epitaxial La0.88Sr0.12MnO3−x Thin Films",

abstract = "Oxygen stoichiometry is a critical factor in transition-metal oxides, such as manganites, as it has a substantial influence on their electronic and magnetic properties through the generation of oxygen vacancies. However, the significance of oxygen stoichiometry is often underestimated in manganite thin films. In this study, we explore the formation of oxygen vacancies within La0.88Sr0.12MnO3 (LSMO) under standard thin-film deposition conditions and elucidate how these vacancies can be effectively filled through exposure to high oxygen partial pressure (PO2) on the order of several hundreds of Torr during the cooling phase. The oxygen replenishment process has a profound impact on the electronic band structure, resulting in alterations in electron occupancy near the Fermi level. This phenomenon is observed by optical spectroscopy and analyzed by density functional theory calculations. These findings underscore the indispensable nature of postdeposition oxygen annealing steps to attain stoichiometric LSMO thin films.",

keywords = "X-ray absorption spectroscopy, band structure, manganite thin film, oxygen vacancy, pulsed laser deposition",

author = "Sangkyun Ryu and Jaejin Hwang and Jinhyung Cho and Younghak Kim and Ambrose Seo and Jaekwang Lee and Hyoungjeen Jeen",

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AU - Ryu, Sangkyun

AU - Hwang, Jaejin

AU - Cho, Jinhyung

AU - Kim, Younghak

AU - Seo, Ambrose

AU - Lee, Jaekwang

AU - Jeen, Hyoungjeen

PY - 2024

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N2 - Oxygen stoichiometry is a critical factor in transition-metal oxides, such as manganites, as it has a substantial influence on their electronic and magnetic properties through the generation of oxygen vacancies. However, the significance of oxygen stoichiometry is often underestimated in manganite thin films. In this study, we explore the formation of oxygen vacancies within La0.88Sr0.12MnO3 (LSMO) under standard thin-film deposition conditions and elucidate how these vacancies can be effectively filled through exposure to high oxygen partial pressure (PO2) on the order of several hundreds of Torr during the cooling phase. The oxygen replenishment process has a profound impact on the electronic band structure, resulting in alterations in electron occupancy near the Fermi level. This phenomenon is observed by optical spectroscopy and analyzed by density functional theory calculations. These findings underscore the indispensable nature of postdeposition oxygen annealing steps to attain stoichiometric LSMO thin films.

AB - Oxygen stoichiometry is a critical factor in transition-metal oxides, such as manganites, as it has a substantial influence on their electronic and magnetic properties through the generation of oxygen vacancies. However, the significance of oxygen stoichiometry is often underestimated in manganite thin films. In this study, we explore the formation of oxygen vacancies within La0.88Sr0.12MnO3 (LSMO) under standard thin-film deposition conditions and elucidate how these vacancies can be effectively filled through exposure to high oxygen partial pressure (PO2) on the order of several hundreds of Torr during the cooling phase. The oxygen replenishment process has a profound impact on the electronic band structure, resulting in alterations in electron occupancy near the Fermi level. This phenomenon is observed by optical spectroscopy and analyzed by density functional theory calculations. These findings underscore the indispensable nature of postdeposition oxygen annealing steps to attain stoichiometric LSMO thin films.

KW - X-ray absorption spectroscopy

KW - band structure

KW - manganite thin film

KW - oxygen vacancy

KW - pulsed laser deposition

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