Investigations on the Origin of Topotactic Phase Transition of LaCoO3 Thin Films with In Situ XRD and Ambient Pressure Hard X-ray Photoelectron Spectroscopy

Shin, Hyunsuk; Yun, Youngmin; Seo, Okkyun; Kim, Seongeun; Seo, Minsik; Kim, Dongwoo; Lim, Hojoon; Oh, Hojun; Jang, Subin; Kim, Kyungmin; Kang, Sae Hyun; Hunt, Adrian; Waluyo, Iradwikanari; Noh, Do Young; Mun, Bongjin Simon; Kang, Hyon Chol

doi:10.1021/acsami.4c15505

Title: Investigations on the Origin of Topotactic Phase Transition of LaCoO₃ Thin Films with In Situ XRD and Ambient Pressure Hard X-ray Photoelectron Spectroscopy

Journal Article · 26 December 2024 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.4c15505 · OSTI ID:2506715

^[1];

^[2]; Kim, Seongeun ^[3]; Seo, Minsik ^[1]; Kim, Dongwoo ^[4];

^[5]; Oh, Hojun ^[1]; Jang, Subin ^[1]; Kim, Kyungmin ^[1]; Kang, Sae Hyun ^[1];

^[5];

^[5]; Noh, Do Young ^[1];

^[1]; Kang, Hyon Chol ^[3]

Gwangju Inst. of Science and Technology (Korea, Republic of)
Japan Synchrotron Radiation Research Institute, Sayo, Hyogo (Japan)
Chosun University, Gwangju (Korea, Republic of)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

With the applications of in situ X-ray diffraction (XRD), electrical I–V measurement, and ambient pressure hard X-ray photoelectron spectroscopy (AP-HAXPES), the characteristics of the topotactic phase transition of LaCoO₃ (LCO) thin films are examined. XRD measurements show clear evidence of structural phase transition (SPT) of the LCO thin films from the perovskite (PV) LaCoO₃ to the brownmillerite (BM) La₂Co₂O₅ phases through the intermediate La₃Co₃O₈ phase at a temperature of 350 °C under high-vacuum conditions, ~10^–5 mbar. The reverse SPT from BM to PV phases is also found under ambient pressure (>100 mbar) of air near 100 °C. Both observed SPTs in XRD are also identified in the electrical I–V measurements, i.e., the metallic PV phase to the insulating BM phase and vice versa. During the onset of SPTs, the bulk chemical and electronic states of LCO thin films are monitored with AP-HAXPES. The oxidation states in Co 2p spectra indicate that the oxygen vacancies are closely related to the SPT of LCO thin films. Also, the presence of enlarged band gap is observed as the SPT from PV to BM phases takes place, revealing the modified electronic properties of LCO due to the creation of oxygen vacancies. In conclusion, the analysis of valence band structures is further compared to the I–V measurements.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Research Foundation of Korea (NRF); Japan Synchrotron Radiation Research Institute (JASRI)

Grant/Contract Number:: SC0012704

OSTI ID:: 2506715

Report Number(s):: BNL--227513-2025-JAAM

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 1 Vol. 17; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
AP-HAXPES
I–V measurement
LaCoO3
XRD
in situ
multimodal probe
structural phase transition
topotactic phase transition

Title: Investigations on the Origin of Topotactic Phase Transition of LaCoO3 Thin Films with In Situ XRD and Ambient Pressure Hard X-ray Photoelectron Spectroscopy

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Title: Investigations on the Origin of Topotactic Phase Transition of LaCoO₃ Thin Films with In Situ XRD and Ambient Pressure Hard X-ray Photoelectron Spectroscopy