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Title: Comparative study of GeO2/Ge and SiO2/Si structures on anomalous charging of oxide films upon water adsorption revealed by ambient-pressure X-ray photoelectron spectroscopy

Abstract

The energy difference between the oxide and bulk peaks in X-ray photoelectron spectroscopy (XPS) spectra was investigated in this paper for both GeO2/Ge and SiO2/Si structures with thickness-controlled water films. This was achieved by obtaining XPS spectra at various values of relative humidity (RH) of up to ~15%. The increase in the energy shift is more significant for thermal GeO2 on Ge than for thermal SiO2 on Si above ~10-4% RH, which is due to the larger amount of water molecules that infiltrate into the GeO2 film to form hydroxyls. Analyzing the origins of this energy shift, we propose that the positive charging of a partially hydroxylated GeO2 film, which is unrelated to X-ray irradiation, causes the larger energy shift for GeO2/Ge than for SiO2/Si. A possible microscopic mechanism of this intrinsic positive charging is the emission of electrons from adsorbed water species in the suboxide layer of the GeO2 film to the Ge bulk, leaving immobile cations or positively charged states in the oxide. Finally, this may be related to the reported negative shift of flat band voltages in metal-oxide-semiconductor diodes with an air-exposed GeO2 layer.

Authors:
 [1];  [2];  [2];  [1];  [1];  [3];  [3];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Osaka Univ. (Japan). Graduate School of Engineering. Dept. of Precision Science and Technology
  2. Osaka Univ. (Japan). Graduate School of Engineering. Dept. of Material and Life Science
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Japan Society for the Promotion of Science (JSPS) (Japan); Murata Science Foundation (Japan); Mikiya Science and Technology Foundation (Japan)
OSTI Identifier:
1377479
Grant/Contract Number:  
AC02-05CH11231; JP24686020; JP26630026; JP16K14133
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 120; Journal Issue: 9; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Germanium; Elemental semiconductors; Water vapor; X-ray photoelectron spectroscopy; Adsorption

Citation Formats

Mori, Daichi, Oka, Hiroshi, Hosoi, Takuji, Kawai, Kentaro, Morita, Mizuho, Crumlin, Ethan J., Liu, Zhi, Watanabe, Heiji, and Arima, Kenta. Comparative study of GeO2/Ge and SiO2/Si structures on anomalous charging of oxide films upon water adsorption revealed by ambient-pressure X-ray photoelectron spectroscopy. United States: N. p., 2016. Web. doi:10.1063/1.4962202.
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Mori, Daichi, Oka, Hiroshi, Hosoi, Takuji, Kawai, Kentaro, Morita, Mizuho, Crumlin, Ethan J., Liu, Zhi, Watanabe, Heiji, & Arima, Kenta. Comparative study of GeO2/Ge and SiO2/Si structures on anomalous charging of oxide films upon water adsorption revealed by ambient-pressure X-ray photoelectron spectroscopy. United States. https://doi.org/10.1063/1.4962202
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Mori, Daichi, Oka, Hiroshi, Hosoi, Takuji, Kawai, Kentaro, Morita, Mizuho, Crumlin, Ethan J., Liu, Zhi, Watanabe, Heiji, and Arima, Kenta. Fri . "Comparative study of GeO2/Ge and SiO2/Si structures on anomalous charging of oxide films upon water adsorption revealed by ambient-pressure X-ray photoelectron spectroscopy". United States. https://doi.org/10.1063/1.4962202. https://www.osti.gov/servlets/purl/1377479.
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@article{osti_1377479,
title = {Comparative study of GeO2/Ge and SiO2/Si structures on anomalous charging of oxide films upon water adsorption revealed by ambient-pressure X-ray photoelectron spectroscopy},
author = {Mori, Daichi and Oka, Hiroshi and Hosoi, Takuji and Kawai, Kentaro and Morita, Mizuho and Crumlin, Ethan J. and Liu, Zhi and Watanabe, Heiji and Arima, Kenta},
abstractNote = {The energy difference between the oxide and bulk peaks in X-ray photoelectron spectroscopy (XPS) spectra was investigated in this paper for both GeO2/Ge and SiO2/Si structures with thickness-controlled water films. This was achieved by obtaining XPS spectra at various values of relative humidity (RH) of up to ~15%. The increase in the energy shift is more significant for thermal GeO2 on Ge than for thermal SiO2 on Si above ~10-4% RH, which is due to the larger amount of water molecules that infiltrate into the GeO2 film to form hydroxyls. Analyzing the origins of this energy shift, we propose that the positive charging of a partially hydroxylated GeO2 film, which is unrelated to X-ray irradiation, causes the larger energy shift for GeO2/Ge than for SiO2/Si. A possible microscopic mechanism of this intrinsic positive charging is the emission of electrons from adsorbed water species in the suboxide layer of the GeO2 film to the Ge bulk, leaving immobile cations or positively charged states in the oxide. Finally, this may be related to the reported negative shift of flat band voltages in metal-oxide-semiconductor diodes with an air-exposed GeO2 layer.},
doi = {10.1063/1.4962202},
journal = {Journal of Applied Physics},
number = 9,
volume = 120,
place = {United States},
year = {Fri Sep 02 00:00:00 EDT 2016},
month = {Fri Sep 02 00:00:00 EDT 2016}
}
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https://doi.org/10.1063/1.4962202
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    GeO 2 Encapsulated Ge Nanostructure with Enhanced Lithium-Storage Properties
    journal, January 2019

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    • Advanced Functional Materials, Vol. 29, Issue 8
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