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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
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NIST X-ray Photoelectron Spectroscopy Database; National Institute of Standards and Technology: Gaithersburg, MD.
Note that the bulk peak of Ge was fixed at 29.7 eV in our previous paper,17 which was reported as the value for Ge 3d.22 Because we found 29.36 eV to be the binding energy of a more specific Ge 3d5/2 core line signal for the Ge bulk,23 we used it as the energy reference for the measured Ge 3d spectra.
NIST Electron Inelastic-Mean-Free-Path Database; National Institute of Standards and Technology: Gaithersburg, MD.
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The energy difference between the oxide and bulk peaks in X-ray photoelectron spectroscopy
(XPS) spectra was investigated 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. This may be related to the reported negative shift of flat band voltages in metal-oxide-semiconductor diodes with an air-exposed GeO2 layer.
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