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Title: Irradiation-induced reactions at the CeO2/SiO2/Si interface

Abstract

The influence of high-energy (1.6 MeV) Ar2+ irradiation on the interfacial interaction between cerium oxide thin films (~15 nm) with a SiO2/Si substrate is investigated using transmission electron microscopy, ultrahigh vacuum x-ray photoelectron spectroscopy (XPS), and a carbon monoxide (CO) oxidation catalytic reaction using ambient pressure XPS. The combination of these methods allows probing the dynamics of vacancy generation and its relation to chemical interactions at the CeO2/SiO2/Si interface. The results suggest that irradiation causes amorphization of some portion of CeO2 at the CeO2/SiO2/Si interface and creates oxygen vacancies due to the formation of Ce2O3 at room temperature. The subsequent ultra-high-vacuum annealing of irradiated films increases the concentration of Ce2O3 with the simultaneous growth of the SiO2 layer. Interactions with CO molecules result in an additional reduction of cerium and promote the transition of Ce2O3 to a silicate compound. Furthermore, thermal annealing of thin films exposed to oxygen or carbon monoxide shows that the silicate phase is highly stabile even at 450 °C.

Authors:
ORCiD logo [1];  [1];  [2];  [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Univ. of Notre Dame, IN (United States)
  2. Univ. of Hong Kong, Pokfulam (Hong Kong)
Publication Date:
Research Org.:
Univ. of Notre Dame, IN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1642347
Grant/Contract Number:  
NA0003888; PHY-1713857; FC02-04ER15533
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 152; Journal Issue: 10; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Oxide chemistry and catalysis; transmission electron microscopy; annealing; x-ray photoelectron spectroscopy; thin films; chemical processes; catalysts and catalysis; carbon monoxide

Citation Formats

Sapkota, Pitambar, Aprahamian, Ani, Chan, Kwong Yu, Frentz, Bryce, Macon, Kevin T., Ptasinska, Sylwia, Robertson, Daniel, and Manukyan, Khachatur. Irradiation-induced reactions at the CeO2/SiO2/Si interface. United States: N. p., 2020. Web. doi:10.1063/1.5142619.
Sapkota, Pitambar, Aprahamian, Ani, Chan, Kwong Yu, Frentz, Bryce, Macon, Kevin T., Ptasinska, Sylwia, Robertson, Daniel, & Manukyan, Khachatur. Irradiation-induced reactions at the CeO2/SiO2/Si interface. United States. https://doi.org/10.1063/1.5142619
Sapkota, Pitambar, Aprahamian, Ani, Chan, Kwong Yu, Frentz, Bryce, Macon, Kevin T., Ptasinska, Sylwia, Robertson, Daniel, and Manukyan, Khachatur. Mon . "Irradiation-induced reactions at the CeO2/SiO2/Si interface". United States. https://doi.org/10.1063/1.5142619. https://www.osti.gov/servlets/purl/1642347.
@article{osti_1642347,
title = {Irradiation-induced reactions at the CeO2/SiO2/Si interface},
author = {Sapkota, Pitambar and Aprahamian, Ani and Chan, Kwong Yu and Frentz, Bryce and Macon, Kevin T. and Ptasinska, Sylwia and Robertson, Daniel and Manukyan, Khachatur},
abstractNote = {The influence of high-energy (1.6 MeV) Ar2+ irradiation on the interfacial interaction between cerium oxide thin films (~15 nm) with a SiO2/Si substrate is investigated using transmission electron microscopy, ultrahigh vacuum x-ray photoelectron spectroscopy (XPS), and a carbon monoxide (CO) oxidation catalytic reaction using ambient pressure XPS. The combination of these methods allows probing the dynamics of vacancy generation and its relation to chemical interactions at the CeO2/SiO2/Si interface. The results suggest that irradiation causes amorphization of some portion of CeO2 at the CeO2/SiO2/Si interface and creates oxygen vacancies due to the formation of Ce2O3 at room temperature. The subsequent ultra-high-vacuum annealing of irradiated films increases the concentration of Ce2O3 with the simultaneous growth of the SiO2 layer. Interactions with CO molecules result in an additional reduction of cerium and promote the transition of Ce2O3 to a silicate compound. Furthermore, thermal annealing of thin films exposed to oxygen or carbon monoxide shows that the silicate phase is highly stabile even at 450 °C.},
doi = {10.1063/1.5142619},
journal = {Journal of Chemical Physics},
number = 10,
volume = 152,
place = {United States},
year = {Mon Mar 09 00:00:00 EDT 2020},
month = {Mon Mar 09 00:00:00 EDT 2020}
}

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