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Title: Thin-film nano-thermogravimetry applied to praseodymium-cerium oxide films at high temperatures

Abstract

High precision measurements of oxygen nonstoichiometry δ in thin film metal oxides MaOb±δ at elevated temperatures and controlled oxygen partial pressures pO2 are reported with the aid of resonant microbalances. The resonant microbalances applied here consisted of y-cut langasite (La3Ga5SiO14) and CTGS (Ca3TaGa3Si2O14) piezoelectric resonators, operated in the thickness shear mode at ~5 MHz. Measurements of variations in δ of Pr0.1Ce0.9O2-δ (PCO) films are reported for the oxygen partial pressure range from 10–8 bar to 0.2 bar at 700 °C, and these findings were discovered to be in good agreement with previously reported oxygen nonstoichiometry δ data derived from chemical capacitance studies. The PCO thin-films were deposited via pulsed laser deposition on both sides of the resonators, whose series resonance frequency was tracked, converted into mass changes and, finally, into nonstoichiometry. The nonstoichiometry was observed to reach a plateau as the oxygen partial pressure dropped below about 10–5 bar, the behavior being attributed to the full reduction of Pr to the trivalent state. These resonators enable stable operation up to temperatures above 1000 °C, thereby maintaining high mass resolution suitable for determining oxygen nonstoichiometry variations in thin films deposited on such resonators. Here, for the given experimental conditions, a massmore » resolution of ~50 ng was achieved at 700 °C with the CTGS resonator.« less

Authors:
 [1];  [1];  [2];  [3];  [4]
  1. Technical Univ. of Clausthal, Goslar (Germany)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Redox Power Systems, College Park, MD (United States)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Stanford Univ., CA (United States)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1540184
Alternate Identifier(s):
OSTI ID: 1438069
Grant/Contract Number:  
SC0002633; DE SC0002633
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 112; Journal Issue: 21; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Schröder, Sebastian, Fritze, Holger, Bishop, Sean, Chen, Di, and Tuller, Harry L. Thin-film nano-thermogravimetry applied to praseodymium-cerium oxide films at high temperatures. United States: N. p., 2018. Web. doi:10.1063/1.5025389.
Schröder, Sebastian, Fritze, Holger, Bishop, Sean, Chen, Di, & Tuller, Harry L. Thin-film nano-thermogravimetry applied to praseodymium-cerium oxide films at high temperatures. United States. doi:10.1063/1.5025389.
Schröder, Sebastian, Fritze, Holger, Bishop, Sean, Chen, Di, and Tuller, Harry L. Mon . "Thin-film nano-thermogravimetry applied to praseodymium-cerium oxide films at high temperatures". United States. doi:10.1063/1.5025389. https://www.osti.gov/servlets/purl/1540184.
@article{osti_1540184,
title = {Thin-film nano-thermogravimetry applied to praseodymium-cerium oxide films at high temperatures},
author = {Schröder, Sebastian and Fritze, Holger and Bishop, Sean and Chen, Di and Tuller, Harry L.},
abstractNote = {High precision measurements of oxygen nonstoichiometry δ in thin film metal oxides MaOb±δ at elevated temperatures and controlled oxygen partial pressures pO2 are reported with the aid of resonant microbalances. The resonant microbalances applied here consisted of y-cut langasite (La3Ga5SiO14) and CTGS (Ca3TaGa3Si2O14) piezoelectric resonators, operated in the thickness shear mode at ~5 MHz. Measurements of variations in δ of Pr0.1Ce0.9O2-δ (PCO) films are reported for the oxygen partial pressure range from 10–8 bar to 0.2 bar at 700 °C, and these findings were discovered to be in good agreement with previously reported oxygen nonstoichiometry δ data derived from chemical capacitance studies. The PCO thin-films were deposited via pulsed laser deposition on both sides of the resonators, whose series resonance frequency was tracked, converted into mass changes and, finally, into nonstoichiometry. The nonstoichiometry was observed to reach a plateau as the oxygen partial pressure dropped below about 10–5 bar, the behavior being attributed to the full reduction of Pr to the trivalent state. These resonators enable stable operation up to temperatures above 1000 °C, thereby maintaining high mass resolution suitable for determining oxygen nonstoichiometry variations in thin films deposited on such resonators. Here, for the given experimental conditions, a mass resolution of ~50 ng was achieved at 700 °C with the CTGS resonator.},
doi = {10.1063/1.5025389},
journal = {Applied Physics Letters},
number = 21,
volume = 112,
place = {United States},
year = {2018},
month = {5}
}

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    Works referencing / citing this record:

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