Journal
ADVANCED MATERIALS
Volume 31, Issue 33, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201902493
Keywords
chemomechanical coupling; electrochemical titration; oxide perovskites; Raman spectroscopy
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Funding
- Swiss National Science Foundation (SNF) [BSSGI0_155986] Funding Source: Swiss National Science Foundation (SNF)
- U.S. Department of Energy (DOE) [DE-SC0002633] Funding Source: U.S. Department of Energy (DOE)
- National Science Foundation [DMR-14-19807] Funding Source: Medline
- Swiss National Science Foundation [BSSGI0_155986 / 1] Funding Source: Medline
- U.S. Department of Energy [DE-SC0002633] Funding Source: Medline
- US-DOE Basic Energy Sciences [DE-SC0002633] Funding Source: Medline
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Effective integration of perovskite films into devices requires knowledge of their electro-chemomechanical properties. Raman spectroscopy is an excellent tool for probing such properties as the films' vibrational characteristics couple to the lattice volumetric changes during chemical expansion. While lattice volumetric changes are typically accessed by analyzing Raman shifts as a function of pressure, stress, or temperature, such methods can be impractical for thin films and do not capture information on chemical expansion. An in situ Raman spectroscopy technique using an electrochemical titration cell to change the oxygen nonstoichiometry of a model perovskite film, Sr(Ti,Fe)O-3-(y)& x2006;, is reported and the lattice vibrational properties are correlated to the material's chemical expansion. How to select an appropriate Raman vibrational mode to track the evolution in oxygen nonstoichiometry is discussed. Subsequently, the frequency of the oxygen stretching mode around Fe4+ is tracked, as it decreases during reduction as the material expands and increases during reoxidation as the material shrinks. This methodology of oxygen pumping and in situ Raman spectroscopy of oxide films enables future in operando measurements even for small material volumes, as is typical for applications of films as electrodes or electrolytes utilized in electrochemical energy conversion or memory devices.
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