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Title: Engineering metal oxidation using epitaxial strain

Journal Article · · Nature Nanotechnology
ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2];  [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6];  [3];  [3]; ORCiD logo [1];  [4]; ORCiD logo [1]
  1. Univ. of Minnesota, Minneapolis, MN (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Auburn Univ., AL (United States)
  4. Univ. of Delaware, Newark, DE (United States)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States). Materials Science Division
  6. Argonne National Laboratory (ANL), Argonne, IL (United States). X-ray Science Division

The oxides of platinum group metals are promising for future electronics and spintronics due to the delicate interplay of spin-orbit coupling and electron correlation energies. However, their synthesis as thin films remains challenging due to their low vapour pressures and low oxidation potentials. Here we show how epitaxial strain can be used as a control knob to enhance metal oxidation. Using Ir as an example, we demonstrate the use of epitaxial strain in engineering its oxidation chemistry, enabling phase-pure Ir or IrO2 films despite using identical growth conditions. The observations are explained using a density-functional-theory-based modified formation enthalpy framework, which highlights the important role of metal-substrate epitaxial strain in governing the oxide formation enthalpy. We also validate the generality of this principle by demonstrating epitaxial strain effect on Ru oxidation. The IrO2 films studied in our work further revealed quantum oscillations, attesting to the excellent film quality. The epitaxial strain approach we present could enable growth of oxide films of hard-to-oxidize elements using strain engineering.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
Grant/Contract Number:
SC0012704; SC0020211; SC0023478; AC02-06CH11357; FA9550-21-1-0025; FA9550-21-0460; FA9550-20-1-0034; DMR-2011401; DMR-2129879; DMR-2011824; DMR-150099; 2138259; 2138286; 2138307; 2137603; 2138296; 1919839
OSTI ID:
1984413
Report Number(s):
BNL-224486-2023-JAAM
Journal Information:
Nature Nanotechnology, Vol. 18; ISSN 1748-3387
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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