Journal
NANO LETTERS
Volume 17, Issue 2, Pages 794-799Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b03986
Keywords
Strongly correlated oxides; strain engineering; oxygen vacancies; X-ray spectroscopy
Categories
Funding
- U.S. Army Research Office [W911NF-15-1-0181]
- U.S. Department of Energy, Office of Science [DE-SC0004764]
- ETH Zurich
- ERG Advanced Grant program [291151]
- European research Council (ERG) [340279]
- Office of Science, Office of Basic Energy Sciences, US Department of Energy [DE-AC02-05CH11231]
- Swiss Supercomputing Center (CSCS) [s624]
- U.S. Department of Energy (DOE) [DE-SC0004764] Funding Source: U.S. Department of Energy (DOE)
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We demonstrate a novel pathway to control and stabilize oxygen vacancies in complex transition-metal oxide thin films. Using atomic layer-by-layer pulsed laser deposition (PLD) from two separate targets, we synthesize high-quality single-crystalline CaMnO3 films with systematically varying oxygen vacancy defect formation energies as controlled by coherent tensile strain. The systematic increase of the oxygen vacancy content in CaMnO3 as a function of applied in-plane strain is observed and confirmed experimentally using high-resolution soft X-ray absorption spectroscopy (XAS) in conjunction with bulk-sensitive hard X-ray photoemission spectroscopy (HAXPES). The relevant defect states in the densities of states are identified and the vacancy content in the films quantified using the combination of first-principles theory and corehole multiplet calculations with holistic fitting. Our findings open up a promising avenue for designing and controlling new ionically active properties and functionalities of complex transition-metal oxides via strain-induced oxygen-vacancy formation and ordering.
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