title: Strain-Engineered Oxygen Vacancies in CaMnO3Thin Films.
abstract: 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 CaMnO3films with systematically varying oxygen vacancy defect formation energies as controlled by coherent tensile strain. The systematic increase of the oxygen vacancy content in CaMnO3as 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 core-hole 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.
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.|Temple Materials Institute, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Ravini U
authors.identifier: 0000-0001-8766-0965
authors.initials: RU
authors.lastname: Chandrasena
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.|Temple Materials Institute, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Weibing
authors.initials: W
authors.lastname: Yang
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.|Temple Materials Institute, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Qingyu
authors.initials: Q
authors.lastname: Lei
authors.affiliation: Inorganic Chemistry & Catalysis, Debye Institute for Nanomaterials Science, Utrecht University , Universiteitsweg 99, Utrecht 3584 CG, The Netherlands.
authors.forename: Mario U
authors.initials: MU
authors.lastname: Delgado-Jaime
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.|Temple Materials Institute, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Kanishka D
authors.initials: KD
authors.lastname: Wijesekara
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.|Temple Materials Institute, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Maryam
authors.initials: M
authors.lastname: Golalikhani
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Bruce A
authors.initials: BA
authors.lastname: Davidson
authors.affiliation: Advanced Light Source, Lawrence Berkeley National Laboratory , One Cyclotron Road, Berkeley, California 94720, United States.
authors.forename: Elke
authors.initials: E
authors.lastname: Arenholz
authors.affiliation: Materials Sciences Research Center, Japan Atomic Energy Agency , 1-1-1 Kouto, Sayo-cho, Hyogo 679-5148, Japan.
authors.forename: Keisuke
authors.initials: K
authors.lastname: Kobayashi
authors.affiliation: Materials Sciences Research Center, Japan Atomic Energy Agency , 1-1-1 Kouto, Sayo-cho, Hyogo 679-5148, Japan.
authors.forename: Masaaki
authors.initials: M
authors.lastname: Kobata
authors.affiliation: Inorganic Chemistry & Catalysis, Debye Institute for Nanomaterials Science, Utrecht University , Universiteitsweg 99, Utrecht 3584 CG, The Netherlands.
authors.forename: Frank M F
authors.initials: FM
authors.lastname: de Groot
authors.affiliation: Materials Theory, ETH Zurich , Wolfgang-Pauli-Strasse 27, CH-8093 Zürich, Switzerland.|Department of Chemistry and Biochemistry, University of Bern , Freiestrasse 3, CH-3012 Bern, Switzerland.
authors.forename: Ulrich
authors.identifier: 0000-0002-1165-6377
authors.initials: U
authors.lastname: Aschauer
authors.affiliation: Materials Theory, ETH Zurich , Wolfgang-Pauli-Strasse 27, CH-8093 Zürich, Switzerland.
authors.forename: Nicola A
authors.initials: NA
authors.lastname: Spaldin
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.|Temple Materials Institute, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Xiaoxing
authors.initials: X
authors.lastname: Xi
authors.affiliation: Department of Physics, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.|Temple Materials Institute, Temple University , 1925 North 12th Street, Philadelphia, Pennsylvania 19122, United States.
authors.forename: Alexander X
authors.initials: AX
authors.lastname: Gray
keywords: Strongly correlated oxides; X-ray spectroscopy; oxygen vacancies; strain engineering,