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Register a new userStrain Control of Oxygen Vacancies in Epitaxial Strontium Cobaltite Films
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The ability to manipulate oxygen anion defects rather than metal cations in complex oxides can facilitate creating new functionalities critical for emerging energy and device technologies. However, the difficulty in activating oxygen at reduced temperatures hinders the deliberate control of important defects, oxygen vacancies. Here, strontium cobaltite (SrCoOx) is used to demonstrate that epitaxial strain is a powerful tool for manipulating the oxygen vacancy concentration even under highly oxidizing environments and at annealing temperatures as low as 300 C. By applying a small biaxial tensile strain (2%), the oxygen activation energy barrier decreases by ~30%, resulting in a tunable oxygen deficient steady-state under conditions that would normally fully oxidize unstrained cobaltite. These strain-induced changes in oxygen stoichiometry drive the cobaltite from a ferromagnetic metal towards an antiferromagnetic insulator. The ability to decouple the oxygen vacancy concentration from its typical dependence on the operational environment is useful for effectively designing oxides materials with a specific oxygen stoichiometry.
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Oxygen-defect control has long been considered an influential tuning knob for producing various property responses in complex oxide films. In addition to physical property changes, modification to the lattice structure, specifically lattice expansion, with increasing oxygen vacancy concentrations has been reported often and has become the convention for oxide materials. However, the current understanding of the lattice behavior in oxygen-deficient films becomes disputable when considering compounds containing different bonding environments or atomic layering. Moreover, tensile strain has recently been discovered to stabilize oxygen vacancies in epitaxial films, which further complicates the interpretation of lattice behavior resulting from their appearance. Here, we report on the selective strain control of oxygen vacancy formation and resulting lattice responses in the layered, Ruddlesden-Popper phases, La1.85Sr0.15CuO4. We found that a drastically reduced Gibbs free energy for oxygen vacancy formation near the typical growth temperature for tensile-strained epitaxial LSCO accounts for the large oxygen non-stoichiometry. Additionally, oxygen vacancies form preferentially in the equatorial position of the CuO2 plane, leading to a lattice contraction, rather than the expected expansion, observed with apical oxygen vacancies. Since oxygen stoichiometry plays a key role in determining the physical properties of many complex oxides, the strong strain coupling of oxygen nonstoichiometry and the unusual structural response reported here can provide new perspectives and understanding to the structure and property relationships of many other functional oxide materials.
The interrelation between the epitaxial strain and oxygen deficiency in La0.7Ca0.3MnO3-{delta} thin films was studied in terms of structural and functional properties. The films with a thickness of 1000{AA} were prepared using a PLD system equipped with a RHEED facility and a pyrometric film temperature control. The epitaxial strain and the oxygen deficiency in the samples were systematically modified using three different substrates: SrTiO3, (LaAlO3)0.3-(Sr2AlTaO6)0.7 and LaSrAlO4, and four different oxygen pressures during film growth ranging from 0.27mbar to 0.1mbar. It could be demonstrated that the oxygen incorporation depends on the epitaxial strain: oxygen vacancies were induced to accommodate tensile strain whereas the compressive strain suppressed the generation of oxygen vacancies.
Using {it ab initio} methods, we investigate the modification of the magnetic properties of the $m=2$ member of the strontium iridates Ruddlesden-Popper series Sr$_{m+1}$Ir$_{m}$O$_{3m+1}$, bilayer Sr$_3$Ir$_2$O$_7$, induced by epitaxial strain and oxygen vacancies. Unlike the single layer compound Sr$_2$IrO$_4$, which exhibits a robust in-plane magnetic order, the energy difference between in-plane and out-of-plane magnetic orderings in Sr$_3$Ir$_2$O$_7$ is much smaller and it is expected that small external perturbations could induce magnetic transitions. Our results indicate that epitaxial strain yields a spin-flop transition, that is driven by the crossover between the intralayer $J_1$ and interlayer $J_2$ magnetic exchange interactions upon compressive strain. While $J_1$ is essentially insensitive to strain effects, the strength of $J_2$ changes by one order of magnitude for tensile strains $geq$ 3~%. In addition, our study clarifies that the unusual in-plane magnetic response observed in Sr$_3$Ir$_2$O$_7$ upon the application of an external magnetic field originates from the canting of the local magnetic moments due to oxygen vacancies, which tilt the octahedral networks - thereby allowing for noncollinear spin configurations.
Elemental defects in transition metal oxides is an important and intriguing subject that result in modifications in variety of physical properties including atomic and electronic structure, optical and magnetic properties. Understanding the formation of elemental vacancies and their influence on different physical properties is essential in studying the complex oxide thin films. In this study, we investigated the physical properties of epitaxial SrRuO3 thin films by systematically manipulating cation and/or oxygen vacancies, via changing the oxygen partial pressure (P(O2)) during the pulsed laser epitaxy (PLE) growth. Ru vacancies in the low-P(O2)-grown SrRuO3 thin films induce lattice expansion with the suppression of the ferromagnetic TC down to ~120 K. Sr vacancies also disturb the ferromagnetic ordering, even though Sr is not a magnetic element. Our results indicate that both A and B cation vacancies in an ABO3 perovskite can be systematically engineered via PLE, and the structural, electrical, and magnetic properties can be tailored accordingly.
In the perovskite oxide SrCrO$_{3}$ the interplay between crystal structure, strain and orbital ordering enables a transition from a metallic to an insulating electronic structure under certain conditions. We identified a narrow window of oxygen partial pressure in which highly strained SrCrO$_{3}$ thin films can be grown using radio-frequency (RF) off-axis magnetron sputtering on three different substrates, (LaAlO$_{3}$)$_{0.3}$-(Sr$_{2}$TaAlO$_{6}$)$_{0.7}$ (LSAT), SrTiO$_{3}$ (STO) and DyScO$_{3}$ (DSO). X-ray diffraction and atomic force microscopy confirmed the quality of the films and a metal-insulator transition driven by the substrate induced strain was demonstrated.
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