Abstract
Combining neutron diffraction with pair distribution function analysis, we have uncovered hidden reduced symmetry in the correlated metallic d1 perovskite, SrVO3. Specifically, we show that both the local and global structures are better described using a GdFeO3 distorted (orthorhombic) model as opposed to the ideal cubic ABO3 perovskite type. Recent reports of imaginary phonon frequencies in the density functional theory (DFT)-calculated phonon dispersion for cubic SrVO3 suggest a possible origin of this observed non-cubicity. Namely, the imaginary frequencies computed could indicate that the cubic crystal structure is unstable at T = 0 K. However, our DFT calculations provide compelling evidence that point defects in the form of oxygen vacancies, and not an observable symmetry breaking associated with calculated imaginary frequencies, primarily result in the observed non-cubicity of SrVO3. These experimental and computational results are broadly impactful because they reach into the thin-film and theoretical communities who have shown that SrVO3 is a technologically viable transparent conducting oxide material and have used SrVO3 to develop theoretical methods, respectively.
| Original language | English |
|---|---|
| Pages (from-to) | 3007-3017 |
| Number of pages | 11 |
| Journal | Inorganic Chemistry |
| Volume | 61 |
| Issue number | 7 |
| DOIs | |
| State | Published - Feb 21 2022 |
Funding
This research was mostly supported by the National Science Foundation (Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials) under Cooperative Agreement DMR-1539918. The neutron scattering portion of this research conducted at Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. S.P.R. and W.A.P. acknowledge DOE-Triad Contract 89233218NCA000001. All authors are grateful to Anja Völzke (Max Planck), who helped with the ICP-OES experiments, and W.A.P. and S.R.P. thank Sarah Hernandez (Los Alamos National Laboratory) for stimulating discussions. This research was mostly supported by the National Science Foundation (Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials) under Cooperative Agreement DMR-1539918. The neutron scattering portion of this research conducted at Oak Ridge National Laboratory?s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. S.P.R. and W.A.P. acknowledge DOE-Triad Contract 89233218NCA000001. All authors are grateful to Anja Vo?lzke (Max Planck), who helped with the ICP-OES experiments, and W.A.P. and S.R.P. thank Sarah Hernandez (Los Alamos National Laboratory) for stimulating discussions.