TY - JOUR
T1 - Octahedral rotations in Ruddlesden-Popper layered oxides under pressure from first principles
AU - Ramkumar, Sriram P.
AU - Nowadnick, Elizabeth A.
N1 - Funding Information:
U.S. Department of Energy
Funding Information:
This research used resources of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under Contract No. DE-SC0012704. This work also used the Extreme Science and Engineering Discovery Environment (XSEDE) Comet Cluster at the San Diego Supercomputer Center through the HPC@UC program. In addition, we acknowledge the use of computational resources supported by Academic and Research Computing Systems at the New Jersey Institute of Technology. The authors would like to acknowledge useful discussions with K. Rabe and D. Vanderbilt, as well as C. S. Hellberg, P. Nukala, and R. Cohen during the Ferro-2020 workshop.
Publisher Copyright:
© 2021 American Physical Society
PY - 2021/10/1
Y1 - 2021/10/1
N2 - The combination of reduced dimensionality and tunable structural distortions in layered perovskite oxides makes these materials ideal platforms for designing novel properties and functionalities. One example is hybrid improper ferroelectricity in Ruddlesden-Popper oxides, where the combination of a layered crystal structure and rotations of the metal-oxide octahedra break symmetry and induce a polarization. Precisely controlling the octahedral rotation distortions, for example by the application of hydrostatic pressure, provides a pathway to tune and optimize the properties of these materials. We combine group theoretic methods, density functional theory calculations, and Landau theory analysis to investigate how octahedral rotations respond to pressure in the hybrid improper ferroelectrics , and . We find that factors that are known to control the pressure response of perovskites—the formal charge of the - and -site cations, tolerance factor, and -site chemistry—also impact the pressure response of these layered perovskites. We also show that coupling between the octahedral rotation and strain order parameters plays a key role in determining the overall pressure response. Despite some similarities, we find that these layered perovskites display a distinct pressure response compared to their perovskite analogs. By identifying trends and underlying mechanisms that control octahedral rotations in Ruddlesden-Popper oxides under pressure, this work lays the foundation for tailoring the structure and properties of these materials.
AB - The combination of reduced dimensionality and tunable structural distortions in layered perovskite oxides makes these materials ideal platforms for designing novel properties and functionalities. One example is hybrid improper ferroelectricity in Ruddlesden-Popper oxides, where the combination of a layered crystal structure and rotations of the metal-oxide octahedra break symmetry and induce a polarization. Precisely controlling the octahedral rotation distortions, for example by the application of hydrostatic pressure, provides a pathway to tune and optimize the properties of these materials. We combine group theoretic methods, density functional theory calculations, and Landau theory analysis to investigate how octahedral rotations respond to pressure in the hybrid improper ferroelectrics , and . We find that factors that are known to control the pressure response of perovskites—the formal charge of the - and -site cations, tolerance factor, and -site chemistry—also impact the pressure response of these layered perovskites. We also show that coupling between the octahedral rotation and strain order parameters plays a key role in determining the overall pressure response. Despite some similarities, we find that these layered perovskites display a distinct pressure response compared to their perovskite analogs. By identifying trends and underlying mechanisms that control octahedral rotations in Ruddlesden-Popper oxides under pressure, this work lays the foundation for tailoring the structure and properties of these materials.
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U2 - 10.1103/PhysRevB.104.144105
DO - 10.1103/PhysRevB.104.144105
M3 - Article
AN - SCOPUS:85117072856
SN - 2469-9950
VL - 104
JO - Physical Review B
JF - Physical Review B
IS - 14
M1 - 144105
ER -