TY - JOUR
T1 - Magnetic frustration control through tunable stereochemically driven disorder in entropy-stabilized oxides
AU - Meisenheimer, Peter B.
AU - Williams, Logan D.
AU - Sung, Suk Hyun
AU - Gim, Jiseok
AU - Shafer, Padraic
AU - Kotsonis, George N.
AU - Maria, Jon Paul
AU - Trassin, Morgan
AU - Hovden, Robert
AU - Kioupakis, Emmanouil
AU - Heron, John T.
N1 - Funding Information:
This work was supported by IMRA America. This work was supported by National Science Foundation (NSF) CAREER Grant No. DMR-1847847. This work was funded in part by NSF Grant No. DMR-0420785 (XPS) and NSF major research instrumentation Grant No. DMR-1428226 (PPMS). Computational resources were provided by the DOE NERSC facility (DE-AC02-05CH11231) and NSF Grant No. DMR-1810119. This research used resources of the Advanced Light Source, which is a Department of Energy (DOE) Office of Science User Facility under Contract No. DE-AC02-05CH11231. We acknowledge use of the NSF PARADIM facilities (DMR-1539918) at Cornell University. We thank the University of Michigan's Michigan Center for Materials Characterization, ( MC ) 2 , for its assistance with XPS, as well as Professor L. Li and Dr. Z. Xiang for their assistance with PPMS measurements. We thank M. Waters for his assistance with the bond analysis of the DFT calculations. APPENDIX A:
Publisher Copyright:
©2019 American Physical Society.
PY - 2019/10/28
Y1 - 2019/10/28
N2 - Entropy-stabilized oxides possess a large configurational entropy that allows for the unique ability to include typically immiscible concentrations of species in different configurations. Particularly in oxides, where the physical behavior is strongly correlated to stereochemistry and electronic structure, entropic stabilization creates a unique platform to tailor the interplay of extreme structural and chemical disorder to realize unprecedented functionalities. Here, we control stereochemically driven structural disorder in single crystalline, rocksalt, (MgCoNiCuZn)O-type entropy-stabilized oxides through the incorporation of Cu2+ cations. We harness the disorder to tune the degree of glassiness in the antiferromagnetic structure. Structural distortions driven by the Jahn-Teller effect lead to a difference in valence on the Co cation sites, which extends to dilution and disorder of the magnetic lattice. A spin glass model reveals that the fractional spin ordering of the magnetic lattice can be tuned by ∼65%. These findings demonstrate entropy-stabilization as a tool for control of functional phenomena.
AB - Entropy-stabilized oxides possess a large configurational entropy that allows for the unique ability to include typically immiscible concentrations of species in different configurations. Particularly in oxides, where the physical behavior is strongly correlated to stereochemistry and electronic structure, entropic stabilization creates a unique platform to tailor the interplay of extreme structural and chemical disorder to realize unprecedented functionalities. Here, we control stereochemically driven structural disorder in single crystalline, rocksalt, (MgCoNiCuZn)O-type entropy-stabilized oxides through the incorporation of Cu2+ cations. We harness the disorder to tune the degree of glassiness in the antiferromagnetic structure. Structural distortions driven by the Jahn-Teller effect lead to a difference in valence on the Co cation sites, which extends to dilution and disorder of the magnetic lattice. A spin glass model reveals that the fractional spin ordering of the magnetic lattice can be tuned by ∼65%. These findings demonstrate entropy-stabilization as a tool for control of functional phenomena.
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U2 - 10.1103/PhysRevMaterials.3.104420
DO - 10.1103/PhysRevMaterials.3.104420
M3 - Article
AN - SCOPUS:85074436831
VL - 3
JO - Physical Review Materials
JF - Physical Review Materials
SN - 2475-9953
IS - 10
M1 - 104420
ER -