Designing Magnetism in High Entropy Oxides

Mazza, Alessandro R.; Skoropata, Elizabeth; Sharma, Yogesh; Lapano, Jason; Heitmann, Thomas W.; Musico, Brianna L.; Keppens, Veerle; Gai, Zheng; Freeland, John W.; Charlton, Timothy R.; Brahlek, Matthew; Moreo, Adriana; Dagotto, Elbio; Ward, Thomas Z.

doi:10.1002/advs.202200391

Title: Designing Magnetism in High Entropy Oxides

Journal Article · 11 February 2022 · Advanced Science

DOI: https://doi.org/10.1002/advs.202200391 · OSTI ID:1845071

Mazza, Alessandro R. ^[1]; Skoropata, Elizabeth ^[1]; Sharma, Yogesh ^[2]; Lapano, Jason ^[1]; Heitmann, Thomas W. ^[3]; Musico, Brianna L. ^[4]; Keppens, Veerle ^[4]; Gai, Zheng ^[5]; Freeland, John W. ^[6]; Charlton, Timothy R. ^[7]; Brahlek, Matthew ^[1]; Moreo, Adriana ^[8]; Dagotto, Elbio ^[8];

^[1]

Materials Science and Technology Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Materials Science and Technology Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA, Center for Integrated Nanotechnologies Los Alamos National Laboratory Los Alamos NM 87545 USA
University of Missouri Research Reactor The University of Missouri Columbia MO 65211 USA
Department of Materials Science and Engineering University of Tennessee Knoxville TN 37996‐4545 USA
Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA
Neutron Science Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA
Materials Science and Technology Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA, Department of Physics and Astronomy University of Tennessee Knoxville TN 37996 USA

Abstract In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder are lacking. Here, it is demonstrated that high entropy oxides present a previously unexplored route to designing materials in which the presence of strong local compositional disorder may be exploited to generate tunable magnetic behaviors—from macroscopically ordered states to frustration‐driven dynamic spin interactions. Single‐crystal La(Cr _0.2 Mn _0.2 Fe _0.2 Co _0.2 Ni _0.2 )O ₃ films are used as a model system hosting a magnetic sublattice with a high degree of microstate disorder in the form of site‐to‐site spin and exchange type inhomogeneity. A classical Heisenberg model simplified to represent the highest probability microstates well describes how compositionally disordered systems can paradoxically host magnetic uniformity and demonstrates a path toward continuous control over ordering types and critical temperatures. Model‐predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition, this leads to highly controllable exchange bias behaviors previously accessible only in intentionally designed bilayer heterojunctions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1845071

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 10 Vol. 9; ISSN 2198-3844

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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36 MATERIALS SCIENCE
disorder
exchange bias
frustration
high entropy oxides
magnetism

Title: Designing Magnetism in High Entropy Oxides

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