Enhanced ordering temperatures in antiferromagnetic manganite superlattices

S. J. May; P. J. Ryan; J. L. Robertson; J. W. Kim; T. S. Santos; E. Karapetrova; J. L. Zarestky; X. Zhai; S. G.E. Te Velthuis; J. N. Eckstein; S. D. Bader; A. Bhattacharya

doi:10.1038/nmat2557

Enhanced ordering temperatures in antiferromagnetic manganite superlattices

S. J. May, P. J. Ryan, J. L. Robertson, J. W. Kim, T. S. Santos, E. Karapetrova, J. L. Zarestky, X. Zhai, S. G.E. Te Velthuis, J. N. Eckstein, S. D. Bader, A. Bhattacharya

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Abstract

The disorder inherent to doping by cation substitution in the complex oxides can have profound effects on collective-ordered states. Here, we demonstrate that cation-site ordering achieved through digital-synthesis techniques can dramatically enhance the antiferromagnetic ordering temperatures of manganite films. Cation-ordered (LaMnO 3) m /(SrMnO 3) 2m superlattices show Néel temperatures (TN) that are the highest of any La 1x Sr x MnO 3 compound, 70 K greater than compositionally equivalent randomly doped La 1/3 Sr 2/3 MnO 3. The antiferromagnetic order is A-type, consisting of in-plane double-exchange-mediated ferromagnetic sheets coupled antiferromagnetically along the out-of-plane direction. Through synchrotron X-ray scattering, we have discovered an in-plane structural modulation that reduces the charge itinerancy and hence the ordering temperature within the ferromagnetic sheets, thereby limiting TN. This modulation is mitigated and driven to long wavelengths by cation ordering, enabling the higher TN values of the superlattices. These results provide insight into how cation-site ordering can enhance cooperative behaviour in oxides through subtle structural phenomena.

Original language	English (US)
Pages (from-to)	892-897
Number of pages	6
Journal	Nature Materials
Volume	8
Issue number	11
DOIs	https://doi.org/10.1038/nmat2557
State	Published - Nov 2009

ASJC Scopus subject areas

Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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10.1038/nmat2557

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title = "Enhanced ordering temperatures in antiferromagnetic manganite superlattices",

abstract = "The disorder inherent to doping by cation substitution in the complex oxides can have profound effects on collective-ordered states. Here, we demonstrate that cation-site ordering achieved through digital-synthesis techniques can dramatically enhance the antiferromagnetic ordering temperatures of manganite films. Cation-ordered (LaMnO 3) m /(SrMnO 3) 2m superlattices show N{\'e}el temperatures (TN) that are the highest of any La 1x Sr x MnO 3 compound, 70 K greater than compositionally equivalent randomly doped La 1/3 Sr 2/3 MnO 3. The antiferromagnetic order is A-type, consisting of in-plane double-exchange-mediated ferromagnetic sheets coupled antiferromagnetically along the out-of-plane direction. Through synchrotron X-ray scattering, we have discovered an in-plane structural modulation that reduces the charge itinerancy and hence the ordering temperature within the ferromagnetic sheets, thereby limiting TN. This modulation is mitigated and driven to long wavelengths by cation ordering, enabling the higher TN values of the superlattices. These results provide insight into how cation-site ordering can enhance cooperative behaviour in oxides through subtle structural phenomena.",

author = "May, {S. J.} and Ryan, {P. J.} and Robertson, {J. L.} and Kim, {J. W.} and Santos, {T. S.} and E. Karapetrova and Zarestky, {J. L.} and X. Zhai and {Te Velthuis}, {S. G.E.} and Eckstein, {J. N.} and Bader, {S. D.} and A. Bhattacharya",

note = "Funding Information: We are grateful to M. Fitzsimmons for discussions. Work at Argonne, including use of the Advanced Photon Source and the Center for Nanoscale Materials, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract No DE-AC02-06CH11357. Work at Oak Ridge National Laboratory{\textquoteright}s High Flux Isotope Reactor was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy.",

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doi = "10.1038/nmat2557",

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AU - May, S. J.

AU - Ryan, P. J.

AU - Robertson, J. L.

AU - Kim, J. W.

AU - Santos, T. S.

AU - Karapetrova, E.

AU - Zarestky, J. L.

AU - Zhai, X.

AU - Te Velthuis, S. G.E.

AU - Eckstein, J. N.

AU - Bader, S. D.

AU - Bhattacharya, A.

N1 - Funding Information: We are grateful to M. Fitzsimmons for discussions. Work at Argonne, including use of the Advanced Photon Source and the Center for Nanoscale Materials, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract No DE-AC02-06CH11357. Work at Oak Ridge National Laboratory’s High Flux Isotope Reactor was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy.

PY - 2009/11

Y1 - 2009/11

N2 - The disorder inherent to doping by cation substitution in the complex oxides can have profound effects on collective-ordered states. Here, we demonstrate that cation-site ordering achieved through digital-synthesis techniques can dramatically enhance the antiferromagnetic ordering temperatures of manganite films. Cation-ordered (LaMnO 3) m /(SrMnO 3) 2m superlattices show Néel temperatures (TN) that are the highest of any La 1x Sr x MnO 3 compound, 70 K greater than compositionally equivalent randomly doped La 1/3 Sr 2/3 MnO 3. The antiferromagnetic order is A-type, consisting of in-plane double-exchange-mediated ferromagnetic sheets coupled antiferromagnetically along the out-of-plane direction. Through synchrotron X-ray scattering, we have discovered an in-plane structural modulation that reduces the charge itinerancy and hence the ordering temperature within the ferromagnetic sheets, thereby limiting TN. This modulation is mitigated and driven to long wavelengths by cation ordering, enabling the higher TN values of the superlattices. These results provide insight into how cation-site ordering can enhance cooperative behaviour in oxides through subtle structural phenomena.

AB - The disorder inherent to doping by cation substitution in the complex oxides can have profound effects on collective-ordered states. Here, we demonstrate that cation-site ordering achieved through digital-synthesis techniques can dramatically enhance the antiferromagnetic ordering temperatures of manganite films. Cation-ordered (LaMnO 3) m /(SrMnO 3) 2m superlattices show Néel temperatures (TN) that are the highest of any La 1x Sr x MnO 3 compound, 70 K greater than compositionally equivalent randomly doped La 1/3 Sr 2/3 MnO 3. The antiferromagnetic order is A-type, consisting of in-plane double-exchange-mediated ferromagnetic sheets coupled antiferromagnetically along the out-of-plane direction. Through synchrotron X-ray scattering, we have discovered an in-plane structural modulation that reduces the charge itinerancy and hence the ordering temperature within the ferromagnetic sheets, thereby limiting TN. This modulation is mitigated and driven to long wavelengths by cation ordering, enabling the higher TN values of the superlattices. These results provide insight into how cation-site ordering can enhance cooperative behaviour in oxides through subtle structural phenomena.

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Enhanced ordering temperatures in antiferromagnetic manganite superlattices

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