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DOE OSTI · 2569981

Evidence of antiferromagnetism in ultrathin metallic (111)-oriented LaNiO 3 films

Kane, Margaret [Stanford Univ., CA (United States)] (ORCID:0000000332592031)·Balakrishnan, Purnima P. [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:000000021426669X)·Köksal, Okan [Universität Duisburg-Essen (Germany)] (ORCID:0000000339552542)·Holtz, Megan [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000257403359)·Suter, Andreas [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] (ORCID:0000000292146474)·Fitzsimmons, Michael R. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States); Shull Wollan Center, Oak Ridge, TN (United States)]·Yang, Chao-Yao [National Yang Ming Chiao Tung University (Taiwan)] (ORCID:0000000304584624)·Klewe, Christoph [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Quarterman, Paige [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000162726243)·Charlton, Timothy R. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)]·Herzing, Andrew A. [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000159442610)·Salman, Zaher [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] (ORCID:0000000234318135)·Prokscha, Thomas [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] (ORCID:0000000276434695)·Pentcheva, Rossitza [Universität Duisburg-Essen (Germany)] (ORCID:0000000244238980)·Grutter, Alexander J. [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000268767625)·Suzuki, Yuri [Stanford Univ., CA (United States)] (ORCID:0000000268834293)
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Abstract

Antiferromagnets with exotic spin textures promise low-power spintronic devices with extremely high operating frequencies and resistance to external perturbations. In particular, the combination of highly tunable correlated electron physics, as in complex oxides, with metallicity and antiferromagnetism is desirable but exceedingly rare. LaNiO 3 , the lone example of a perovskite nickelate which is metallic across all temperatures, has long been a promising candidate, but the antiferromagnetic metallic state has remained elusive. Here, we demonstrate the emergence of this state in ultrathin films of (111)-oriented LaNiO 3 using a combination of polarized neutron reflectometry, low-energy muon spectroscopy and anomalous Hall effect measurements, and density functional theory calculations with a Hubbard U term. Further, we find a highly strained symmetry-breaking interfacial region which may support canting of the AFM moments leading to a vanishingly small net magnetization at the film-substrate interface, providing a convenient route toward control of the Néel order. Evidence of antiferromagnetic metallic behavior in (111)LNO films highlights the role of crystal symmetry in tuning the novel quantum states in complex oxides.

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36 MATERIALS SCIENCEantiferromagnetismcomplex oxidesepitaxial strainmagnetismmagnetotransportnickelatesperovskitesthin films

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Kane, Margaret [Stanford Univ., CA (United States)] (ORCID:0000000332592031), Balakrishnan, Purnima P. [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:000000021426669X), Köksal, Okan [Universität Duisburg-Essen (Germany)] (ORCID:0000000339552542), Holtz, Megan [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000257403359), Suter, Andreas [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] (ORCID:0000000292146474), Fitzsimmons, Michael R. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States); Shull Wollan Center, Oak Ridge, TN (United States)], Yang, Chao-Yao [National Yang Ming Chiao Tung University (Taiwan)] (ORCID:0000000304584624), Klewe, Christoph [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Quarterman, Paige [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000162726243), Charlton, Timothy R. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)], Herzing, Andrew A. [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000159442610), Salman, Zaher [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] (ORCID:0000000234318135), Prokscha, Thomas [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] (ORCID:0000000276434695), Pentcheva, Rossitza [Universität Duisburg-Essen (Germany)] (ORCID:0000000244238980), Grutter, Alexander J. [National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)] (ORCID:0000000268767625), Suzuki, Yuri [Stanford Univ., CA (United States)] (ORCID:0000000268834293). 2024-12-11. Evidence of antiferromagnetism in ultrathin metallic (111)-oriented LaNiO 3 films. https://doi.org/10.1103/physrevmaterials.8.124406

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The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

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