Revisiting the ground state of CoAl2O4 : Comparison to the conventional antiferromagnet MnAl2O4

MacDougall, Gregory J.; Aczel, Adam A.; Su, Yixi; Schweika, Werner; Faulhaber, E.; Schneidewind, A.; Christianson, Andrew D.; Zarestky, Jerel L.; Zhou, H. D.; Mandrus, David; Nagler, Stephen E.

doi:10.1103/PhysRevB.94.184422

Title: Revisiting the ground state of ${CoAl}_{2} O_{4}$ : Comparison to the conventional antiferromagnet ${MnAl}_{2} O_{4}$

Journal Article · Thu Nov 17 00:00:00 EST 2016 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.94.184422· OSTI ID:1335348

MacDougall, Gregory J. ^[1]; Aczel, Adam A. ^[2]; Su, Yixi ^[3]; Schweika, Werner ^[4]; Faulhaber, E. ^[5]; Schneidewind, A. ^[6]; Christianson, Andrew D. ^[2]; Zarestky, Jerel L. ^[7]; Zhou, H. D. ^[8]; Mandrus, David ^[9]; Nagler, Stephen E. ^[10]

Univ. of Illinois, Urbana, IL (United States). Dept. of Physics; Seitz Materials Research Lab.; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
Forschungszentrum Julich GmbH, Garching (Germany). Julich Centre for Neutron Science (JCNS) at Heinz Maier-Leibnitz Zentrum (MLZ)
Forschungszentrum Julich GmbH (Germany). Julich Centre for Neutron Science (JCNS)
Forschungszentrum Julich GmbH, Garching (Germany). Julich Centre for Neutron Science (JCNS) at Heinz Maier-Leibnitz Zentrum (MLZ); Helmholtz-Zentrum Berlin for Materials and Energy, Berlin (Germany)
Helmholtz-Zentrum Berlin for Materials and Energy, Berlin (Germany); Forschungsneutronenquell Heinz Meier-Leibnitz (FRM-II), Garching (Germany)
Ames Lab. and Iowa State Univ., Ames, IA (United States). Division of Materials Science and Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy; National High Magnetic Field Lab., Tallahassee, FL (United States)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division; Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center

The A-site spinel material CoAl₂O₄ is a physical realization of the frustrated diamond-lattice antiferromagnet, a model in which unique incommensurate or “spin-spiral-liquid” ground states are predicted. Our previous single-crystal neutron scattering study instead classified it as a “kinetically inhibited” antiferromagnet, where the long-ranged correlations of a collinear Néel ground state are blocked by the freezing of domain-wall motion below a first-order phase transition at T*=6.5 K. This study provides new data sets from a number of experiments, which support and expand this work in several important ways. We show that the phenomenology leading to the kinetically inhibited order is unaffected by sample measured and instrument resolution, while new low-temperature measurements reveal spin correlations are unchanging between T=2 K and 250 mK, consistent with a frozen state. Polarized diffuse neutron measurements show several interesting magnetic features, which can be entirely explained by the existence of short-ranged Néel order. Finally, and crucially, this paper presents some neutron scattering studies of single crystalline MnAl₂O₄, which acts as an unfrustrated analog to CoAl₂O₄ and shows all the hallmarks of a classical antiferromagnet with a continuous phase transition to Néel order at T_N=39 K. Direct comparison between the two compounds indicates that CoAl₂O₄ is unique, not in the nature of high-temperature diffuse correlations, but rather in the nature of the frozen state below T*. Finally, the higher level of cation inversion in the MnAl₂O₄ sample indicates that this behavior is primarily an effect of greater next-nearest-neighbor exchange.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; DMR-1455264-CAR; NSF-DMR-1157490

OSTI ID:: 1335348

Alternate ID(s):: OSTI ID: 1332590

Journal Information:: Physical Review B, Vol. 94, Issue 18; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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Ferrimagnetism in manganese-rich gallium and aluminium spinels due to mixed valence Mn ²⁺ –Mn ³⁺ states Bekheet, Maged F.; Schlicker, Lukas; Doran, Andrew Dalton Transactions, Vol. 47, Issue 8 https://doi.org/10.1039/c7dt04765g	journal	January 2018
Spectroscopic and magnetic investigations of a spin-frustrated Mn-doped CoAl ₂ O ₄ spinel Pradhan, Suman Kalyan; Dalal, Biswajit; Sarkar, Ankita Physical Chemistry Chemical Physics, Vol. 21, Issue 2 https://doi.org/10.1039/c8cp07140c	journal	January 2019

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Title: Revisiting the ground state of ${CoAl}_{2} O_{4}$ : Comparison to the conventional antiferromagnet ${MnAl}_{2} O_{4}$