Synthesis and Characterization of Metastable Cobalt Honeycomb KCoAsO4

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Abstract

The Kitaev model has served as a long-sought-after target in the realization of a quantum spin liquid that could host Majorana Fermions. Such non-Abelian anyons could revolutionize quantum computing if properly implemented to overcome decoherence. A 3d7 electronic configuration, like Co2+, has been explored by theory and experimental work to design Kitaev materials. Here, we report the synthesis of a new cobaltate honeycomb material KCoAsO4. The compound is synthesized through a low-temperature solution route and crystallized in space group R¯3 with lattice parameters a = 5.0394(1) and c = 28.6790(1) as determined by neutron powder diffraction. The crystal structure follows motifs similar to those of the honeycomb compound BaCo2(AsO4)2 but presents differing magnetic behavior. Magnetization/heat capacity measurements on the powder show antiferromagnetic transition TN = 14 K. Two lower-temperature transitions are present in susceptibility at low field that resemble spin reorientations. Magnetization data as a function of field have curvature indicative of metamagnetic behavior below the magnetic ordering temperature, with the magnetic ordering suppressed upon application of a higher magnetic field. Computational studies suggest the presence of a weak nearest-neighbor Kitaev term, K1, consistent with related honeycomb cobaltates. Together, the data suggest that this material should present a new platform for developing Kitaev quantum spin liquids.

Original languageEnglish
Pages (from-to)13696-13704
Number of pages9
JournalInorganic Chemistry
Volume64
Issue number27
DOIs
StatePublished - Jul 14 2025

Funding

This research was primarily supported by the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers, Quantum Science Center. A portion of this research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory. The beamtime on HB-2A was allocated on proposal IPTS-30277. The electron microscopy data collection was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. Initial investigations on KCoAsO4 were conducted by J.F. and sponsored by the Laboratory Directed Research and Development Program (LDRD) of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. Notice: This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (https://www.energy.gov/doe-public-access-plan). This research was primarily supported by the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers, Quantum Science Center. A portion of this research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory. The beamtime on HB-2A was allocated on proposal IPTS-30277. The electron microscopy data collection was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. Initial investigations on KCoAsO were conducted by J.F. and sponsored by the Laboratory Directed Research and Development Program (LDRD) of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. Notice: This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( https://www.energy.gov/doe-public-access-plan ). 4

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