Hybrid excitations due to crystal field, spin-orbit coupling, and spin waves in LiFePO4

Yuen Yiu, Manh Duc Le, Rasmus Toft-Peterson, Georg Ehlers, Robert J. McQueeney, David Vaknin

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    9 Scopus citations

    Abstract

    We report on the spin waves and crystal field excitations in single crystal LiFePO4 by inelastic neutron scattering over a wide range of temperatures, below and above the antiferromagnetic transition of this system. In particular, we find extra excitations below TN=50 K that are nearly dispersionless and are most intense around magnetic zone centers. We show that these excitations correspond to transitions between thermally occupied excited states of Fe2+ due to splitting of the S=2 levels that arise from the crystal field and spin-orbit interactions. These excitations are further amplified by the highly distorted nature of the oxygen octahedron surrounding the iron atoms. Above TN, magnetic fluctuations are observed up to at least 720 K, with an additional inelastic excitation around 4 meV, which we attribute to single-ion effects, as its intensity weakens slightly at 720 K compared to 100 K, which is consistent with the calculated cross sections using a single-ion model. Our theoretical analysis, using the MF-RPA model, provides both detailed spectra of the Fe d shell and estimates of the average ordered magnetic moment and TN. By applying the MF-RPA model to a number of existing spin-wave results from other LiMPO4 (M=Mn, Co, and Ni), we are able to obtain reasonable predictions for the moment sizes and transition temperatures.

    Original languageEnglish
    Article number104409
    JournalPhysical Review B
    Volume95
    Issue number10
    DOIs
    StatePublished - Mar 9 2017

    Funding

    We thank Jens Jensen for very detailed and fruitful discussions. Research at Ames Laboratory is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Contract No. DE-AC02-07CH11358. Use of the Spallation Neutron Source at the Oak Ridge National Laboratory is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Scientific Users Facilities Division.

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