Abstract
We report a comprehensive investigation of Ln2NiIrO6 (Ln=La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density-functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La2NiIrO6, a collinear ferrimagnetic Ni and Ir state that is driven to long-range antiferromagnetism upon the onset of Nd ordering in Nd2NiIrO6, and a noncollinear ferrimagnetic Ni and Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr2NiIrO6. For Pr2NiIrO6, heat-capacity results reveal the presence of two independent magnetic sublattices, and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. A first principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr2NiIrO6 and offers insight into the behavior in La2NiIrO6 and Nd2NiIrO6. Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t2g manifold of octahedral Ir4+ into a Jeff=12 and Jeff=32 state for all members of the series considered.
| Original language | English |
|---|---|
| Article number | 064408 |
| Journal | Physical Review Materials |
| Volume | 5 |
| Issue number | 6 |
| DOIs | |
| State | Published - Jun 2021 |
Funding
This paper has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the US Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this paper, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan . This research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. This work was partly supported by the US Department of Energy (DOE), Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education for the DOE under Contract No. DE-SC0014664. Research at Oak Ridge National Laboratory (ORNL) was supported by the DOE, Office of Science, Basic Energy Sciences (BES), Materials Science and Engineering Division (sample synthesis and characterization, T.F. and A.S.; first principles calculations, D.P.). Sample synthesis and structural characterization performed at the University of South Carolina were supported by the National Science Foundation under Awards No. DMR-1301757 and No. DMR-1806279. This work used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US DOE Office of Science by Argonne National Laboratory.
| Funders | Funder number |
|---|---|
| Office of Science Graduate Student Research | |
| SCGSR | |
| National Science Foundation | DMR-1806279, DMR-1301757 |
| U.S. Department of Energy | |
| Office of Science | |
| Basic Energy Sciences | |
| Workforce Development for Teachers and Scientists | |
| Oak Ridge National Laboratory | |
| Oak Ridge Institute for Science and Education | DE-SC0014664 |
| Division of Materials Sciences and Engineering |