Abstract
The emergence of novel magnetic states becomes more likely when the inversion symmetry of the crystal field, relative to the center between two spins, is broken. We propose that placing magnetic spins in inequivalent sites in a polar lattice can promote a realization of nontrivial magnetic states and associated magnetic properties. To test our hypothesis, we study Fe2(SeO3)(H2O)3 as a model system that displays two distinct Fe(1) and Fe(2) magnetic sites in a polar structure (R3c space group). At low fields μ0H ≤ 0.06 T, the material undergoes an antiferromagnetic ordering with TN1 = 77 K and a second transition at TN2 ≈ 4 K. At μ0H ≥ 0.06 T and 74 K ≤ T ≤ 76 K, a positive entropy change of ∼0.12 mJ mol−1 K−1 can be associated with a metamagnetic transition to possibly nontrivial spin states. At zero field, Fe(1) is nearly fully ordered at T ≈ 25 K, while Fe(2) features magnetic frustration down to T = 4 K. The magnetic ground state, a result corroborated by single-crystal neutron diffraction and 57Fe Mössbauer spectroscopy, is a noncollinear antiparallel arrangement of ferrimagnetic Fe(1)-Fe(2) dimers along the c-axis. The results demonstrate that placing distinct magnetic sites in a polar crystal lattice can enable a new pathway to modifying spin, orbital, and lattice degrees of freedom for unconventional magnetism.
| Original language | English |
|---|---|
| Article number | 121115 |
| Journal | APL Materials |
| Volume | 12 |
| Issue number | 12 |
| DOIs | |
| State | Published - Dec 1 2024 |
Funding
This work was supported by the NSF (Award Nos. NSF-DMR-2338014 and NSF-OIA-2227933). X.H. and T.T.T. thank the Arnold and Mabel Beckman Foundation (2023 BYI grant to T.T.T.) for the support. M.M. and H.C. thank the U.S. DOE Office of Science, Office of Basic Energy Sciences, Early Career Research Program Award No. KC0402020, under Contract No. DE-AC05-00OR22725. Research at Gdansk University of Technology was supported by the National Science Center (Poland) under SONATA-15 (Grant No. 2019/35/D/ST5/03769). A portion of this research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The use of the Advanced Photon Source at Argonne National Laboratory was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This manuscript has been authored by UT-Batelle, LLC, under Contract No. 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 ( http://energy.gov/downloads/doe-public-access-plan ). M\u00F6ssbauer measurements were performed by AB using equipment of the M\u00F6ssbauer Spectroscopy Laboratory, Pedagogical University, Krak\u00F3w, Poland.