Journal article
Cleavable quaternary oxychlorides with high magnetic ordering temperatures
Physical review materials, v 9(3), 034002
Mar 2025
Abstract
Quaternary oxychlorides derived from Ruddlesden–Popper 3𝑑 transition metal oxides offer a route to cleavable crystals with bulk antiferromagnetic ordering temperatures reaching at least 550 K. Here, we study the magnetic, optical, and mechanical behavior of Sr2FeO3Cl, Ca2FeO3Cl, Ca3Fe2O5Cl2, and Sr3Fe2O5Cl2. Through optical absorption measurements, we show that these antiferromagnetic semiconductors have optical band gaps of ≈2.1(1)eV. The magnetic ordering symmetries and temperatures were probed by neutron powder diffraction and Mössbauer spectroscopy on polycrystalline samples, demonstrating Néel temperatures (𝑇N) near room temperature in the single layer Sr2FeO3Cl (𝑇N≈311K) and Ca2FeO3Cl (𝑇N≈360K), and the double-layer compound Sr3Fe2O5Cl2 has 𝑇N≈545K. The high-spin moments of Fe3+ lie within the basal plane and the magnetic structures are compensated within each magnetic layer and characterized by magnetic propagation vectors 𝒌=(
1
2
1
2
0). Magnetization results demonstrate the quasi-2D nature of the magnetism, with a broad maximum in the susceptibility near 2𝑇N for Sr2FeO3Cl. Scotch tape tests and mechanical exfoliation onto SiO2 confirm the micaceous nature of these crystals with cleavage down to a single unit cell (two magnetic layers) achieved for Sr3Fe2O5Cl2. This paper highlights strong antiferromagnetic interactions, semiconducting band gaps, and cleavability of quaternary Fe-based oxychlorides and motivates future work on crystals and exfoliated flakes of these and related oxyhalide systems.
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Details
- Title
- Cleavable quaternary oxychlorides with high magnetic ordering temperatures
- Creators
- Andrew F. May - Oak Ridge National LaboratoryGeorge Yumnam - Oak Ridge National LaboratoryRaphael P. Hermann - Oak Ridge National LaboratoryStuart Calder - Oak Ridge National LaboratoryBenjamin M. Lefler - Drexel UniversitySteven J. May - Drexel UniversityZachary E. Brubaker - Oak Ridge National LaboratoryMatthew Brahlek - Oak Ridge National LaboratoryXiaodong Xu - University of WashingtonDmitry Ovchinnikov - University of WashingtonMichael A. McGuire - Oak Ridge National Laboratory
- Publication Details
- Physical review materials, v 9(3), 034002
- Publisher
- American Physical Society
- Number of pages
- 10
- Grant note
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, EPSCoR, and Materials Sciences and Engineering Division: DE-SC0025319 National Science Foundation: CMMI-2001888
This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. This research used resources at the High Flux Isotope Reactor, a U.S. DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The beam time was allocated to HB-2A (POWDER) on Proposal No. IPTS-29118. Exfoliation efforts (D.O., X.X.) were supported by Air Force Office of Scientific Research (AFOSR) Multidisciplinary University Research Initiative (MURI) program, Grant No. FA9550-19-1-0390. Atomic force microscopy analysis (DO) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, EPSCoR, and Materials Sciences and Engineering Division under Award No. DE-SC0025319. Optical measurements (B.M.L. and S.J.M.) were supported by the National Science Foundation, under Grant No. CMMI-2001888. We are grateful to R. Synowicki for assistance with ellipsometry measurements from the SrFeO2.5 and SrFeO2F films. We thank M. Gibertini for useful discussions regarding the Materials Cloud 2D crystals database. Finally, we thank A. Christianson and J. Yan for useful discussions.
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Materials Science and Engineering
- Web of Science ID
- WOS:001468676900003
- Scopus ID
- 2-s2.0-105001029639
- Other Identifier
- 991022042269504721
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Materials Science, Multidisciplinary