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New and old materials for permanent magnets based on earth-abundant elements
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Materials Science and Engineering, Solid State Physics. Uppsala university.ORCID iD: 0000-0003-3574-2146
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Electrical motors, which find use in e.g. electrical vehicles, require per-manent magnets to function. Comparing ferrite magnets and Nd-based magnets reveals a large difference in their price and performance. During the last decade, gap-magnets, with performance in between ferrites and Nd-based magnets have attracted considerable research interest world-wide due to the “rare-earth crisis”. During this crisis, the price of certain rare-earth elements experienced volatile changes. This thesis deals with materials that could be relevant as gap-magnets. The thesis starts with introducing key properties and constraints relevant for gap-magnets. In the thesis, four different systems were investigated. The four systems show that permanent magnets need to be understood and optimized on three distinct levels, the crystal level, the structural level, and the micro-structural level. They show how old and new materials can potentially be utilized as permanent magnets. Lastly, the thesis ends with an outlook that presents new ideas for finding new permanent magnets. The ideas presented in the outlook are ideas that were not treated in this thesis, and thus may represent new ways for further work in developing materials for gap-magnets. 

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2022. , p. 83
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 2160
Keywords [en]
permanent magnets, material development, sustainability
National Category
Condensed Matter Physics
Research subject
Engineering Science with specialization in Solid State Physics
Identifiers
URN: urn:nbn:se:uu:diva-473377ISBN: 978-91-513-1525-6 (print)OAI: oai:DiVA.org:uu-473377DiVA, id: diva2:1654204
Public defence
2022-06-14, Polhelmssalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:00 (English)
Opponent
Supervisors
Available from: 2022-05-23 Created: 2022-04-26 Last updated: 2022-06-15
List of papers
1. Magnetic properties of the Fe5SiB2−Fe5PB2 system
Open this publication in new window or tab >>Magnetic properties of the Fe5SiB2−Fe5PB2 system
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2017 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 96, no 9, article id 094433Article in journal (Refereed) Published
Abstract [en]

The magnetic properties of the compound Fe5Si1−xPxB2 have been studied, with a focus on the Curie temperature TC, saturation magnetization MS, and magnetocrystalline anisotropy. Field and temperature dependent magnetization measurements were used to determine TC(x) and MS(x). The saturation magnetization at 10 K (300 K) is found to monotonically decrease from 1.11MA/m (1.03MA/m) to 0.97MA/m (0.87MA/m), as x increases from 0 to 1. The Curie temperature is determined to be 810 and 615 K in Fe5SiB2 and Fe5PB2, respectively. The highest TC is observed for x=0.1, while it decreases monotonically for larger x. The Curie temperatures have also been theoretically determined to be 700 and 660 K for Fe5SiB2 and Fe5PB2, respectively, using a combination of density functional theory and Monte Carlo simulations. The magnitude of the effective magnetocrystalline anisotropy was extracted using the law of approach to saturation, revealing an increase with increasing phosphorus concentration. Low-field magnetization vs temperature results for x=0,0.1,0.2 indicate that there is a transition from easy-axis to easy-plane anisotropy with decreasing temperature.

Place, publisher, year, edition, pages
American Physical Society, 2017
Keywords
Magnetism, Ferromagnetism, First-principle calculations, Magnetic interactions, Magnetic order parameter, Magnetic phase transition
National Category
Condensed Matter Physics Engineering and Technology
Research subject
Physics
Identifiers
urn:nbn:se:uu:diva-330463 (URN)10.1103/PhysRevB.96.094433 (DOI)000411975700001 ()
Funder
Swedish Research CouncilGöran Gustafsson Foundation for Research in Natural Sciences and MedicineKnut and Alice Wallenberg Foundation, 2013.0020, 2012.0031EU, Horizon 2020
Available from: 2017-09-29 Created: 2017-09-29 Last updated: 2022-05-24Bibliographically approved
2. Magnetocrystalline anisotropy of Fe5PB2 and its alloys with Co and 5d elements: A combined first-principles and experimental study
Open this publication in new window or tab >>Magnetocrystalline anisotropy of Fe5PB2 and its alloys with Co and 5d elements: A combined first-principles and experimental study
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2018 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 98, no 21, article id 214431Article in journal (Refereed) Published
Abstract [en]

The Fe5PB2 compound offers tunable magnetic properties via the possibility of various combinations of substitutions on the Fe and P sites. Here, we present a combined computational and experimental study of the magnetic properties of (Fe1-xCox)(5)PB2. Computationally, we are able to explore the full concentration range, while the real samples were only obtained for 0 <= x <= 0.7. The calculated magnetic moments, Curie temperatures, and magnetocrystalline anisotropy energies (MAEs) are found to decrease with increasing Co concentration. Co substitution allows for tuning the Curie temperature in a wide range of values, from about six hundred to zero kelvins. As the MAE depends on the electronic structure in the vicinity of the Fermi energy, the geometry of the Fermi surface of Fe5PB2 and the k-resolved contributions to the MAE are discussed. Low-temperature measurements of an effective anisotropy constant for a series of (Fe1-xCox)(5)PB2 samples determined the highest value of 0.94 MJ m(-3) for the terminal Fe5PB2 composition, which then decreases with increasing Co concentration, thus confirming the computational result that Co alloying of Fe5PB2 is not a good strategy to increase the MAE of the system. However, the relativistic version of the fixed spin moment method reveals that a reduction in the magnetic moment of Fe5PB2, by about 25%, produces a fourfold increase of the MAE. Furthermore, calculations for (Fe0.95X0.05)(5)PB2 (X = 5d element) indicate that 5% doping of Fe5PB2 with W or Re should double the MAE. These are results of high interest for, e.g., permanent magnet applications, where a large MAE is crucial.

National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-373233 (URN)10.1103/PhysRevB.98.214431 (DOI)000454163400003 ()
Funder
Swedish Research CouncilSwedish Foundation for Strategic Research
Available from: 2019-01-14 Created: 2019-01-14 Last updated: 2022-04-26Bibliographically approved
3. Influence of cobalt substitution on the magnetic properties of Fe5PB2
Open this publication in new window or tab >>Influence of cobalt substitution on the magnetic properties of Fe5PB2
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2018 (English)In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 57, no 2, p. 777-784Article in journal (Refereed) Published
Abstract [en]

In this study the effects of cobalt substitutions in Fe5PB2 have been studied. An increased cobalt content reduces the magnetic exchange interactions. This has been concluded from a large, linear decrease in both the Curie temperature as well as the saturated magnetic moment. At high cobalt concentrations, cobalt prefers to order at the M(2) position in the crystal structure. A tunable Curie transition like this shows some prerequisites for magnetic cooling applications.

The substitutional effects of cobalt in (Fe1–xCox)5PB2 have been studied with respect to crystalline structure and chemical order with X-ray diffraction and Mössbauer spectroscopy. The magnetic properties have been determined from magnetic measurements, and density functional theory calculations have been performed for the magnetic properties of both the end compounds, as well as the chemically disordered intermediate compounds. The crystal structure of (Fe1–xCox)5PB2 is tetragonal (space group I4/mcm) with two different metal sites, with a preference for cobalt atoms in the M(2) position (4c) at higher cobalt contents. The substitution also affects the magnetic properties with a decrease of the Curie temperature (TC) with increasing cobalt content, from 622 to 152 K for Fe5PB2 and (Fe0.3Co0.7)5PB2, respectively. Thus, the Curie temperature is dependent on composition, and it is possible to tune TC to a temperature near room temperature, which is one prerequisite for magnetic cooling materials.

National Category
Inorganic Chemistry Condensed Matter Physics Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-331758 (URN)10.1021/acs.inorgchem.7b02663 (DOI)000422810900030 ()29298054 (PubMedID)
Funder
Swedish Research CouncilSwedish Energy AgencyEuropean Regional Development Fund (ERDF)
Available from: 2017-10-19 Created: 2017-10-19 Last updated: 2023-10-31Bibliographically approved
4. Magnetic and Structural Properties of the Fe5Si1-xGexB2 System
Open this publication in new window or tab >>Magnetic and Structural Properties of the Fe5Si1-xGexB2 System
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2022 (English)In: Journal of Solid State Chemistry, ISSN 0022-4596, E-ISSN 1095-726X, Vol. 316, article id 123576Article in journal (Refereed) Published
Abstract [en]

A series of compounds with compositions Fe5Si1-xGexB2 were synthesised and their structural and magnetic properties were investigated. The Mo5SiB2-type structure with tetragonal I4/mcm space group is maintained for all compounds with x < 0.15, which is estimated as the compositional limit of the system. The unit cell pa-rameters expand with Ge content before reaching a plateau of a = 5.5581(1) and c = 10.3545(1) angstrom at x = 0.15. The saturation magnetisation (MS) decreased slightly with increasing Ge content whilst the magnetocrystalline anisotropy energy (MAE) remains almost unaffected. The Curie temperature for all compounds studied is at 790 K whilst the spin-reorientation temperature shows suppression from 172 K to 101 K where x = 0.15. Ab Initio calculations reveal an increase in MAE for compositions up to x = 0.25 and a decreased magnitude of MAE of-0.14 MJ/m3 for the hypothetical compound Fe5GeB2 relative to the parent compound Fe5SiB2.

National Category
Condensed Matter Physics
Research subject
Engineering Science with specialization in Solid State Physics
Identifiers
urn:nbn:se:uu:diva-473290 (URN)10.1016/j.jssc.2022.123576 (DOI)000863761000008 ()
Funder
Swedish Foundation for Strategic Research, EM-16-0039Swedish Research Council, 2019-00207
Available from: 2022-04-25 Created: 2022-04-25 Last updated: 2022-10-28Bibliographically approved
5. Structural, microstructural and magnetic evolution in cryo milled carbon doped MnAl
Open this publication in new window or tab >>Structural, microstructural and magnetic evolution in cryo milled carbon doped MnAl
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2018 (English)In: Scientific Reports, E-ISSN 2045-2322, Vol. 8, no 1, article id 2525Article in journal (Refereed) Published
Abstract [en]

The low cost, rare earth free τ-phase of MnAl has high potential to partially replace bonded Nd2Fe14B rare earth permanent magnets. However, the τ-phase is metastable and it is experimentally difficult to obtain powders suitable for the permanent magnet alignment process, which requires the fine powders to have an appropriate microstructure and high τ-phase purity. In this work, a new method to make high purity τ-phase fne powders is presented. A high purity τ-phase Mn0.55Al0.45C0.02 alloy was synthesized by the drop synthesis method. The drop synthesized material was subjected to cryo milling and followed by a fash heating process. The crystal structure and microstructure of the drop synthesized, cryo milled and flash heated samples were studied by X-ray in situ powder diffraction, scanning electron microscopy, X-ray energy dispersive spectroscopy and electron backscatter diffraction. Magnetic properties and magnetic structure of the drop synthesized, cryo milled, flash heated samples were characterized by magnetometry and neutron powder diffraction, respectively. The results reveal that the 2 and 4hours cryo milled and flash heated samples both exhibit high τ-phase purity and micron-sized round particle shapes. Moreover, the fash heated samples display high saturation magnetization as well as increased coercivity.

National Category
Materials Chemistry Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-341024 (URN)10.1038/s41598-018-20606-8 (DOI)000424189500012 ()29410462 (PubMedID)
Funder
Swedish Energy AgencySweGRIDS - Swedish Centre for Smart Grids and Energy StorageSwedish Research Council
Available from: 2018-02-06 Created: 2018-02-06 Last updated: 2022-09-15Bibliographically approved
6. One step towards MnAl-based permanent magnets: Differences in magnetic, and microstructural properties from an intermediate annealing step during synthesis
Open this publication in new window or tab >>One step towards MnAl-based permanent magnets: Differences in magnetic, and microstructural properties from an intermediate annealing step during synthesis
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2019 (English)In: Journal of Solid State Chemistry, ISSN 0022-4596, E-ISSN 1095-726X, Vol. 274, p. 229-236Article in journal (Refereed) Published
Abstract [en]

The influence of an additional annealing step during synthesis on the preparation of MnAl based permanent magnet alloys has been investigated. Bulk samples of Mn55Al45C2 alloys were synthesized using induction heating through drop synthesis from 1400 °C. Samples produced using cooling directly from 1400 °C (from the melt), and from 1400 °C to an intermediate annealing step at 1200 °C for ~ 30 min before cooling were compared with respect to differences in phase purity, microstructure and magnetic properties. We found that the phase purity was significantly enhanced using the route with an intermediate annealing step at 1200 °C. From XRD the phase purity of the tau-phase was improved from ~ 91 wt% for the sample cooled directly from 1400 °C to ~ 95.1 - 99.5 wt% for the sample exposed to an intermediate annealing step before cooling. Additionally, EBSD, and SEM with EDS indicates a clear difference in the phase composition and differences in the distribution of the magnetic tau phase and the non-magnetic epsilon-, beta-, and gamma-phases. Magnetic properties also indicate, an improvement in saturation magnetization for the sample exposed to the extra annealing step during synthesis. Our results suggest that an intermediate annealing step in the production of MnAl based alloys will provide a simple way of achieving better phase purity and magnetic properties in the bulk alloy.

Keywords
permanent magnet, rare earth free, microstructure
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-368283 (URN)10.1016/j.jssc.2019.03.035 (DOI)000467663700032 ()
Funder
SweGRIDS - Swedish Centre for Smart Grids and Energy StorageSwedish Foundation for Strategic Research
Available from: 2018-12-03 Created: 2018-12-03 Last updated: 2023-10-31Bibliographically approved
7. Influence of nano-VC on the structural and magnetic properties of MnAlC-alloy
Open this publication in new window or tab >>Influence of nano-VC on the structural and magnetic properties of MnAlC-alloy
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2021 (English)In: Scientific Reports, E-ISSN 2045-2322, Vol. 11, article id 14453Article in journal (Refereed) Published
Abstract [en]

Alloys of Mn55Al45C2 with additions of VC nano-particles have been synthesized and their properties evaluated. The Mn55Al45C2(VC)(x) (x=0.25, 0.5 and 1) alloys have been prepared by induction melting resulting in a high content of the ferromagnetic tau -phase (>94 wt.%). Powder X-ray diffraction indicates that nano-VC can be dissolved in the alloy matrix up to 1 at.%. On the other side, metallography investigations by scanning electron microscopy and scanning transmission electron microscope show inclusions of the nanosized additives in the microstructure. The effect of nano-VC on the grain and twin boundaries has been studied by electron backscattering diffraction. The magnetization has been measured by magnetometry up to 9 T while the domain structure has been studied using both magnetic force microscopy as well as Kerr-microscopy. For nano-VC contents above 0.25 at.%, a clear increase of the coercive force is observed, from 57 to 71 kA/m. The optimum appears to be for 0.5 at.% nano-VC which shows a 25% increase in coercive force without losing any saturation magnetization. This independent increase in coercivity is believed to originate from the nano-VC reducing the overall magnetic domain size. Overall, we observe that addition of nano-VC could be an interesting route to increase the coercive force of MnAl, without sacrificing saturation magnetization.

Place, publisher, year, edition, pages
Springer NatureNATURE RESEARCH, 2021
National Category
Condensed Matter Physics Metallurgy and Metallic Materials
Identifiers
urn:nbn:se:uu:diva-452947 (URN)10.1038/s41598-021-93395-2 (DOI)000675633500020 ()34262064 (PubMedID)
Available from: 2021-09-13 Created: 2021-09-13 Last updated: 2024-01-15Bibliographically approved
8. Structural and magnetic properties of new members of the 3:29 phase from the Ce-Fe-Mn system and 1:11 from the Ce-Co-Mn
Open this publication in new window or tab >>Structural and magnetic properties of new members of the 3:29 phase from the Ce-Fe-Mn system and 1:11 from the Ce-Co-Mn
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2021 (English)In: Journal of Alloys and Compounds, ISSN 0925-8388, E-ISSN 1873-4669, Vol. 855, article id 157435Article in journal (Refereed) Published
Abstract [en]

The Ce–Fe–Mn and Ce–Co–Mn systems have been re-visited with the intent of finding new potential phases for application as permanent magnets. Two new ternary compounds, Ce3(Fe0.638Mn0.362)29 (Nd3(Fe,Ti)29-type, space group P21/c, No. 14, Pearson Symbol mP128) and CeCo8Mn3 (Ce(Ni,Mn)11-type, space group P4/mbm, No. 127, Pearson Symbol tP24) have been discovered in the compositional range where the Ce2(T,Mn)17 (T = Fe, Co) phases are expected to exist with a (H)–Th2Ni17-type structure (space group P63/mmc, No. 194, Pearson Symbol hP38). Detailed investigations of the crystal structures have been performed using X-ray powder diffraction (XRPD) with supporting energy-dispersive X-ray (EDS) analysis. Compositions of the new compounds have been defined based on the EDS analysis as follows: Ce9.7Fe57.5Mn32.8 and Ce9.2Co65.2Mn25.6. A short discussion on the crystal structure peculiarities of the 1:5, 1:11, 1:12, 2:17 and 3:29 compounds in the Ce–T–Mn (T = Fe, Co, Ni, Cu) systems has been made. We present magnetic measurements on selected representatives of the studied phases. The most interesting being the Ce3(Fe0.638Mn0.362)29 phase which has a transition temperature well above room temperature. CeNi4.95Mn6.05 and CeCo8Mn3 exhibits properties characteristic of a canted antiferromagnetic state.

Place, publisher, year, edition, pages
Elsevier, 2021
Keywords
Intermetallic compounds, Crystal structure, Magnetic properties
National Category
Materials Chemistry Metallurgy and Metallic Materials
Identifiers
urn:nbn:se:uu:diva-432623 (URN)10.1016/j.jallcom.2020.157435 (DOI)000601001500058 ()
Funder
Swedish Foundation for Strategic Research , EM16-0039Swedish Energy AgencySweGRIDS - Swedish Centre for Smart Grids and Energy Storage
Available from: 2021-01-25 Created: 2021-01-25 Last updated: 2024-01-15Bibliographically approved
9. Hard magnetic phases of CeFe11W1-xTix
Open this publication in new window or tab >>Hard magnetic phases of CeFe11W1-xTix
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(English)Manuscript (preprint) (Other academic)
National Category
Condensed Matter Physics
Research subject
Engineering Science with specialization in Solid State Physics
Identifiers
urn:nbn:se:uu:diva-473289 (URN)
Available from: 2022-04-25 Created: 2022-04-25 Last updated: 2022-04-26
10. Magnetic Structure and Properties of CeFe12-xMnx
Open this publication in new window or tab >>Magnetic Structure and Properties of CeFe12-xMnx
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(English)Manuscript (preprint) (Other academic)
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-473375 (URN)
Available from: 2022-04-26 Created: 2022-04-26 Last updated: 2022-04-26
11. Data-driven design of a new class of rare-earth free permanent magnets
Open this publication in new window or tab >>Data-driven design of a new class of rare-earth free permanent magnets
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2021 (English)In: Acta Materialia, ISSN 1359-6454, E-ISSN 1873-2453, Vol. 212, article id 116913Article in journal (Refereed) Published
Abstract [en]

A new class of rare-earth-free permanent magnets is proposed. The parent compound of this class is Co3Mn2Ge, and its discovery is the result of first principles theory combined with experimental synthesis and characterisation. The theory is based on a high-throughput/data-mining search among materials listed in the ICSD database. From ab-initio theory of the defect free material it is predicted that the saturation magnetization is 1.71 T, the uniaxial magnetocrystalline anisotropy is 1.44 MJ/m3, and the Curie temperature is 700 K. Co3Mn2Ge samples were then synthesized and characterised with respect to structure and magnetism. The crystal structure was found to be the MgZn2-type, with partial disorder of Co and Ge on the crystallographic lattice sites. From magnetization measurements a saturation polarization of 0.86 T at 10 K was detected, together with a uniaxial magnetocrystalline anisotropy constant of 1.18 MJ/m3, and the Curie temperature of TC = 359 K. These magnetic properties make Co3Mn2Ge a very promising material as a rare-earth free permanent magnet, and since we can demonstrate that magnetism depends critically on the amount of disorder of the Co and Ge atoms, a further improvement of the magnetism is possible. We demonstrate here that the class of compounds based on T3Mn2X (T = Co or alloys between Fe and Ni; X = Ge, Al or Ga) in the MgZn2 structure type, form a new class of rare-earth free permanent magnets with very promising performance.

Place, publisher, year, edition, pages
Elsevier, 2021
Keywords
Permanent magnets, Rare-earth, Synthesis, DFT, Magnetism
National Category
Condensed Matter Physics Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-448912 (URN)10.1016/j.actamat.2021.116913 (DOI)000663657100005 ()
Funder
VinnovaSwedish Foundation for Strategic Research SweGRIDS - Swedish Centre for Smart Grids and Energy StorageSwedish Energy AgencySwedish Research CouncilKnut and Alice Wallenberg FoundationStandUpSwedish National Infrastructure for Computing (SNIC)
Available from: 2021-07-12 Created: 2021-07-12 Last updated: 2024-01-15Bibliographically approved
12. Influence of Mn/Co ratio on the magnetic properties of the hexagonal Mn(Co,Ge)2 phase
Open this publication in new window or tab >>Influence of Mn/Co ratio on the magnetic properties of the hexagonal Mn(Co,Ge)2 phase
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(English)Manuscript (preprint) (Other academic)
National Category
Condensed Matter Physics
Research subject
Engineering Science with specialization in Solid State Physics
Identifiers
urn:nbn:se:uu:diva-473291 (URN)
Available from: 2022-04-25 Created: 2022-04-25 Last updated: 2022-10-06
13. Revealing the Magnetic Structure and Properties of Mn(Co,Ge)2
Open this publication in new window or tab >>Revealing the Magnetic Structure and Properties of Mn(Co,Ge)2
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2022 (English)In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 61, no 44, p. 17673-17681Article in journal (Refereed) Published
Abstract [en]

The atomic and magnetic structures of Mn(Co,Ge)2 are reported herein. The system crystallizes in the space group P63/mmc as a superstructure of the MgZn2-type structure. The system exhibits two magnetic transitions with associated magnetic structures, a ferromagnetic (FM) structure around room temperature, and an incommensurate structure at lower temperatures. The FM structure, occurring between 193 and 329 K, is found to be a member of the magnetic space group P63/mmc′. The incommensurate structure found below 193 K is helical with propagation vector k = (0 0 0.0483). Crystallographic results are corroborated by magnetic measurements and ab initio calculations.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2022
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-473292 (URN)10.1021/acs.inorgchem.2c02758 (DOI)000877353500001 ()36270053 (PubMedID)
Funder
Swedish Foundation for Strategic Research, EM-16-0039eSSENCE - An eScience CollaborationSwedish National Infrastructure for Computing (SNIC), snic2021-1-36Swedish National Infrastructure for Computing (SNIC), snic2021-5-340Swedish Research Council, 2019-00645Knut and Alice Wallenberg Foundation
Available from: 2022-04-25 Created: 2022-04-25 Last updated: 2023-02-22Bibliographically approved

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