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Miniotaite, U. (2025). Probing Magnetism in Complex Transition Metal Oxides: Insights into Magnetic and Structural Behaviour. (Licentiate dissertation). Stockholm: KTH Royal Institute of Technology
Open this publication in new window or tab >>Probing Magnetism in Complex Transition Metal Oxides: Insights into Magnetic and Structural Behaviour
2025 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Transition metal oxides (TMOs) exhibit a wide range of electronic and magnetic properties, making them essential in condensed matter physics. In magnetic TMOs, the ability to tune the magnetic properties offers valuable insights into correlated electron systems and potential functionalities in next-generation materials.

This Licentiate thesis investigates how antiferromagnetic (AFM) ordering can be tuned in powder AReO4 (A = Mg, Zn), and LiFePO4 using large-scale facility techniques. We explore how the application of hydrostatic pressure or the substitution of the non-magnetic ion affects the magnetic structure and ordering temperatures.

The work utilises muon spin spectroscopy and resonance ($\mu^+$SR) and neutron powder diffraction (NPD) to probe the magnetic properties of these materials. For LiFePO4, high-pressure μ+SR experiments reveal that compressive strain enhances AFM ordering, contrary to theoretical predictions. For AReO4, NPD and μ+SR suggest two possible AFM spin structures. Our measurements show a remarkably low ordered magnetic moment for both MgReO4 and ZnReO4. Bond valence sum (BVS) analysis supports a Re6+ oxidation state in both compounds, and we attribute the low magnetic moment to strong spin-orbit coupling (SOC).

This thesis demonstrates how NPD and μ+SR serve as complementary techniques for investigating complex magnetic systems and how a local probe, the muon, sensing only its immediate environment, can provide insight into macroscopic magnetic properties. The findings contribute to a deeper understanding of the magnetic phase of LiFePO4 and Re6+ magnetism in octahedral coordination with oxygen.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2025. p. 41
Series
TRITA-SCI-FOU ; 202518
Keywords
Antiferromagnetic, Transition Metal Oxides, Muon Spin Spectroscopy, Neutron Diffraction, X-ray Diffraction, Spin Orbit Coupling, LiFePO4, ZnReO4, MgReO4, Rhenium Oxides, Antiferromagnetism, övergångsmetalloxid, myon spin spektroskopi, neutrondiffraktion, röntgendiffraktion, spin-ban-koppling, LiFePO4, ZnReO4, MgReO4, rheniumoxider
National Category
Condensed Matter Physics
Research subject
Physics, Material and Nano Physics
Identifiers
urn:nbn:se:kth:diva-361710 (URN)978-91-8106-249-6 (ISBN)
Presentation
2025-04-23, 4204, Hannes Alfvéns väg 12, Stockholm, 09:25 (English)
Opponent
Supervisors
Funder
Swedish Research Council
Available from: 2025-04-04 Created: 2025-03-27 Last updated: 2025-04-04Bibliographically approved
Umegaki, I., Moriyama, K., Yoshinaga, K., Ohishi, K., Elson, F., Miniotaite, U., . . . Sugiyama, J. (2024). Magnetic phase diagram of Eu 1- x Ca x Co 2 P 2 determined using muon spin rotation and relaxation. Physical Review B, 109(14), Article ID 144408.
Open this publication in new window or tab >>Magnetic phase diagram of Eu 1- x Ca x Co 2 P 2 determined using muon spin rotation and relaxation
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2024 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 109, no 14, article id 144408Article in journal (Refereed) Published
Abstract [en]

The present study investigated the magnetic nature of a solid solution system consisting of EuCo2P2 and CaCo2P2 using a muon spin rotation and relaxation (mu +SR) technique, which is sensitive to local magnetic environments. The former compound EuCo2P2 is known to enter an incommensurate helical antiferromagnetic (AF) phase below 66 K with neutrons, which was confirmed by the present mu +SR. The magnitude of the ordered Eu moments proposed with neutrons was found to be consistent with that estimated by mu +SR. Furthermore, the latter lattice-collapsed tetragonal phase compound CaCo2P2 is known to enter an A-type AF phase below 90 K, and mu +SR measurements on single crystals revealed the presence of a spin reorientation transition at around 40 K, below which the A-type AF order is likely to be completed. Although all Eu1-xCaxCo2P2 compounds were found to enter a magnetic phase at low temperatures regardless of x, a static ordered state was formed only at the vicinity of the two end compounds, i.e., 0 x 0.4 and 0.9 x 1. Instead, a disordered state, i.e., a random spin-glass state, short-range ordered state, or highly fluctuating state was found in the x range between 0.4 and 0.9, even at the lowest measured temperature (2 K). Together with the magnetization data, our findings clarified the magnetic phase diagram of Eu1-xCaxCo2P2, where a ferromagnetic exchange interaction between Co ions through the Eu2+ ion competes with a direct AF interaction among the Co ions, particularly in the x range between 0.57 and 0.9. This competition yielded multiple phases in Eu1-xCaxCo2P2.

Place, publisher, year, edition, pages
American Physical Society (APS), 2024
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-348107 (URN)10.1103/PhysRevB.109.144408 (DOI)001235369800002 ()2-s2.0-85190343911 (Scopus ID)
Note

QC 20240619

Available from: 2024-06-19 Created: 2024-06-19 Last updated: 2024-08-02Bibliographically approved
Galeski, S., Miniotaite, U., Elson, F., Månsson, M., Gooth, J. & et al., . (2024). Quantum oscillation signatures of the Bloch-Grüneisen temperature in the Dirac semimetal ZrTe5. Physical Review B, 110(12), Article ID L121103.
Open this publication in new window or tab >>Quantum oscillation signatures of the Bloch-Grüneisen temperature in the Dirac semimetal ZrTe5
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2024 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 110, no 12, article id L121103Article in journal (Refereed) Published
Abstract [en]

The electron-phonon interaction is in many ways a solid state equivalent of quantum electrodynamics. Being always present, the e-p coupling is responsible for the intrinsic resistance of metals at finite temperatures, making it one of the most fundamental interactions present in solids. In typical metals, different regimes of e-p scattering are separated by a characteristic phonon energy scale - the Debye temperature. However, in metals harboring very small Fermi surfaces a new scale emerges - the Bloch-Grüneisen temperature. This is a temperature at which the average phonon momentum becomes comparable to the Fermi momentum of the electrons. Here we report sub-Kelvin transport and sound propagation experiments on the Dirac semimetal ZrTe5. The combination of the simple band structure with only a single small Fermi surface sheet allowed us to directly observe the Bloch-Grüneisen temperature and its consequences on electronic transport of a 3D metal in the limit where the small size of the Fermi surface leads to effective restoration of translational invariance of free space. Our results indicate that on entering this hydrodynamic transport regime, the viscosity of the Dirac electronic liquid undergoes an anomalous increase beyond the theoretically predicted T5 temperature dependence. Extension of our measurements to strong magnetic fields reveal that, despite the dimensional reduction of the electronic band structure, the electronic liquid retains characteristics of the zero-field hydrodynamic regime up to the quantum limit. This is vividly reflected by an anomalous suppression of the amplitude of quantum oscillations seen in the Shubnikov-de Haas effect.

Place, publisher, year, edition, pages
American Physical Society (APS), 2024
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-353925 (URN)10.1103/PhysRevB.110.L121103 (DOI)001364270000008 ()2-s2.0-85203855259 (Scopus ID)
Note

QC 20250120

Available from: 2024-09-25 Created: 2024-09-25 Last updated: 2025-01-20Bibliographically approved
Nocerino, E., Forslund, O. K., Wang, C., Sakurai, H., Elson, F., Palm, R., . . . Månsson, M. (2023). Magnetic nature of wolframite MgReO4. In: Prando, G Pratt, F (Ed.), 15th International Conference on Muon Spin Rotation, Relaxation and Resonance, MuSR 2022: . Paper presented at 15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR), AUG 28-SEP 02, 2022, Univ Parma, Parma, ITALY. IOP Publishing, 2462, Article ID 012037.
Open this publication in new window or tab >>Magnetic nature of wolframite MgReO4
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2023 (English)In: 15th International Conference on Muon Spin Rotation, Relaxation and Resonance, MuSR 2022 / [ed] Prando, G Pratt, F, IOP Publishing , 2023, Vol. 2462, article id 012037Conference paper, Published paper (Refereed)
Abstract [en]

Rhenium oxides belonging to the family AReO4 where A is a metal cation, exhibit interesting electronic and magnetic properties. In this study we have utilized the muon spin rotation/relaxation (mu+SR) technique to study the magnetic properties of the MgReO4 compound. To the best of our knowledge, this is the first investigation reported on this interesting material, that is stabilized in a wolframite crystal structure using a special highpressure synthesis technique. Bulk magnetic studies show the onset of an antiferromagnetic (AF) long range order, or a possible singlet spin state at T-C1 approximate to 90 K, with a subtle second hightemperature transition at T-C2 approximate to 280 K. Both transitions are also confirmed by heat capacity (Cp) measurements. From our mu+SR measurements, it is clear that the sample enters an AF order below T-C1 = T-N approximate to 85 K. We find no evidence of magnetic signal above TN, which indicates that T-C2 is likely linked to a structural transition. Further, via sensitive zero field (ZF) mu(+) SR measurements we find evidence of a spin reorientation at T-Cant approximate to 65 K. This points towards a transition from a collinear AF into a canted AF order at low temperature, which is proposed to be driven by competing magnetic interactions.

Place, publisher, year, edition, pages
IOP Publishing, 2023
Series
Journal of Physics Conference Series, ISSN 1742-6588
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-329458 (URN)10.1088/1742-6596/2462/1/012037 (DOI)000995428200037 ()2-s2.0-85152622076 (Scopus ID)
Conference
15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR), AUG 28-SEP 02, 2022, Univ Parma, Parma, ITALY
Note

QC 20230621

Available from: 2023-06-21 Created: 2023-06-21 Last updated: 2023-12-07Bibliographically approved
Miniotaite, U., Forslund, O. K., Nocerino, E., Elson, F., Palm, R., Matsubara, N., . . . Månsson, M. (2023). Magnetic Properties of Multifunctional (LiFePO4)-Li-7 under Hydrostatic Pressure. In: Prando, G Pratt, F (Ed.), Proceedings 15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR): . Paper presented at 15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR), AUG 28-SEP 02, 2022, Univ Parma, Parma, ITALY. IOP Publishing, 2462, Article ID 012049.
Open this publication in new window or tab >>Magnetic Properties of Multifunctional (LiFePO4)-Li-7 under Hydrostatic Pressure
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2023 (English)In: Proceedings 15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR) / [ed] Prando, G Pratt, F, IOP Publishing , 2023, Vol. 2462, article id 012049Conference paper, Published paper (Refereed)
Abstract [en]

LiFePO4 (LFPO) is an archetypical and well-known cathode material for rechargeable Li-ion batteries. However, its quasi-one-dimensional (Q1D) structure along with the Fe ions, LFPO also displays interesting low-temperature magnetic properties. Our team has previously utilized the muon spin rotation (mu+SR) technique to investigate both magnetic spin order as well as Li-ion diffusion in LFPO. In this initial study we extend our investigation and make use of high-pressure mu+SR to investigate effects on the low-T magnetic order. Contrary to theoretical predictions we find that the magnetic ordering temperature as well as the ordered magnetic moment increase at high pressure (compressive strain).

Place, publisher, year, edition, pages
IOP Publishing, 2023
Series
Journal of Physics Conference Series, ISSN 1742-6588
National Category
Other Materials Engineering
Identifiers
urn:nbn:se:kth:diva-329856 (URN)10.1088/1742-6596/2462/1/012049 (DOI)000995428200049 ()2-s2.0-85152635129 (Scopus ID)
Conference
15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR), AUG 28-SEP 02, 2022, Univ Parma, Parma, ITALY
Note

QC 20230626

Available from: 2023-06-26 Created: 2023-06-26 Last updated: 2025-03-27Bibliographically approved
Elson, F., Das, D., Simutis, G., Forslund, O. K., Miniotaite, U., Palm, R., . . . Månsson, M. (2023). TRIM Simulations Tool for mu(+) Stopping Fraction in Hydrostatic Pressure Cells. In: Prando, G Pratt, F (Ed.), 15th International Conference on Muon Spin Rotation, Relaxation and Resonance, MuSR 2022: . Paper presented at 15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR), AUG 28-SEP 02, 2022, Univ Parma, Parma, ITALY. IOP Publishing, 2462, Article ID 012024.
Open this publication in new window or tab >>TRIM Simulations Tool for mu(+) Stopping Fraction in Hydrostatic Pressure Cells
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2023 (English)In: 15th International Conference on Muon Spin Rotation, Relaxation and Resonance, MuSR 2022 / [ed] Prando, G Pratt, F, IOP Publishing , 2023, Vol. 2462, article id 012024Conference paper, Published paper (Refereed)
Abstract [en]

For quantum systems or materials, a common procedure for probing their behaviour is to tune electronic/magnetic properties using external parameters, e.g. temperature, magnetic field or pressure. Pressure application as an external stimuli is a widely used tool, where the sample in question is inserted into a pressure cell providing a hydrostatic pressure condition. Such device causes some practical problems when using in Muon Spin Rotation/Relaxation (mu+SR) experiments as a large proportion of the muons will be implanted in the pressure cell rather than in the sample, resulting in a higher background signal. This issue gets further amplified when the temperature dependent response from the sample is much smaller than that of the pressure cell,which may cause the sample response to be lost in the background and cause difficulties in aligning the sample within the beam. To tackle this issue, we have used pySRIM [1] to construct a practical and helpful simulation tool for calculating muon stopping fractions, specifically for the pressure cell setup at the mu E1 beamline using the GPD spectrometer at the Paul Scherrer Institute, with the use of TRIM simulations. The program is used to estimate the number of muon stopping in both the sample and the pressure cell at a given momentum. The simultion tool is programmed into a GUI, making it accessible to user to approximate prior to their experiments at GPD what fractions will belong to the sample and the pressure cell in their fitting procedure.

Place, publisher, year, edition, pages
IOP Publishing, 2023
Series
Journal of Physics Conference Series, ISSN 1742-6588
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-329454 (URN)10.1088/1742-6596/2462/1/012024 (DOI)000995428200024 ()2-s2.0-85152619404 (Scopus ID)
Conference
15th International Conference on Muon Spin Rotation, Relaxation and Resonance (SR), AUG 28-SEP 02, 2022, Univ Parma, Parma, ITALY
Note

QC 20230621

Available from: 2023-06-21 Created: 2023-06-21 Last updated: 2023-06-21Bibliographically approved
Nocerino, E., Forslund, O. K., Wang, C., Sakurai, H., Elson, F., Palm, R., . . . Månsson, M. Magnetic nature of wolframite MgReO4.
Open this publication in new window or tab >>Magnetic nature of wolframite MgReO4
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(English)In: ISSN 2165-5286Article in journal (Other academic) Accepted
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-321703 (URN)10.48550/arXiv.2209.11966 (DOI)
Note

QC 20221129

Available from: 2022-11-21 Created: 2022-11-21 Last updated: 2025-03-27Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-6523-8448

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