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Synthesis and characterization of magnetic (Cr0.5Mn0.5)2GaC thin films
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
Department of Physics and Astronomy, Uppsala University, Uppsala, Sweden.
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2015 (English)In: Journal of Materials Science, ISSN 0022-2461, E-ISSN 1573-4803, Vol. 50, no 13, p. 4495-4502Article in journal (Refereed) Published
Abstract [en]

Growth of (Cr0.5Mn0.5)2GaC thin films from C, Ga, and compound Cr0.5Mn0.5 targets is reported for depositions on MgO (111), 4H-SiC (0001), and Al2O3 (0001) with and without a NbN (111) seed layer. Structural quality is found to be highly dependent on the choice of substrate with MgO (111) giving the best results as confirmed by X-ray diffraction and transmission electron microscopy. Phase pure, high crystal quality MAX phase thin films are realized, with a Cr:Mn ratio of 1:1. Vibrating sample magnetometry shows a ferromagnetic component from 30 K up to 300 K, with a measured net magnetic moment of 0.67 μB per metal (Cr + Mn) atom at 30 K and 5 T. The temperature dependence of the magnetic response suggests competing magnetic interactions with a resulting non-collinear magnetic ordering.

Place, publisher, year, edition, pages
Springer Berlin/Heidelberg, 2015. Vol. 50, no 13, p. 4495-4502
Keyword [en]
magnetism, thin films, magnetron sputtering, MAX phase
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-118837DOI: 10.1007/s10853-015-8999-8ISI: 000354093500005OAI: oai:DiVA.org:liu-118837DiVA, id: diva2:818175
Note

At the time for thesis presentation publication was in status: Manuscript

Funding Agencies|European Research Council under the European Community [258509]; Swedish Research Council (VR) [642-2013-8020, 621-2012-4425]; KAW Fellowship program; SSF synergy grant FUNCASE; Icelandic University Research fund

Available from: 2015-06-08 Created: 2015-06-04 Last updated: 2018-03-15Bibliographically approved
In thesis
1. Synthesis and characterization of Ga-containing MAX phase thin films
Open this publication in new window or tab >>Synthesis and characterization of Ga-containing MAX phase thin films
2014 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

The study of magnetic Mn+1AXn (MAX) phases (n = 1 − 3, M – a transition metal, A – an A group element, X – C or N) is a recently established research area, fuelled by theoretical predictions and first confirmed experimentally through alloying of Mn into the well-known Cr2AlC and Cr2GeC. Theoretical phase stability investigations suggested a new magnetic MAX phase, Mn2GaC, containing Ga which is liquid close to room temperature. Hence, alternative routes for MAX phase synthesis were needed, motivating a further development of magnetron sputtering from liquid targets.

In this thesis, (Cr1-xMnx)2GaC 0 ≤ x ≤ 1  MAX phase thin films have been synthesized from elemental and/or compound targets, using ultra high vacuum magnetron sputtering. Initial thin film synthesis of Cr2GaC was performed using elemental targets, including liquid Ga. Process optimization ensured optimal target size and crucible geometry for containing the Ga. Films were deposited at 650 °C on MgO(111) substrates. X-ray diffraction and transmission electron microscopy confirms the growth of epitaxial Cr2GaC MAX phase with minor inclusions of Cr3Ga.

To explore the magnetic characteristics upon Mn alloying, synthesis of (Cr0.5Mn0.5)2GaC thin films was performed from elemental Ga and C and a composite Cr/Mn target of 1:1 composition. Films were deposited on MgO(111), Al2O3(0001) (with or without NbN seed layer), and 4° off-cut 4H-SiC(0001) substrates. The films are smooth and of high structural quality as confirmed by X-ray diffraction and transmission electron microscopy. The film composition measured by high resolution energy dispersive X-ray spectroscopy confirms a composition corresponding to (Cr0.5Mn0.5)2GaC. The magnetic response, as measured with vibrating sample magnetometry, displays a ferromagnetic component, however, the temperature dependence of the magnetic moments and saturation fields suggests competing magnetic interaction and possible non-collinear magnetic ordering.

Finally, inspired by theoretical predictions, a new member of the MAX phase family, Mn2GaC, was synthesized. This is the first MAX phase containing Mn as a sole M element. X-ray diffraction and transmission electron microscopy confirms the characteristic MAX phase structure with a 2:1:1 composition. Theoretical work suggests that the magnetic ground state is almost degenerate between ferromagnetic and anti-ferromagnetic. Vibrating sample magnetometry shows ferromagnetic response with a transition temperature Tc of 230 K. However, also for this phase, complex magnetism is suggested. Altogether, the results indicate a new family of magnetic nanolaminates with a rich variation of magnetic ground states.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2014. p. 29
Series
Linköping Studies in Science and Technology. Thesis, ISSN 0280-7971 ; 1680
National Category
Physical Sciences Materials Engineering
Identifiers
urn:nbn:se:liu:diva-110764 (URN)10.3384/lic.diva-110764 (DOI)978-91-7519-224-6 (ISBN)
Presentation
2014-10-23, Planck, Fysikhuset, Campus Valla, Linköping, 13:15 (English)
Opponent
Supervisors
Available from: 2014-09-22 Created: 2014-09-22 Last updated: 2017-10-17Bibliographically approved
2. Synthesis and characterization of magnetic nanolaminated carbides
Open this publication in new window or tab >>Synthesis and characterization of magnetic nanolaminated carbides
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

MAX phases are a group of nanolaminated ternary carbides and nitrides, with a composition expressed by the general formula Mn+1AXn (𝑛 = 1 − 3), where M is a transition metal, A is an A-group element, and X is carbon and/or nitrogen. MAX phases have attracted interest due to their unique combination of metallic and ceramic properties, related to their inherently laminated structure of a transition metal carbide (Mn+1Xn) layer interleaved by an A-group metal layer.

This Thesis explores synthesis and characterization of magnetic MAX phases, where the A-group element is gallium (Ga). Due to the low melting point of Ga (T = 30 °C), conventional thin film synthesis methods become challenging, as the material is in liquid form at typical process temperatures. Development of existing methods has therefore been investigated, for reliable/reproducible synthesis routes, including sputtering from a liquid target, and resulting high quality material. Routes for minimizing trial-and-error procedures during optimization of thin film synthesis have also been studied, allowing faster identification of optimal deposition conditions and a simplified transfer of essential deposition parameters between different deposition systems.

A large part of this Thesis is devoted towards synthesis of MAX phase thin films in the Cr-Mn-Ga-C system. First, through process development, thin films of Cr2GaC were deposited by magnetron sputtering. The films were epitaxial, however with small amount of impurity phase Cr3Ga, as confirmed by X-ray diffraction (XRD) measurements. The film structure was confirmed by scanning transmission electron microscopy (STEM) and the composition by energy dispersive X-ray spectroscopy (EDX) inside the TEM.

Inspired by predictive ab initio calculations, the new MAX phase Mn2GaC was successfully synthesized in thin film form by magnetron sputtering. Structural parameters and magnetic properties were analysed. The material was found to have two magnetic transitions in the temperature range 3 K to 750 K, with a first order transition at around 214 K, going from non-collinear antiferromagnetic state at lower temperature to an antiferromagnetic state at higher temperature. The Neél temperature was determined to be 507 K, changing from an antiferromagnetic to a paramagnetic state. Above 800 K, Mn2GaC decomposes. Furthermore, magnetostrictive, magnetoresistive and magnetocaloric properties of the material were iv determined, among which a drastic change in lattice parameters upon the first magnetic transition was observed. This may be of interest for magnetocaloric applications.

Synthesis of both Cr2GaC and Mn2GaC in thin film form opens the possibility to tune the magnetic properties through a solid solution on the transition metal site, by alloying the aforementioned Cr2GaC with Mn, realizing (Cr1-xMnx)2GaC. From a compound target with a Cr:Mn ratio of 1:1, thin films of (Cr0.5Mn0.5)2GaC were synthesized, confirmed by TEM-EDX. Optimized structure was obtained by deposition on MgO substrates at a deposition temperature of 600 ºC. The thin films were phase pure and of high structural quality, allowing magnetic measurements. Using vibrating sample magnetometry (VSM), it was found that (Cr0.5Mn0.5)2GaC has a ferromagnetic component in the temperature range from 30 K to 300 K, with the measured magnetic moment at high field decreasing by increasing temperature. The remanent moment and coercive field is small, 0.036 μB, and 12 mT at 30 K, respectively. Using ferromagnetic resonance spectroscopy, it was also found that the material has pure spin magnetism, as indicated by the determined spectroscopic splitting factor g = 2.00 and a negligible magnetocrystalline anisotropy energy.

Fuelled by the recent discoveries of in-plane chemically ordered quaternary MAX phases, so called i-MAX phases, and guided by ab initio calculations, new members within this family, based on Cr and Mn, were synthesized by pressureless sintering methods, realizing (Cr2/3Sc1/3)2GaC and (Mn2/3Sc1/3)2GaC. Their structural properties were determined. Through these phases, the Mn content is the highest obtained in a bulk MAX phase to date.

This work has further developed synthesis processes for sputtering from liquid material, for an optimized route to achieve thin films of controlled composition and a high structural quality. Furthermore, through this work, Mn has been added as a new element in the family of MAX phase elements. It has also been shown, that alloying with different content of Mn gives rise to varying magnetic properties in MAX phases. As a result of this Thesis, it is expected that the MAX phase family can be further expanded, with more members of new compositions and new properties.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2018. p. 58
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1918
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-145679 (URN)10.3384/diss.diva-145679 (DOI)9789176853429 (ISBN)
Public defence
2018-04-16, Planck, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2018-03-15 Created: 2018-03-15 Last updated: 2018-03-22Bibliographically approved

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Petruhins, AndrejsIngason, Arni SigurdurLu, JunRosén, Johanna

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