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Atomically Layered and Ordered Rare-Earth i-MAX Phases: A New Class of Magnetic Quaternary Compounds
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0001-5036-2833
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Oak Ridge Natl Lab, TN 37831 USA.
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2019 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 31, no 7, p. 2476-2485Article in journal (Refereed) Published
Abstract [en]

In 2017, we discovered quaternary i-MAX phases atomically layered solids, where M is an early transition metal, A is an A group element, and X is C-with a ((M2/3M1/32)-M-1)(2)AC chemistry, where the M-1 and M-2 atoms are in-plane ordered. Herein, we report the discovery of a class of magnetic i-MAX phases in which bilayers of a quasi-2D magnetic frustrated triangular lattice overlay a Mo honeycomb arrangement and an Al Kagome lattice. The chemistry of this family is (Mo2/3RE1/3)(2)AlC, and the rare-earth, RE, elements are Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm, and Lu. The magnetic properties were characterized and found to display a plethora of ground states, resulting from an interplay of competing magnetic interactions in the presence of magnetocrystalline anisotropy.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2019. Vol. 31, no 7, p. 2476-2485
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-157225DOI: 10.1021/acs.chemmater.8b05298ISI: 000464477100029OAI: oai:DiVA.org:liu-157225DiVA, id: diva2:1324349
Note

Funding Agencies|Knut and Alice Wallenberg (KAW) Foundation [KAW 2015.0043]; Swedish Research Council [642-2013-8020, 2015-00607, 621-2014-4890]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]; DFG [SA 3095/2-1]; IAEC Pazy Foundation Grant; NSF [DMR-1740795]

Available from: 2019-06-13 Created: 2019-06-13 Last updated: 2020-03-26
In thesis
1. Synthesis and characterization of two- and three-dimensional nanolaminated carbides
Open this publication in new window or tab >>Synthesis and characterization of two- and three-dimensional nanolaminated carbides
2020 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis is focused towards the synthesis and characterization of novel nanolaminated materials in primarily bulk (powder) form. Of particular interest is magnetic materials, or laminates that can be used as precursor for two-dimensional (2D) materials. 2D materials typically display a large surface-to-volume ratio, and as such they are very promising for applications within energy storage and catalysis. A more recently discovered family of 2D transition metal carbides/nitrides, called MXenes, are currently attracting a lot of attention. MXenes are produced by selective etching of parent 3D nanolaminates, so called MAX phases, facilitating removal of selected atomic layers, and formation of 2D sheets.

In my work on new nanolaminates as precursors for 2D materials, I have synthesized (Mo2/3Sc1/3)2AlC and have studied its crystal structure. It was found that Mo and Sc are chemically ordered in the metal layers, with the in-plane ordering motivating the notation i-MAX for this new type of MAX phase alloy. By selective etching of Sc and Al, we thereafter produced a 2D materials with ordered vacancies, Mo1.33C, and studied the electrochemical properties. It was found that the material displayed a high capacitance, ~1200 F cm-3, which is 65% higher that the counterpart without vacancies, Mo2C.

I also synthesized a previously not known out-of-plane ordered Mo2ScAlC2 MAX phase. By selective etching of Al, we produced a 2D material, Mo2ScC2, which is correspondingly ordered in the out-of-plane direction. Another related laminated material was also discovered and synthesized, Sc2Al2C3, and its crystal structure was determined. The material is potentially useful for conversion into a 2D material. I have also shown that Sc2Al2C3 is an example of a series of materials with the same crystal structure, with Sc replaced by other metals.

Magnetic materials are used in many applications, such as for data storage devices. In particular, layered magnetic materials are of interest due to their anisotropic structure and potential formation of interesting magnetic characteristics. I have been synthesizing and characterizing magnetic nanolaminates, starting with the (V,Mn)3GaC2 MAX phase in the form of an epitaxial thin film. Analysis of the magnetic behavior showed a ferromagnetic response above room temperature I thereafter showed that our previously discovered family of i-MAX phases could be expanded with a subclass of ordered nanolaminates based on rare earth (RE) elements, of the general formula (Mo2/3RE1/3)2AlC , where RE=Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm, and Lu. I studied their crystal structure by scanning transmission microscopy (STEM), X-ray diffraction (XRD), and neutron diffraction. We found that these phases can crystalize in three different structures, of space group C2/m, C2/c, and Cmcm, respectively. The magnetic behavior was studied and the magnetic structure of two materials could be determined. We suggest that the complex behavior identified is due to competing magnetic interaction and frustration.

I also synthesized another rare earth-based nanolaminate, Mo4Ce4Al7C3. The crystal structure was investigated by single crystal X-ray diffraction and STEM. Magnetization analysis reveal a ferromagnetic ground state below 10.5 K. X-ray absorption near-edge structure provide evidence that Ce is in a mixed-valence state. X-ray magnetic circular dichroism shows that only one of the two Ce sites are magnetic. 

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2020. p. 44
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 2058
National Category
Physical Sciences
Identifiers
urn:nbn:se:liu:diva-163847 (URN)10.3384/diss.diva-163847 (DOI)9789179298791 (ISBN)
Public defence
2020-03-26, F-building, Campus Valla, Linköping, 13:00 (English)
Opponent
Supervisors
Funder
Swedish Research CouncilKnut and Alice Wallenberg Foundation
Available from: 2020-03-02 Created: 2020-02-21 Last updated: 2020-03-11Bibliographically approved

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