Doctoral thesis (Dissertations and theses)
STUDY AND CHARACTERIZATION OF MAGNETIC AND MULTIFERROIC MATERIALS BY FIRST-PRINCIPLES CALCULATIONS
Garcia Castro, Andrés Camilo
2016
 

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Keywords :
Ferroelectrics; Magnetics; Multiferroics; Fluorides; Perovskites; Density-Functional Theory
Abstract :
[en] In the last fifteen years, multifunctional materials, and more specifically, multi- functional oxides have been widely studied due to its wide range of properties. Properties that go from superconductivity to ferroelectricity passing through mag- netism and multiferroism have been reported. Nonetheless, the fluoride family was left aside and little information is known about its possible ferroelectricity or mul- tiferroism. In this Ph.D thesis, we explored the electronic, vibrational, structural and magnetic properties of fluoride perovskite-based compounds. To such pur- poses, We performed ab-initio calculations based in the density-functional theory (DFT) as implemented in VASP and CRYSTAL codes. Our first step was to perform vibrational analyses in a large set of fluoroper- ovskites ABF3. Based on the results, we proposed a model that establishes an A-site geometrically driven ferroelectric vibrational instability in fluorides. Our studies reveal a different behavior as a function of isotropic pressure for NaBF3 with respect to oxides (e.g. BaTiO3) with B = Ca, V, Mn, and Zn. For these compounds we found an increase of the ferroelectric instability as a function of hydrostatic pressure. This probably due to the “transformation” of eigendisplace- ments responsible for the mode that creates the corresponding instability. In particular, an increase of ionic A-site radii present a strong influence in FE-polar instability. We also have shown, based on our first-principles calculations and symmetry theory analysis that all post-perovskites ABX3 with an active magnetic B-site cation can exhibit a noncollinear magnetic configuration, which happens to be allowed by symmetry. With these findings, the magnetic properties found exper- imentally were clarified for this particular high-pressure phase perovskite found at the Earth’s mantle. Additionally, We have predicted that NaMnF3 suffers a structural phase transition under pressure to a post-perovskite phase, where non- collinear ferromagnetism and large magnetic moment components are obtained within this high-pressure phase.. Going beyond, We have shown that it is possible to achieve multiferroic-induced state in NaMnF3 under epitaxial strain at compressive or tensile strain. We found a nonlinear behavior of the ferroelectric instability as well as a non-linear piezo- electric response as a function of epitaxial strain. The later completely different as the one found in oxide perovskites. Similarly, an out-of-plane polarization was observed, a property that has not been observed in oxides. We observed a Na + Mn sites cooperative ferroelectric ordering for compressive strain against a pure A-site geometrically driven ferroelectricity at tensile values of the ac-strain. Magnetic ordering reveals a non-collinear ground state with the GzAxFy repre- sentation. Even more interesting, and non-linear magnetoelectric coupling was found under the strained Pna1 ground state becoming the first known multifer- roic/magnetoelectric perovskite fluoride. Later, in order to go further, We studied the electronic and structural proper- ties of novel heterostructures based on oxyfluorides (KTaO3)n/(KBF3)l B = Zn and Ni interfaces. We found that the orbital levels splitting at the interfaces is strongly modified by the O–B–F coordination. The polar catastrophe phenomena also takes place in the oxyfluoride interfaces similarly to oxide heterostructure, however, we found that less number of layers are needed in order to achieve the insulator-to-metal transition when comparing to SrTiO3/LaAlO3 superlat- tices. We observed that the magnetism in the KTaO3/KNiF3 exhibits a moment magnitude modulations. Nevertheless, the magnetic structure keeps the G-type antiferromagnetism such as in the bulk former compound. Surprisingly, we ob- served a large k3-Rashba type splitting in at the oxyfluoride interfaces, at least four times larger than the one reported in SrTiO3/LaAlO3 interface and twice of the KTaO3-based transistor. In conclusion, we observed that fluorides-perovskites are good prototypes for multifunctional properties as oxides. Therefore, based on the results reported in this thesis, we expect that experimentalist and theoreticians can be motivated in characterization of fluorides, which can lead to a new set of unexplored materials with potential novel applications in electronics.
Disciplines :
Physics
Author, co-author :
Garcia Castro, Andrés Camilo ;  Université de Liège - ULiège > Doct. sc. (physique - Bologne)
Language :
English
Title :
STUDY AND CHARACTERIZATION OF MAGNETIC AND MULTIFERROIC MATERIALS BY FIRST-PRINCIPLES CALCULATIONS
Defense date :
12 April 2016
Institution :
ULiège - Université de Liège
Degree :
Doctorat en Sciences: Physique
Promotor :
Bousquet, Eric  ;  Université de Liège - ULiège > Complex and Entangled Systems from Atoms to Materials (CESAM)
Romero Castro, Aldo Humberto
President :
Ghosez, Philippe  ;  Université de Liège - ULiège > Complex and Entangled Systems from Atoms to Materials (CESAM)
Jury member :
Spaldin, Nicola
Castanedo Perez, Rebeca
Jimenez Sandoval, Sergio Joaquin
Mendoza Galvan, Arturo
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