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Structural and magnetic disorder in crystalline materials: a first principles study
Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
2019 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Disorder in crystalline materials can take different forms and originate from different sources. In particular, temperature introduces disorder in any kind of material. This can be observed as the appearance of vacant lattice sites in an otherwise perfect crystal, or as a random distribution of different elements on the same lattice in an alloy; at the same time, if the material is magnetic, temperature induces disorder also on the magnetic degrees of freedom. In this thesis, different levels of disorder associated to structure and magnetism are investigated by means of density functional theory and thermodynamic models.

I start with diffusion of Ti vacancies in TiN, which is studied by means of nonequilibrium ab initio molecular dynamics using the color diffusion algorithm at different temperatures. The result is an Arrhenius behavior of Ti vacancy jump rates.

A method to perform structural relaxations in magnetic materials in their hightemperature paramagnetic phase is then developed based on the disordered local moments approach in order to study vacancies, interstitial atoms, and combinations of defects in paramagnetic bcc Fe and B1 CrN, as well as the mixing enthalpy of bcc Fe1−xCrx random alloys. A correction to the energetics of every system due to the relaxation in the disordered magnetic state is observed in all cases.

Not related to temperature and disorder, but very important for an accurate description of magnetic materials, is the choice of the exchange and correlation functional to be employed in the first principles calculations. We have investigated the performance of a recently developed meta-GGA functional, the strongly constrained and appropriately normed (SCAN) functional, in comparison with the more commonly used LDA and PBE on the ferromagnetic elemental solids bcc Fe, fcc Ni, and hcp Co, and SCAN it is found to give negligible improvements, if not a worsening, in the description of these materials.

Finally, the coupling between vibrational and magnetic degrees of freedom is discussed by reviewing the literature and proposing an investigation of the influence of vibrations on longitudinal spin fluctuations. These excitations are here studied by means of thermodynamic models based on Landau expansion of the energy in even powers of the magnitude of the local magnetic moments. We find that vibrational and magnetic disorder alter the energy landscapes as a function of moment size also in bcc Fe, which is often considered a Heisenberg system, inducing a more itinerant electron behavior.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2019. , p. 70
Series
Linköping Studies in Science and Technology. Licentiate Thesis, ISSN 0280-7971 ; 1837
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:liu:diva-156835DOI: 10.3384/lic.diva-156835ISBN: 9789176850817 (print)OAI: oai:DiVA.org:liu-156835DiVA, id: diva2:1315467
Presentation
2019-05-23, Planck, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2019-05-14 Created: 2019-05-14 Last updated: 2019-05-14Bibliographically approved
List of papers
1. Nonequilibrium ab initio molecular dynamics determination of Ti monovacancy migration rates in B1 TiN
Open this publication in new window or tab >>Nonequilibrium ab initio molecular dynamics determination of Ti monovacancy migration rates in B1 TiN
2017 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 96, no 10, article id 104306Article in journal (Refereed) Published
Abstract [en]

We use the color diffusion (CD) algorithm in nonequilibrium (accelerated) ab initio molecular dynamics simulations to determine Ti monovacancy jump frequencies in NaCl-structure titanium nitride (TiN), at temperatures ranging from 2200 to 3000 K. Our results showthat theCDmethod extended beyond the linear-fitting rate-versus-force regime [Sangiovanni et al., Phys. Rev. B 93, 094305 (2016)] can efficiently determine metal vacancy migration rates in TiN, despite the low mobilities of lattice defects in this type of ceramic compound. We propose a computational method based on gamma-distribution statistics, which provides unambiguous definition of nonequilibrium and equilibrium (extrapolated) vacancy jump rates with corresponding statistical uncertainties. The acceleration-factor achieved in our implementation of nonequilibrium molecular dynamics increases dramatically for decreasing temperatures from 500 for T close to the melting point T-m, up to 33 000 for T approximate to 0.7 T-m

Place, publisher, year, edition, pages
AMER PHYSICAL SOC, 2017
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-141712 (URN)10.1103/PhysRevB.96.104306 (DOI)000411076000005 ()
Note

Funding Agencies|Swedish Foundation for Strategic Research (SSF) project SRL [10-0026]; Swedish Research Council (VR) [621-2011-4417, 2015-04391, 330-2014-6336]; Swedish Government Strategic Research Area Grant in Materials Science on Advanced Functional Materials [MatLiU 2009-00971]; Ministry of Education and Science of the Russian Federation [14.Y26.31.0005]; Marie Sklodowska Curie Actions [INCA 600398]; Swedish Foundation for Strategic Research; Stiftelsen Olle Engkvist Byggmastare

Available from: 2017-10-05 Created: 2017-10-05 Last updated: 2019-06-28
2. Lattice relaxations in disordered Fe-based materials in the paramagnetic state from first principles
Open this publication in new window or tab >>Lattice relaxations in disordered Fe-based materials in the paramagnetic state from first principles
2018 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 98, no 6, article id 064105Article in journal (Refereed) Published
Abstract [en]

The first-principles calculation of many material properties, in particular related to defects and disorder, starts with the relaxation of the atomic positions of the system under investigation. This procedure is routine for nonmagnetic and magnetically ordered materials. However, when it comes to magnetically disordered systems, in particular the paramagnetic phase of magnetic materials, it is not clear how the relaxation procedure should be performed or which geometry should be used. Here we propose a method for the structural relaxation of magnetic materials in the paramagnetic regime, in an adiabatic fast-magnetism approximation within the disordered local moment (DLM) picture in the framework of density functional theory. The method is straightforward to implement using any ab initio code that allows for structural relaxations. We illustrate the importance of considering the disordered magnetic state during lattice relaxations by calculating formation energies and geometries for an Fe vacancy and C insterstitial atom in body-centered cubic (bcc) Fe as well as bcc Fe1-xCrx random alloys in the paramagnetic state. In the vacancy case, the nearest neighbors to the vacancy relax toward the vacancy of 0.14 angstrom (-5% of the ideal bcc nearest-neighbor distance), which is twice as large as the relaxation in the ferromagnetic case. The vacancy formation energy calculated in the DLM state on these positions is 1.60 eV, which corresponds to a reduction of about 0.1 eV compared to the formation energy calculated using DLM but on ferromagnetic-relaxed positions. The carbon interstitial formation energy is found to be 0.41 eV when the DLM relaxed positions are used, as compared to 0.59 eV when the FM-relaxed positions are employed. For bcc Fe0.5Cr0.5 alloys, the mixing enthalpy is reduced by 5 meV/atom, or about 10%, when the DLM state relaxation is considered, as compared to positions relaxed in the ferromagnetic state.

Place, publisher, year, edition, pages
AMER PHYSICAL SOC, 2018
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-151199 (URN)10.1103/PhysRevB.98.064105 (DOI)000443139600004 ()
Note

Funding Agencies|Swedish Research Council (VR) [2014-6336]; Marie Sklodowska Curie Actions, Cofund [INCA 600398]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFOMatLiU) [2009 00971]; Swedish Foundation for Strategic Research

Available from: 2018-09-13 Created: 2018-09-13 Last updated: 2019-05-14
3. Assessing the SCAN functional for itinerant electron ferromagnets
Open this publication in new window or tab >>Assessing the SCAN functional for itinerant electron ferromagnets
Show others...
2018 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 98, no 9, article id 094413Article in journal (Refereed) Published
Abstract [en]

Density functional theory is a standard model for condensed-matter theory and computational material science. The accuracy of density functional theory is limited by the accuracy of the employed approximation to the exchange-correlation functional. Recently, the so-called strongly constrained appropriately normed (SCAN) [Sun, Ruzsinszky, and Perdew, Phys. Rev. Lett. 115, 036402 (2015)] functional has received a lot of attention due to promising results for covalent, metallic, ionic, as well as hydrogen- and van der Waals-bonded systems alike. In this work, we focus on assessing the performance of the SCAN functional for itinerant magnets by calculating basic structural and magnetic properties of the transition metals Fe, Co, and Ni. We find that although structural properties of bcc-Fe seem to be in good agreement with experiment, SCAN performs worse than standard local and semilocal functionals for fcc-Ni and hcp-Co. In all three cases, the magnetic moment is significantly overestimated by SCAN, and the 3d states are shifted to lower energies, as compared to experiments.

Place, publisher, year, edition, pages
AMER PHYSICAL SOC, 2018
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:liu:diva-151640 (URN)10.1103/PhysRevB.98.094413 (DOI)000444348500004 ()
Note

Funding Agencies|Swedish e-Science Research Centre (SeRC); Swedish Research Council (VR) through the International Career Grant [20146336]; Marie Sklodowska CurieActions, Cofund, Project [INCA 600398]; Swedish Foundation for Strategic Research (SSF) through the Future Research Leaders 6 program; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]; competence center FunMat-II - Vinnova [201605156]; Russian Science Foundation [18-12-00492]

Available from: 2018-09-27 Created: 2018-09-27 Last updated: 2019-05-14

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