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Theoretical Descriptions of Complex Magnetism in Transition Metals and Their Alloys
Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, The Institute of Technology.ORCID iD: 0000-0002-7563-1494
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In this thesis, various methods for studying solids by simulations of quantummechanical equations, have been applied to transition metals and their alloys. Transition metals such as Fe, Ni, and Mn, are not only cornerstones in modern technology, but also key components in the very fabric of the Earth interior. Such systems show highly complex magnetic properties. As shown within this thesis, to understand and predict their properties from a microscopic level, is still a highly demanding task for the the quantum theory of solids. This is especially crucial at elevated temperature and pressure.

It is found that the magnetic degrees of freedom are inseparable from the structural, elastic and chemical properties of such alloy systems. This requires theoretical descriptions capable of handling this interplay. Such schemes are discussed and demonstrated.

Furthermore, the importance of the description of Coulomb correlation effects is demonstrated by DFT calculations and also by going beyond the one-electron description by the LDA+DMFT method.

It is also shown how magnetic interactions in the half-metallic compound NiMnSb can be manipulated by alloying. The stability of these alloys is  also evaluated in calculations, and verified by experimental synthesis at ambient conditions.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2012. , 130 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1452
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:liu:diva-78781ISBN: 978-91-7519-885-9 (print)OAI: oai:DiVA.org:liu-78781DiVA: diva2:535818
Public defence
2012-06-14, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 13:15 (English)
Opponent
Supervisors
Available from: 2012-06-20 Created: 2012-06-20 Last updated: 2015-08-19Bibliographically approved
List of papers
1. Structural and magnetic ground-state properties of gamma-FeMn alloys from ab initio calculations
Open this publication in new window or tab >>Structural and magnetic ground-state properties of gamma-FeMn alloys from ab initio calculations
2011 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 84, no 10, 104423- p.Article in journal (Refereed) Published
Abstract [en]

The magnetic properties of fcc-FeMn alloys, especially at the Fe(0.5)Mn(0.5) composition, have been the subject of intense experimental and theoretical investigations for several decades. We carry out an ab initio theoretical study of this system, including simultaneous optimization of structural and magnetic properties, and find that the ground state is the locally relaxed noncollinear 3Q antiferromagnetic structure. We also show that the two most frequently used parameterizations of the generalized gradient approximation not only fail to reproduce the equilibrium lattice constant of FeMn alloys, and consequently the magnetic properties, but also internally yield qualitatively different results. For practical studies of these alloys, which currently attract great attention, we propose a set of approximations, which is internally consistent, and brings the equilibrium lattice constant and magnetic properties in good agreement with the experiment in the whole range of alloy compositions.

Place, publisher, year, edition, pages
American Physical Society, 2011
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-71074 (URN)10.1103/PhysRevB.84.104423 (DOI)000294922100002 ()
Note
Funding Agencies|Goran Gustafsson Foundation for Research in Natural Sciences and Medicine||Swedish e-Science Research Centre (SeRC)||Available from: 2011-09-30 Created: 2011-09-30 Last updated: 2017-12-08
2. Influence of chemical composition and magnetic effects on the elastic properties of fcc Fe-Mn alloys
Open this publication in new window or tab >>Influence of chemical composition and magnetic effects on the elastic properties of fcc Fe-Mn alloys
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2011 (English)In: Acta Materialia, ISSN 1359-6454, E-ISSN 1873-2453, Vol. 59, no 4, 1493-1501 p.Article in journal (Refereed) Published
Abstract [en]

The influence of the Mn content on the elastic properties of face centered cubic Fe-Mn alloys was studied using the combinatorial approach. Fe-Mn thin films with a graded chemical composition were synthesized. Nanoindentation experiments were carried out to investigate the elastic properties as a function of the Mn content. As the Mn content increases from similar to 23 to similar to 39 at.%, the average bulk modulus varies from 143 to 105 GPa. Ab initio calculations served to probe the impact of magnetic effects on the elastic properties. The magnetic state description with disordered local moments yields the best agreement with the experimental results, whereas with non-magnetic and antiferromagnetic configurations the bulk modulus is overestimated. The strong impact of the magnetic configuration may be understood based on the differences in the chemical bonding and the magnetovolume effect. It is suggested that, owing to minute energy differences of competing antiferromagnetic configurations, a mixture of these with a "notional magnetic disorder" is present, which is in fact well described by the disordered local moments model. These results show that the combinatorial thin film synthesis with subsequent nanoindentation is an appropriate tool for investigating the elastic properties of Fe-Mn alloys systematically as a function of the chemical composition, to validate theoretical models.

Place, publisher, year, edition, pages
Elsevier Science B.V., Amsterdam., 2011
Keyword
Iron alloys, Sputtering, Elastic properties, Ab initio calculations, Nanoindentation
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-66331 (URN)10.1016/j.actamat.2010.11.013 (DOI)000287265100018 ()
Available from: 2011-03-11 Created: 2011-03-11 Last updated: 2017-12-11Bibliographically approved
3. Ab initio lattice stability of fcc and hcp Fe-Mn random alloys
Open this publication in new window or tab >>Ab initio lattice stability of fcc and hcp Fe-Mn random alloys
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2010 (English)In: Journal of Physics: Condensed Matter, ISSN 0953-8984, E-ISSN 1361-648X, Vol. 22, no 29, 295402- p.Article in journal (Refereed) Published
Abstract [en]

We have studied the lattice stability of face centred cubic (fcc) versus hexagonal close packed (hcp) Fe-Mn random alloys using ab initio calculations. In the calculations we considered the antiferromagnetic order of local moments, which for fcc alloys models the magnetic configuration of this phase at room temperature (below its Neel temperature) as well as their complete disorder, corresponding to paramagnetic fcc and hcp alloys. For both cases, the results are consistent with our thermodynamic calculations, obtained within the Calphad approach. For the room temperature magnetic configuration, the cross-over of the total energies of the hcp phase and the fcc phase of Fe-Mn alloys is at the expected Mn content, whereas for the magnetic configuration above the fcc Neel temperature, the hcp lattice is more stable within the whole composition range studied. The increase of the total energy difference between hcp and antiferromagnetic fcc due to additions of Mn as well as the stabilizing effect of antiferromagnetic ordering on the fcc phase are well displayed. These results are of relevance for understanding the deformation mechanisms of these random alloys.

Place, publisher, year, edition, pages
Iop Publishing Ltd, 2010
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-58224 (URN)10.1088/0953-8984/22/29/295402 (DOI)000279616000012 ()
Available from: 2010-08-10 Created: 2010-08-09 Last updated: 2017-12-12Bibliographically approved
4. The influence of additions of Al and Si on the lattice stability of fcc and hcp Fe-Mn random alloys
Open this publication in new window or tab >>The influence of additions of Al and Si on the lattice stability of fcc and hcp Fe-Mn random alloys
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2011 (English)In: Journal of Physics: Condensed Matter, ISSN 0953-8984, E-ISSN 1361-648X, Vol. 23, no 24, 246003- p.Article in journal (Refereed) Published
Abstract [en]

We have studied the influence of additions of Al and Si on the lattice stability of face-centred-cubic (fcc) versus hexagonal-closed-packed (hcp) Fe-Mn random alloys, considering the influence of magnetism below and above the fcc Neel temperature. Employing two different ab initio approaches with respect to basis sets and treatment of magnetic and chemical disorder, we are able to quantify the predictive power of the ab initio methods. We find that the addition of Al strongly stabilizes the fcc lattice independent of the regarded magnetic states. For Si a much stronger dependence on magnetism is observed. Compared to Al, almost no volume change is observed as Si is added to Fe-Mn, indicating that the electronic contributions are responsible for stabilization/destabilization of the fcc phase.

Place, publisher, year, edition, pages
Iop Publishing Ltd, 2011
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-69173 (URN)10.1088/0953-8984/23/24/246003 (DOI)000291152500019 ()
Available from: 2011-06-17 Created: 2011-06-17 Last updated: 2017-12-11Bibliographically approved
5. Elastic properties of fcc Fe-Mn-X (X = Al, Si) alloys studied by theory and experiment
Open this publication in new window or tab >>Elastic properties of fcc Fe-Mn-X (X = Al, Si) alloys studied by theory and experiment
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2011 (English)In: Acta Materialia, ISSN 1359-6454, E-ISSN 1873-2453, Vol. 59, no 8, 3145-3155 p.Article in journal (Refereed) Published
Abstract [en]

We have studied the influence of Al and Si additions on the elastic properties of face-centered cubic (fcc) Fe-Mn random alloys with Fe/Mn ratios of 4.00 and 2.33 using ab initio calculations. When Al is added up to 8 at.% the shearing elastic constants (C-11-C-12)/2 and C-44 decrease, resulting in a drop of similar to 20% in shear and similar to 19% in Youngs modulus. In fcc Fe-Mn-Si alloys, the trends in the elastic constants are similar, but less drastic, with a similar to 7% shear and similar to 6% Youngs modulus decrease when Si is added up to 8 at.%. The Fe/Mn ratio exhibits a minor influence on the shear and Youngs modulus values at constant Al and Si contents. To assess the quality of the ab initio data Fe-Mn-Al and Fe-Mn-Si thin films with an fcc structure were combinatorially synthesized and the elastic properties measured using nanoindentation. For both systems the measured and calculated lattice parameters are in good agreement. Although the measured Youngs modulus data showed significant scatter due to the high surface roughness, they are in good agreement with the predicted values. For the Fe-Mn-Al system the calculations generally underestimate the experimental data by similar to 15%. For the Fe-Mn-Si system the calculated data are in general lower by similar to 10% than the experimentally determined values. The presented results are of relevance for multicomponent alloy design, since the effect of Si and Al addition on the elastic properties of Fe-Mn alloys can be predicted based on ab initio data.

Place, publisher, year, edition, pages
Elsevier Science B.V., Amsterdam., 2011
Keyword
Iron alloys, Sputtering, Elastic properties, Ab initio calculations, Nanoindentation
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-68186 (URN)10.1016/j.actamat.2011.01.054 (DOI)000290053100024 ()
Available from: 2011-05-13 Created: 2011-05-13 Last updated: 2017-12-11Bibliographically approved
6. Supercell Calculations of Hyperfine Interactions in Transition-Metal Alloys
Open this publication in new window or tab >>Supercell Calculations of Hyperfine Interactions in Transition-Metal Alloys
(English)Manuscript (preprint) (Other academic)
Abstract [en]

We have performed calculations for the hyperfine field in the disordered Fe0.5Ni0.5 alloy using supercells with up to 864 atoms. The computational scheme is based on exact muffin-tin orbitals and the locally self-consistent Green’s function formalism, which scales linearly with the number of atoms in the supercell. This scheme allows local environment effects, such as chemical and magnetic environment, and short-range order, to be explicitly included. Supercell calculations for Fe-Ni show that while the average fields coincides with that obtained using the coherent potential approximation, there is a significant distribution of the hyperfine fields depending on the local environment. The fields of Fe and Ni show qualitatively different behaviour as a function of the on-site magnetic moment, but scale linearly with the average magnetic moment in the first coordination shell.

National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-78774 (URN)
Available from: 2012-06-20 Created: 2012-06-20 Last updated: 2015-08-19Bibliographically approved
7. Importance of Thermally Induced Magnetic Excitations in First-principles Simulations of Elastic Properties of Transition Metal Alloys
Open this publication in new window or tab >>Importance of Thermally Induced Magnetic Excitations in First-principles Simulations of Elastic Properties of Transition Metal Alloys
2012 (English)In: Solid State Phenomena, ISSN 1012-0394, E-ISSN 1662-9779, Vol. 190, 291-294 p.Article in journal (Refereed) Published
Abstract [en]

We demonstrate the importance of accounting for the complex magnetic ground state and finite temperature magnetic excitations in theoretical simulations of structural and elastic properties of transition metal alloys. Considering Fe72Cr16Ni12 face centered cubic (fcc) alloy, we compare results of first-principles calculations carried out for ferromagnetic and non-magnetic states, as well as for the state with disordered local moments. We show that the latter gives much more accurate description of the elastic properties for paramagnetic alloys. We carry out a determination of the magnetic ground state for fcc Fe-Mn alloys, considering collinear, as well as non-collinear states, and show the sensitively of structural and elastic properties in this system to the detailed alignment between magnetic moments. We therefore conclude that it is essential to develop accurate models of the magnetic state for the predictive description of properties of transition metal alloys.

Keyword
Magnetic transition metal alloys, magnetic ground state, disordered local moments, elastic properties, first-principles simulations
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-78775 (URN)10.4028/www.scientific.net/SSP.190.291 (DOI)000308061600070 ()
Available from: 2012-06-20 Created: 2012-06-20 Last updated: 2017-12-07Bibliographically approved
8. Influence of the Magnetic State on the Chemical Order-Disorder Transition Temperature in Fe-Ni Permalloy
Open this publication in new window or tab >>Influence of the Magnetic State on the Chemical Order-Disorder Transition Temperature in Fe-Ni Permalloy
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2010 (English)In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 105, no 16, 167208- p.Article in journal (Refereed) Published
Abstract [en]

In magnetic alloys, the effect of finite temperature magnetic excitations on phase stability below the Curie temperature is poorly investigated, although many systems undergo phase transitions in this temperature range. We consider random Ni-rich Fe-Ni alloys, which undergo chemical order-disorder transition approximately 100 K below their Curie temperature, to demonstrate from ab initio calculations that deviations of the global magnetic state from ideal ferromagnetic order due to temperature induced magnetization reduction have a crucial effect on the chemical transition temperature. We propose a scheme where the magnetic state is described by partially disordered local magnetic moments, which in combination with Heisenberg Monte Carlo simulations of the magnetization allows us to reproduce the transition temperature in good agreement with experimental data.

Place, publisher, year, edition, pages
American Physical Society, 2010
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-61178 (URN)10.1103/PhysRevLett.105.167208 (DOI)000283056100008 ()
Note
Original Publication: Marcus Ekholm, H Zapolsky, A V Ruban, I Vernyhora, D Ledue and Igor Abrikosov, Influence of the Magnetic State on the Chemical Order-Disorder Transition Temperature in Fe-Ni Permalloy, 2010, PHYSICAL REVIEW LETTERS, (105), 16, 167208. http://dx.doi.org/10.1103/PhysRevLett.105.167208 Copyright: American Physical Society http://www.aps.org/Available from: 2010-11-08 Created: 2010-11-05 Last updated: 2017-12-12Bibliographically approved
9. Importance of correlation effects in hcp iron revealed by a pressure-induced electronic topological transition
Open this publication in new window or tab >>Importance of correlation effects in hcp iron revealed by a pressure-induced electronic topological transition
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2013 (English)In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 110, no 11Article in journal (Refereed) Published
Abstract [en]

We discover that hcp phases of Fe and Fe0.9Ni0.1 undergo an electronic topological transition at pressures of about 40 GPa. This topological change of the Fermi surface manifests itself through anomalous behavior of the Debye sound velocity, c/a lattice parameter ratio, and Mossbauer center shift observed in our experiments. First-principles simulations within the dynamic mean field approach demonstrate that the transition is induced by many-electron effects. It is absent in one-electron calculations and represents a clear signature of correlation effects in hcp Fe. DOI: 10.1103/PhysRevLett.110.117206

Place, publisher, year, edition, pages
American Physical Society, 2013
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-78777 (URN)10.1103/PhysRevLett.110.117206 (DOI)000316172500027 ()
Note

Funding Agencies|Swedish e-Science Research Centre (SeRC)||Swedish Research Council|621-2011-4426|Swedish Foundation for Strategic Research (SSF) programs SRL Grant|10-0026|German Science Foundation (DFG)||German Ministry for Education and Research (BMBF)||National Science Foundation-Earth Sciences|EAR-1128799|Department of Energy-Geosciences|DE-FG02-94ER14466|U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences|DE-AC02-06CH11357|

Available from: 2012-06-20 Created: 2012-06-20 Last updated: 2017-12-07Bibliographically approved
10. Configurational thermodynamics of Fe-Ni alloys at Earths core conditions
Open this publication in new window or tab >>Configurational thermodynamics of Fe-Ni alloys at Earths core conditions
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2011 (English)In: Earth and Planetary Science Letters, ISSN 0012-821X, E-ISSN 1385-013X, Vol. 308, no 1-2, 90-96 p.Article in journal (Refereed) Published
Abstract [en]

By means of ab-initio calculations, we perform an analysis of the configurational thermodynamics, effects of disorder, and structural energy differences in Fe-Ni alloys at the pressure and temperature conditions of the Earths core. We show from ab-initio calculations that the ordering energies of fcc and hcp-structured Fe-Ni solid solutions at these conditions depend sensitively on the alloy configuration, i.e., on the degree of chemical disorder, and are on a scale comparable with the structural energy differences. From configurational thermodynamic simulations we find that a distribution of Fe and Ni atoms in the solutions should be very close to completely disordered at these conditions. Using this model of the Fe-Ni system, we have calculated the fcc-hcp structural free energy difference in a wide pressure-temperature range of 120-360 GPa and 1000-6600K. Our calculations show that alloying of Fe with Ni below 3000 K favours stabilisation of the fcc phase over the hcp, in agreement with experiments. However, above 3000 K the effect is reversed, and at conditions corresponding to those of the Earths inner core, Ni acts as an agent to stabilise the hcp phase.

Place, publisher, year, edition, pages
Elsevier, 2011
Keyword
Earths inner core, Fe-Ni alloy, ab-initio calculations, crystal structure
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-70218 (URN)10.1016/j.epsl.2011.05.035 (DOI)000293486100009 ()
Note
Original Publication: Marcus Ekholm, Arkady Mikhaylushkin, Sergey Simak, B Johansson and Igor Abrikosov, Configurational thermodynamics of Fe-Ni alloys at Earths core conditions, 2011, Earth and Planetary Science Letters, (308), 1-2, 90-96. http://dx.doi.org/10.1016/j.epsl.2011.05.035 Copyright: Elsevier http://www.elsevier.com/Available from: 2011-08-26 Created: 2011-08-26 Last updated: 2017-12-08Bibliographically approved
11. Energetics and magnetic impact of 3d-metal doping of the half-metallic ferromagnet NiMnSb
Open this publication in new window or tab >>Energetics and magnetic impact of 3d-metal doping of the half-metallic ferromagnet NiMnSb
2008 (English)In: Physical Review B Condensed Matter, ISSN 0163-1829, E-ISSN 1095-3795, Vol. 77, no 14, 144414- p.Article in journal (Refereed) Published
Abstract [en]

We have performed a theoretical study of the effect of doping the half-Heusler alloy NiMnSb with the magnetic 3d metals Cr, Mn, Fe, Co, and Ni, with respect to both energetics and magnetic properties. Starting from the formation energies, we discuss the possibility of placing the dopant on different crystallographic positions in the alloy. We calculate total and local magnetic moments, effective exchange interactions, and density of states and also outline strategies to tune the magnetic properties of the alloy. Doping of NiMnSb with Cr as well as substituting some Ni with extra Mn have the largest impact on magnetic interactions in the system while preserving its half-metallic property. Therefore, we suggest the possibility that these dopants increase the thermal stability of half-metallicity in NiMnSb, with implications for its possible usage in spintronics applications.

Keyword
NiMnSb, spintronics, half-metallic, doping, defects
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:liu:diva-60433 (URN)10.1103/PhysRevB.77.144414 (DOI)
Available from: 2010-10-13 Created: 2010-10-13 Last updated: 2017-12-12
12. Ab initio calculations and synthesis of the off-stoichiometric half-Heusler phase Ni1-xMn1+xSb
Open this publication in new window or tab >>Ab initio calculations and synthesis of the off-stoichiometric half-Heusler phase Ni1-xMn1+xSb
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2010 (English)In: JOURNAL OF APPLIED PHYSICS, ISSN 0021-8979, Vol. 108, no 9Article in journal (Refereed) Published
Abstract [en]

We perform a combined theoretical and experimental study of the phase stability and magnetism of the off-stoichiometric Ni1-xMn1+xSb in the half-Heusler crystal phase. Our work is motivated by the need for strategies to engineer the magnetism of potentially half-metallic materials, such as NiMnSb, for improved performance at elevated temperatures. By means of ab initio calculations we investigate Ni1-xMn1+xSb over the whole composition range 0 andlt;= x andlt;= 1 of Ni replacing Mn and show that at relevant temperatures, the half-Heusler phase should be thermodynamically stable up to at least x=0.20 with respect to the competing C38 structure of Mn2Sb. Furthermore we find that half-Heusler Ni1-xMn1+xSb retains half-metallic band structure over the whole concentration range and that the magnetic moments of substitutional Mn-Ni atoms display magnetic exchange interactions an order of magnitude larger than the Ni-Mn interaction in NiMnSb. We also demonstrate experimentally that the alloys indeed can be created by synthesizing off-stoichiometric Ni1-xMn1+xSb films on MgO substrates by means of magnetron sputtering.

Place, publisher, year, edition, pages
American Institute of Physics, 2010
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-63149 (URN)10.1063/1.3476282 (DOI)000284270900068 ()
Note
Original Publication: Marcus Ekholm, Petter Larsson, Björn Alling, Ulf Helmersson and Igor Abrikosov, Ab initio calculations and synthesis of the off-stoichiometric half-Heusler phase Ni1-xMn1+xSb, 2010, JOURNAL OF APPLIED PHYSICS, (108), 9, 093712. http://dx.doi.org/10.1063/1.3476282 Copyright: American Institute of Physics http://www.aip.org/Available from: 2010-12-13 Created: 2010-12-13 Last updated: 2015-08-19Bibliographically approved

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