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Completeness of the exact muffin-tin orbitals: application to hydrogenated alloys
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Material Physics.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Material Physics.
KTH, School of Industrial Engineering and Management (ITM), Materials Science and Engineering, Applied Material Physics.ORCID iD: 0000-0003-2832-3293
2010 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 81, no 4Article in journal (Refereed) Published
Abstract [en]

We investigate the basis set convergence of the exact muffin-tin orbitals by monitoring the equation of state for Al, Cu, and Rh calculated in the conventional face-centered-cubic lattice (str-I) and in a face-centered-cubic lattice with one atomic and three empty sites per primitive cell (str-II). We demonstrate that three (spd) muffin-tin orbitals are sufficient to describe Al in both structures, but for str-II Cu and Rh at least five (spdfg) orbitals are needed to get converged equilibrium Wigner-Seitz radius (within <= 0.8%) and bulk modulus (<= 3.3%). We ascribe this slow convergence to the nearly spherical densities localized around the Cu and Rh atoms, which create strongly asymmetric charge distributions within the nearest cells around the empty sites. The potential sphere radius dependence of the theoretical results for structure str-II is discussed. It is shown that a properly optimized overlapping muffin-tin potential in combination with the spdfg basis yields acceptable errors in the equilibrium bulk properties. The basis set convergence is also shown on hydrogenated Sc and Sc-based alloys.

Place, publisher, year, edition, pages
2010. Vol. 81, no 4
Keyword [en]
total-energy calculations, initio molecular-dynamics, wave basis-set, ab-initio, electron-gas, surface-energy, ground-state, metals, approximation, semiconductors
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:kth:diva-19159DOI: 10.1103/PhysRevB.81.045122ISI: 000274002500053Scopus ID: 2-s2.0-77954824021OAI: oai:DiVA.org:kth-19159DiVA: diva2:337206
Funder
Swedish Research Council
Note

QC 20110121

Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2017-12-12Bibliographically approved
In thesis
1. Describing interstitials in close-packed lattices: first-principles study
Open this publication in new window or tab >>Describing interstitials in close-packed lattices: first-principles study
2010 (English)Licentiate thesis, comprehensive summary (Other academic)
Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2010. 32 p.
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-31124 (URN)978-91-7415-880-9 (ISBN)
Presentation
2011-03-25, Konferensrummet, Materialvetenskap, KTH, Brinellvägen 23, Stockholm, 10:00
Note
QC 20110309Available from: 2011-03-09 Created: 2011-03-09 Last updated: 2011-03-09Bibliographically approved
2. Describing Interstitials in Close-packed Lattices: First-principles Study
Open this publication in new window or tab >>Describing Interstitials in Close-packed Lattices: First-principles Study
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Describing interstitial atoms in intermetallics or simple mono-atomic close-packed metals is a straightforward procedure in common full-potential calculations. One establishes a sufficiently large supercell, introduces the interstitial impurity and performs the electronic structure and total energy calculation. Real systems, however, are rarely mono-atomic or ordered metals. In most of the cases, the matrix is a random or quasirandom mixture of several chemically and/or magnetically distinct components. Because of that a proper computational tool should incorporate advanced alloy theory and at the same time have sufficiently high accuracy to describe interstitial positions in close-packed solids. The purpose of the present thesis is to make a step towards solving this fundamental problem in computational materials science. To this end, in the first part of the thesis a prestudy on some selected metals and compounds was presented, and in the second part tools were applied to investigate the effect of interstitial carbon on the structural properties of steels.

For the prestudy, the equation of state for the selected Al, Cu and Rh was investigated in two equivalent phases: in conventional face-centered-cubic lattice (fcc, str-I) and in a face-centered-cubic lattice with one atomic and three interstitial empty potentialwells per primitive cell (str-II). A proper basis set of the exact muffin-tin orbitals as well as a proper potential sphere radius were established by calculating the equilibrium Wigner-Seitz radius and bulk modulus of the above elements in str-I and str-II using the exact muffin-tin orbitals (EMTO) first-principle density functional method. It was found that for Al spd orbitals are sufficient to describe the equilibrium bulk properties in both structures, while for str-II Rh and Cu at least five orbitals (spdfg) are needed to get accurate equilibrium volume and bulk modulus. Furthermore, it was shown that in general, for the str-II type of structure (close-packed structure with interstitials) the optimized overlapping muffin-tin potential in combination with spdfg orbitals ensures well converged bulk properties.

As an application of the above work in alloys, (i) the chemical reaction between hydrogen H2 molecule and ScAl1−xMgx (0≤x≤0.3) random alloys, (ii) the phase stability of the hydrogenated alloys in different structures and (iii) the hydrogen absorption/desorption temperatures were studied by calculating the Gibbs energy for the components of the reaction. Experimental and theoretical studies by Sahlberg et al . showed that the ScAl0.8Mg0.2 compound with CsCl structure absorbs hydrogen by decomposing into ScH2 with CaF2 structure and fcc Al0.8Mg0.2. This reaction was found to be very fast, even without adding catalyst, and fully reversible. The theoretical hydrogen absorption/desorption temperatures agree well with the experimental values. On the other hand, the stability field of the hydrogenated alloys was found to be strongly depends on Mg content and on the microstructure of the hydrogenated alloys. For a given microstructure, the critical temperature for hydrogen absorption/desorption increases with the Mg concentration.

The second part of the thesis focused on steel materials with special emphases on the effect of interstitial carbon. Steels are considered to be one of the most important engineering materials. They are mainly composed of iron and carbon. Other alloying elements in steel are introduced to get specific properties like microstructure, corrosion resistance, hardness, brittleness, etc. In order to describe the effect of carbon interstitial in iron alloys, it is important to know how the substitutional alloying elements affect the softness and some other properties of iron alloys. For that reason, the alloying effects on the energetic and magnetic structure of paramagnetic Fe0.85Cr0.1M0.05 (M = Cr, Mn, Fe, Co and Ni) alloys along the tetragonal distortion path connecting the body centered cubic (bcc) and the face centered cubic (fcc) phases were investigated. It was shown that Cr stabilizes bcc phase and increases the energy barrier (relative to bcc phase) between fcc and bcc phases. Cobalt and Ni stabilize fcc structure. Cobalt increases whereas Ni slightly decreases the energy barrier relative to fcc structure. Manganese and iron have negligible effect on the structural energy difference as well as on the energy barrier along the Bain path. The local magnetic moments on Fe atoms have maximum values at bcc phase and minimum values at fcc phase. Cobalt atoms possess local magnetic moments only for tetragonal lattices with c/a < 1.30, and the Mn magnetic moments have almost constant value along the Bain path.

The tetragonality of Fe-C martensite was discovered in 1928. Early experimental works showed that the tetragonality of Fe-C is linearly depends on C content. However, Later many observations indicated that the tetragonality of martensite is influenced also by alloying and interstitial carbon distributions. Very few ab initio studies focus on investigating the tetragonality of Fe-C based alloys. In this thesis the interstitial carbon in ferromagnetic Fe-based alloys and it is impact on the tetragonal lattice ratio of Fe matrix as well as the alloying effect on the tetragonality of Fe-C system were investigated. It was found that the ferromagnetic Fe-C system with C content ∼ 1.3 wt. % has a body-centered tetragonal (bct) structure with c/a ∼ 1.07. Alloying has an impact on the tetragonality; adding 5% Al, Co or Ni enhances while 5% Cr addition decreases the tetragonal lattice ratio.

The electronic structure and total energy calculations from this thesis are based on firstprinciples exact muffin-tin orbitals method. The chemical and magnetic disorder was treated using coherent-potential approximation and the paramagnetic phase was modeled by the disordered local magnetic moments approach. Some test calculations involved also full-potential tools as implemented in Vienna ab-initio simulation package (VASP).

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2011. viii, 46 p.
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:kth:diva-47733 (URN)978-91-7501-124-0 (ISBN)
Public defence
2011-12-09, Sal K2, Teknikringen 28, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note
QC 20111118Available from: 2011-11-18 Created: 2011-11-11 Last updated: 2011-11-18Bibliographically approved

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