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Role of N defects in paramagnetic CrN at finite temperatures from first principles
Linköping University, Department of Physics, Chemistry and Biology, Theoretical Chemistry. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.
Linköping University, Department of Science and Technology, Media and Information Technology. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, The Institute of Technology. NUST MISIS, Russia; Tomsk State University, Russia.
2015 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 91, no 9, 094101- p.Article in journal (Refereed) Published
Abstract [en]

Simulations of defects in paramagnetic materials at high temperature constitute a formidable challenge to solid-state theory due to the interaction of magnetic disorder, vibrations, and structural relaxations. CrN is a material where these effects are particularly large due to a strong magnetolattice coupling and a tendency for deviations from the nominal 1: 1 stoichiometry. In this work, we present a first-principles study of nitrogen vacancies and nitrogen interstitials in CrN at elevated temperature. We report on formation energetics, the geometry of interstitial nitrogen dimers, and the impact on the electronic structure caused by the defects. We find a vacancy formation energy of 2.28 eV with a small effect of temperature, i.e., a formation energy for N interstitial in the form of a less than 111 greater than -oriented split bond of 3.77 eV with an increase to 3.97 at 1000 K. Vacancies are found to add three electrons, while split-bond interstitial adds one electron to the conduction band. The band gap of defect-free CrN is smeared out due to vibrations, although it is difficult to draw a conclusion about the exact temperature at which the band gap closes from our calculations. However, it is clear that at 900 K there is a nonzero density of electronic states at the Fermi level. At 300 K, our results indicate a border case where the band gap is about to close.

Place, publisher, year, edition, pages
American Physical Society , 2015. Vol. 91, no 9, 094101- p.
National Category
Physical Sciences Electrical Engineering, Electronic Engineering, Information Engineering
URN: urn:nbn:se:liu:diva-116954DOI: 10.1103/PhysRevB.91.094101ISI: 000350994400001OAI: diva2:802610

Funding Agencies|Swedish Research Council (VR) [621-2011-4426]; Ministry of Education and Science of the Russian Federation [14.Y26.31.0005]; Tomsk State University Academic D. I. Mendeleev Fund Program; VR [621-2011-4417]

Available from: 2015-04-13 Created: 2015-04-10 Last updated: 2016-08-23
In thesis
1. Theoretical Description of the Electron-Lattice Interaction in Molecular and Magnetic Crystals
Open this publication in new window or tab >>Theoretical Description of the Electron-Lattice Interaction in Molecular and Magnetic Crystals
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Electron-lattice interactions are often considered not to play a major role in material's properties as they are assumed to be small, the second-order effects. However, this study shows the importance of taking these effects into account in the simulations. My results demonstrate the impact of the electron-lattice interaction on the physics of the material and our understanding from it. One way to study these effects is to add them as perturbations to the unperturbed Hamiltonians in numerical simulations. The main objective of this thesis is to study electron-lattice interactions in molecular and magnetic crystals. It is devoted to developing numerical techniques considering model Hamiltonians and first-principles calculations to include the effect of lattice vibrations in the simulations of the above mentioned classes of materials.

In particular, I study the effect of adding the non-local electron-phonon coupling on top of the Holstein Hamiltonian to study the polaron stability and polaron dynamics in molecular crystals. The numerical calculations are based on the semi-empirical Holstein-Peierls model in which both intra (Holstein) and inter (Peierls) molecular electron-phonon interactions are taken into account. I study the effect of different parameters including intra and intermolecular electron-phonon coupling strengths and their vibrational frequencies, the transfer integral and the electric field on polaron stability. I found that in an ordered two dimensional molecular lattice the polaron is stable for only a limited range of parameter sets with the polaron formation energies lying in the range between 50 to 100 meV. Using the stable polaron solutions, I applied an electric field to the system and I observed that the polaron is dynamically stable and mobile for only a limited set of parameters. Adding disorder to the system will result in even more restricted parameter set space for which the polaron is stable and moves adiabatically with a constant velocity. In order to study the effect of temperature on polaron dynamics, I include a random force in Newtonian equations of motion in a one dimensional molecular lattice. I found that there is a critical temperature above which the polaron destabilizes and becomes delocalized.

Moreover, I study the role of lattice vibrations coupled to magnetic degrees of freedom in finite temperature paramagnetic state of magnetic materials. Calculating the properties of paramagnetic materials at elevated temperatures is a cumbersome task. In this thesis, I present a new method which allows us to couple lattice vibrations and magnetic disorder above the magnetic transition temperature and treat them on the same footing. The method is based on the combination of disordered local moments model and ab initio molecular dynamics (DLM-MD). I employ the method to study different physical properties of some model systems such as CrN and NiO in which the interaction between the magnetic and lattice degrees of freedom is very strong making them very good candidates for such a study.

I calculate the formation energies and study the effect of nitrogen defects on the electronic structure of paramagnetic CrN at high temperatures. Using this method I also study the temperature dependent elastic properties of paramagnetic CrN. The results highlight the importance of taking into account the magnetic excitations and lattice vibrations in the studies of magnetic materials at finite temperatures. A combination of DLM-MD with another numerical technique namely temperature dependent effective potential (TDEP) method is used to study the vibrational free energy and phase stability of CrN. We found that the combination of magnetic and vibrational contributions to the free energy shifts down the phase boundary between the cubic paramagnetic and orthorhombic antiferromagnetic phases of CrN towards the experimental value.

I used the stress-strain relation to study the temperature-dependent elastic properties of paramagnetic materials within DLM-MD with CrN as my model system. The results from a combinimation of DLM-MD with another newly developed method, symmetry imposed force constants (SIFC) in conjunction with TDEP is also presented as comparison to DLM-MD results.I also apply DLM-MD method to study the electronic structure of NiO in its paramagnetic state at finite temperatures. I found that lattice vibrations have a prominent impact on the electronic structure of paramagnetic NiO at high temperatures and should be included for the proper description of the density of states.

In summary, I believe that the proposed techniques give reliable results and allow us to include the effects from electron-lattice interaction in simulations of materials.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2016. 85 p.
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1766
Molecular crystals, Charge transport, Polaron, Magnetic materials, Paramagnetic state, Molecular dynamics
National Category
Condensed Matter Physics
urn:nbn:se:liu:diva-130517 (URN)10.3384/diss.diva-130517 (DOI)9789176857625 (Print) (ISBN)
Public defence
2016-09-16, Plank, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Available from: 2016-08-23 Created: 2016-08-11 Last updated: 2016-08-23Bibliographically approved

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