| 1. |
- Alekseev, A. Yu, et al.
(författare)
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Stability of 2D Alkaline-Earth Metal Silicides, Germanides and Stannides
- 2019
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Ingår i: International Journal of Nanoscience. - : World Scientific Publishing Co. Pte Ltd. - 0219-581X. ; 18:3-4
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Tidskriftsartikel (refereegranskat)abstract
- By means of ab initio calculations, we have estimated stability of 2D Me2X (Me = Mg, Ca, Sr, Ba and X = Si, Ge, Sn) in the T and Td phases, which are similar to the ones of 2D transition metal chalcogenides, in addition to their phonon spectra. The T phase is found to be more stable for 2D Ca2X, Sr2X and Ba2X, whereas the Td phase is predicted to be the ground state for 2D Mg2X. We have also discussed that imaginary frequencies in the calculated phonon spectra of 2D Me2X, which appeared in the vicinity of the Gamma point, were not necessarily associated with the dynamic instability.
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| 2. |
- Arapan, Sergiu, et al.
(författare)
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Volume-dependent electron localization in ceria
- 2015
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Ingår i: Physical Review B. Condensed Matter and Materials Physics. - : American Physical Society. - 1098-0121 .- 1550-235X. ; 91:12
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Tidskriftsartikel (refereegranskat)abstract
- We have performed a numerical study of the process of electron localization in reduced ceria. Our results show that different localized charge distributions can be attained in a bulk system by varying the lattice parameter. We demonstrate that the effect of electron localization is mainly determined by lattice relaxation and an accurate account for the effects of electronic correlation is necessary to achieve localized charge distribution.
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| 3. |
- Bondarenko, Nina G., et al.
(författare)
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Multi-polaron solutions, nonlocal effects and internal modes in a nonlinear chain
- 2019
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Ingår i: Journal of Physics. - : Institute of Physics (IOP). - 0953-8984 .- 1361-648X. ; 31:41
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Tidskriftsartikel (refereegranskat)abstract
- Multipolaron solutions were studied in the framework of the Holstein one-dimensional molecular crystal model. The study was performed in the continuous limit where the crystal model maps into the nonlinear Schrodinger equation for which a new periodic dnoidal solution was found for the multipolaron system. In addition, the stability of the multi-polaron solutions was examined, and it was found that dnoidal and dnoidal solutions stabilize in different ranges of the parameter space. Moreover, the model was studied under the influence of nonlocal effects and the polaronic dynamics was described in terms of internal solitonic modes.
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| 4. |
- Bondarenko, Nina G., et al.
(författare)
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Spin polaronics : Static and dynamic properties of spin polarons in La-doped CaMnO4
- 2019
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 100:13
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Tidskriftsartikel (refereegranskat)abstract
- The static and dynamic properties of spin polarons in La-doped CaMnO3 are explored theoretically, by means of an effective low-energy Hamiltonian. All parameters of the effective Hamiltonian are evaluated from first-principles theory. The Hamiltonian is used to investigate the temperature stability as well as the response to an external applied electric field, for spin polarons in bulk, surface, and as single two-dimensional layers. Technically this involves atomistic spin-dynamics simulations in combination with kinetic Monte Carlo simulations. Where a comparison can be made, our simulations exhibit excellent agreement with available experimental data and previous theory. Remarkably, we find that excellent control of the mobility of spin polarons in this material can be achieved, and that the critical parameters deciding this are the temperature and strength of the applied electrical field. We outline different technological implications of spin polarons, and point to spin polaronics as an emerging subfield of nanotechnology. In particular, we demonstrate that it is feasible to write and erase information on an atomic scale, by use of spin polarons in CaMnO3.
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| 5. |
- Bondarenko, Nina, et al.
(författare)
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Polaron mobility in oxygen-deficient and lithium-doped tungsten trioxide
- 2015
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Ingår i: Physical Review B. Condensed Matter and Materials Physics. - : AMER PHYSICAL SOC. - 1098-0121 .- 1550-235X. ; 92:16
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Tidskriftsartikel (refereegranskat)abstract
- Electron localization and polaron mobility in oxygen-deficient as well as Li-doped monoclinic tungsten trioxide have been studied in the adiabatic limit in the framework of density functional theory. We show that small polarons formed in the presence of oxygen vacancy prefer the bipolaronicW(5+)-W5+ configuration, whereas the W6+-W4+ configuration is found to be metastable. Our calculations suggest that bipolarons are tightly bound by the vacancy and therefore largely immobile. On the contrary, polarons formed as a result of Li intercalation can be mobile; the activation energy for polaron jumping in this case varies between 98 and 124 meV depending on the crystallographic direction. The formation of W5+-W5+ bipolarons in Li-WO3 is possible. When situated along [001] the bipolaronic configuration is 8 meV lower in energy than two separate W5+ polarons.
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| 6. |
- Bondarenko, N., et al.
(författare)
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Spin-polaron formation and magnetic state diagram in La-doped CaMnO3
- 2017
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 95:22
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Tidskriftsartikel (refereegranskat)abstract
- LaxCa1-xMnO3 (LCMO) has been studied in the framework of density functional theory (DFT) using Hubbard-U correction. We show that the formation of spin polarons of different configurations is possible in the G-type antiferromagnetic phase. We also show that the spin-polaron (SP) solutions are stabilized due to an interplay of magnetic and lattice effects at lower La concentrations and mostly due to the lattice contribution at larger concentrations. Our results indicate that the development of SPs is unfavorable in the C- and A-type antiferromagnetic phases. The theoretically obtained magnetic state diagram is in good agreement with previously reported experimental results.
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| 7. |
- Bondarenko, Nina
(författare)
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Theoretical studies of lattice- and spin-polarons
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Theoretical studies of lattice- and spin-polarons are presented in this thesis, where the primary tool is ab-initio electronic structure calculations. The studies are performed with employment of a variety of analytical and computational methods. For lattice-polarons, we present an analytical study where multipolaron solutions were found in the framework of the Holstein 1D molecular crystal model. Interestingly, we found a new periodic, dnoidal, solution for the multipolaron system. In addition to it, we examined the stability of multipolaron solutions, and it was found that cnoidal and dnoidal solutions stabilize in different ranges of the parameter space. Moreover, we add to the model nonlocal effects and described dynamics in terms of internal solitonic modes.Hole-polaron localization accompanying the formation of a cation vacancy in bulk MgO and CaO and at the (100) MgO/CaO interfaces is presented. We show that the ground state is found to be the O1-O1 bipolaronic configuration both in bulk oxides and at their interfaces. Moreover, the one-centered O2-O0 bipolaron was found to be metastable with its stability being enhanced at the interfaces compared to that in bulk oxides. Also, for several bipolaronic configurations, we analyzed possible transitions from O1-O1 to O2-O0. On the same line of reasoning, electron localization and polaron mobility in oxygen-deficient and Li-doped monoclinic tungsten trioxide has been studied. It is shown for WO3, that small polarons formed in the presence of oxygen vacancy prefer bipolaronic W5+-W5+ configuration rather than W6+-W4+ configuration, which is found to be metastable state. Also, it is demonstrated that the bipolarons are tightly bound to vacancies, and consequently exhibit low mobility in the crystal. On the other hand, we show that polarons formed as a result of Li intercalation are mobile and that they are being responsible for electrochromic properties discovered in the compound.Spin-polaron formation in La-doped CaMnO3, with G-type antiferromagnetic structure, was also studied. We found that for this material, spin-polarons are stabilized due to the interplay of magnetic and lattice-effects at lower La concentrations and mostly due to the lattice contribution at larger concentrations. We show that the formation of SP is unfavourable in the C- and A-type antiferromagnetic phase, in agreement with previously reported experimental studies. We have also studied dynamical and temperature dependent properties of spin-polarons in this compound. We estimated material specific exchange parameters from density functional theory and found that 3D magnetic polarons in the Heisenberg lattice stabilize at slightly higher temperatures than in the case of 2D magnetic polarons. Next, we have proposed a method to calculate magnetic polaron hopping barriers and studied spin-polaron mobility CaMnO3 using additional methods such as atomistic spin dynamics and kinetic Monte Carlo. We make a suggestion of using this system in nano-technological applications.
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| 8. |
- Chanda, Debabrata, et al.
(författare)
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Investigation of electrocatalytic activity on a N-doped reduced graphene oxide surface for the oxygen reduction reaction in an alkaline medium
- 2018
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Ingår i: International journal of hydrogen energy. - : PERGAMON-ELSEVIER SCIENCE LTD. - 0360-3199 .- 1879-3487. ; 43:27, s. 12129-12139
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Tidskriftsartikel (refereegranskat)abstract
- Today the search for new energy resources is a crucial topic for materials science. The development of new effective catalysts for the oxygen reduction reaction can significantly improve the performance of fuel cells as well as electrocatalytic hydrogen production. This study presents the scalable synthesis of nitrogen-doped graphene oxide for the oxygen reduction reaction. The combination of an ab initio theoretical investigation of the oxygen reduction reaction (ORR) mechanism and detailed electrochemical characterization allowed the identification of electrocatalytically active nitrogen functionalities. The dominant effect on electrocatalytic activity is the presence of graphitic and pyridinic nitrogen and also N-oxide functionalities. The overpotential of ORR for nitrogen-doped graphene oxide prepared by microwave-assisted synthesis outperformed the metal-doped graphene materials. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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| 9. |
- Claisse, Antoine, 1988-
(författare)
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Multiscale modeling of nitride fuels
- 2016
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Nitride fuels have always been considered a good candidate for GENIV reactors, as well as space reactors, due to their high fissile density, highthermal conductivity and high melting point. In these concepts, not beingcompatible with water is not a significant problem. However, in recent years,nitride fuels started to raise an interest for application in thermal reactors,as accident tolerant or high performance fuels. However, oxide fuels havebenefited from decades of intensive research, and thousands of reactor-years.As such, a large effort has to be made on qualifying the fuel and developingtools to help assess their performances.In this thesis, the modeling side of this task is chosen. The effort istwo-fold: determining fundamental properties using atomistic models andputting together all the properties to predict the performances under irradi-ation using a fuel performance code. The first part is done combining manyframeworks. The density functional theory is the basis to compute the elec-tronic structure of the materials, to which a Hubbard correction is added tohandle the strong correlation effects. Negative side effects of the Hubbardcorrection are tackled using the so-called occupation matrix control method.This combined framework is first tested, and then used to find electronic andmechanic properties of the bulk material as well as the thermomechanicalbehavior of foreign atoms. Then, another method, the self-consistent meanfield (SCMF) one, is used to reach the dynamics properties of these foreignatoms. In the SCMF theory, the data that were obtained performing the abinitio simulations are treated to provide diffusion and kinetic flux couplingproperties.In the second step of the work, the fuel performance code TRANSURA-NUS is used to model complete fuel pins. An athermal fission gas releasemodel based on the open porosity is developed and tested on oxide fuels.A model for nitride fuels is introduced, and some correlations are bench-marked. Major issues remaining are pointed out and recommendations asto how to solve them are made.
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| 10. |
- Diklic, Natasa P., et al.
(författare)
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Sodium storage via single epoxy group on graphene - The role of surface doping
- 2019
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Ingår i: Electrochimica Acta. - : Elsevier. - 0013-4686 .- 1873-3859. ; 297, s. 523-528
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Tidskriftsartikel (refereegranskat)abstract
- Due to its unique physical and chemical properties, graphene is being considered as a promising material for energy conversion and storage applications. Introduction of functional groups and dopants on/in graphene is a useful strategy for tuning its properties. In order to fully exploit its potential, atomic-level understanding of its interaction with species of importance for such applications is required. We present a DFT study of the interaction of sodium atoms with epoxy-graphene and analyze how this interaction is affected upon doping with boron and nitrogen. We demonstrate how the dopants, combined with oxygen-containing groups alter the reactivity of graphene towards Na. Dopants act as attractors of epoxy groups, enhancing the sodium adsorption on doped oxygen-functionalized graphene when compared to the case of non-doped epoxy-graphene. Furthermore, by considering thermodynamics of the Na interaction with doped epoxy-graphene it has been concluded that such materials are good candidates for Na storage applications. Therefore, we suggest that controlled oxidation of doped carbon materials could lead to the development of advanced anode materials for rechargeable Na-ion batteries.
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