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Skorodumova, Natalia V.
Alternative names
Publications (10 of 93) Show all publications
Nowakowska, S., Mazzola, F., Alberti, M. N., Song, F., Voigt, T., Nowakowski, J., . . . Jung, T. A. (2018). Adsorbate-Induced Modification of the Confining Barriers in a Quantum Box Array. ACS Nano, 12(1), 768-778
Open this publication in new window or tab >>Adsorbate-Induced Modification of the Confining Barriers in a Quantum Box Array
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2018 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 12, no 1, p. 768-778Article in journal (Refereed) Published
Abstract [en]

Quantum devices depend on addressable elements, which can be modified separately and in their mutual interaction. Self-assembly at surfaces, for example, formation of a porous (metal-) organic network, provides an ideal way to manufacture arrays of identical quantum boxes, arising in this case from the confinement of the electronic (Shockley) surface state within the pores. We show that the electronic quantum box state as well as the interbox coupling can be modified locally to a varying extent by a selective choice of adsorbates, here C60, interacting with the barrier. In view of the wealth of differently acting adsorbates, this approach allows for engineering quantum states in on-surface network architectures.

Keywords
quantum box, electronic coupling, on-surface self-assembled network, surface state, adsorption
National Category
Condensed Matter Physics Nano Technology
Identifiers
urn:nbn:se:uu:diva-346371 (URN)10.1021/acsnano.7b07989 (DOI)000423495200082 ()29272579 (PubMedID)
Funder
Swedish Research Council, 348-2012-6196; 2014-5993EU, European Research Council, ERC-2012-StG 307760-SURF-PROKnut and Alice Wallenberg FoundationEuropean Social Fund (ESF)
Available from: 2018-03-23 Created: 2018-03-23 Last updated: 2018-03-23Bibliographically approved
Pasti, I. A., Jovanovic, A., Dobrota, A. S., Mentus, S. V., Johansson, B. & Skorodumova, N. V. (2018). Atomic adsorption on graphene with a single vacancy: systematic DFT study through the periodic table of elements. Physical Chemistry, Chemical Physics - PCCP, 20(2), 858-865
Open this publication in new window or tab >>Atomic adsorption on graphene with a single vacancy: systematic DFT study through the periodic table of elements
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2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 2, p. 858-865Article in journal (Refereed) Published
Abstract [en]

Vacancies in graphene present sites of altered chemical reactivity and open possibilities to tune graphene properties by defect engineering. The understanding of chemical reactivity of such defects is essential for successful implementation of carbon materials in advanced technologies. We report the results of a systematic DFT study of atomic adsorption on graphene with a single vacancy for the elements of rows 1-6 of the periodic table of elements (PTE), excluding lanthanides. The calculations have been performed using the PBE, long-range dispersion interaction-corrected PBE (PBE+D2 and PBE+D3) and non-local vdW-DF2 functionals. We find that most elements strongly bind to the vacancy, except for the elements of groups 11 and 12, and noble gases, for which the contribution of dispersion interaction to bonding is most significant. The strength of the interaction with the vacancy correlates with the cohesive energy of the elements in their stable phases: the higher the cohesive energy is, the stronger bonding to the vacancy can be expected. As most atoms can be trapped at the SV site we have calculated the potentials of dissolution and found that in most cases the metals adsorbed at the vacancy are more "noble" than they are in their corresponding stable phases.

National Category
Chemical Sciences Physical Sciences
Identifiers
urn:nbn:se:uu:diva-341487 (URN)10.1039/c7cp07542a (DOI)000419219700015 ()29238768 (PubMedID)
Available from: 2018-02-28 Created: 2018-02-28 Last updated: 2018-02-28Bibliographically approved
Pasti, I. A., Jovanovic, A., Dobrota, A. S., Mentus, S. V., Johansson, B. & Skorodumova, N. V. (2018). Atomic adsorption on pristine graphene along the Periodic Table of Elements - From PBE to non-local functionals. Applied Surface Science, 436, 433-440
Open this publication in new window or tab >>Atomic adsorption on pristine graphene along the Periodic Table of Elements - From PBE to non-local functionals
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2018 (English)In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 436, p. 433-440Article in journal (Refereed) Published
Abstract [en]

The understanding of atomic adsorption on graphene is of high importance for many advanced technologies. Here we present a complete database of the atomic adsorption energies for the elements of the Periodic Table up to the atomic number 86 (excluding lanthanides) on pristine graphene. The energies have been calculated using the projector augmented wave (PAW) method with PBE, long-range dispersion interaction corrected PBE (PBE+D2, PBE+D3) as well as non-local vdW-DF2 approach. The inclusion of dispersion interactions leads to an exothermic adsorption for all the investigated elements. Dispersion interactions are found to be of particular importance for the adsorption of low atomic weight earth alkaline metals, coinage and s-metals (11th and 12th groups), high atomic weight p-elements and noble gases. We discuss the observed adsorption trends along the groups and rows of the Periodic Table as well some computational aspects of modelling atomic adsorption on graphene.

Place, publisher, year, edition, pages
ELSEVIER SCIENCE BV, 2018
Keywords
Graphene, Adsorption, Atomic adsorption, Periodic Table of Elements, Dispersion interactions
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-350485 (URN)10.1016/j.apsusc.2017.12.046 (DOI)000425723100050 ()
Funder
Swedish Research Council, 348-2012-6196]Swedish Research Council, 2014-5993]Carl Tryggers foundation
Available from: 2018-05-17 Created: 2018-05-17 Last updated: 2018-05-17Bibliographically approved
Klarbring, J., Skorodumova, N. V. & Simak, S. I. (2018). Finite-temperature lattice dynamics and superionic transition in ceria from first principles. Physical Review B, 97(10), Article ID 104309.
Open this publication in new window or tab >>Finite-temperature lattice dynamics and superionic transition in ceria from first principles
2018 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 97, no 10, article id 104309Article in journal (Refereed) Published
Abstract [en]

Ab initio molecular dynamics (AIMD) in combination with the temperature dependent effective potential (TDEP) method has been used to go beyond the quasiharmonic approximation and study the lattice dynamics in ceria, CeO2, at finite temperature. The results indicate that the previously proposed connection between the B-1u phonon mode turning imaginary and the transition to the superionic phase in fluorite structured materials is an artifact of the failure of the quasiharmonic approximation in describing the lattice dynamics at elevated temperatures. We instead show that, in the TDEP picture, a phonon mode coupling to the E-u mode prevents the B-1u mode from becoming imaginary. We directly observe the superionic transition at high temperatures in our AIMD simulations and find that it is initiated by the formation of oxygen Frenkel pairs (FP). These FP are found to form in a collective process involving simultaneous motion of two oxygen ions.

Place, publisher, year, edition, pages
AMER PHYSICAL SOC, 2018
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-350999 (URN)10.1103/PhysRevB.97.104309 (DOI)000427982100003 ()
Funder
Swedish Research Council, 2014-4750Swedish Research Council, 2014-5993
Available from: 2018-05-17 Created: 2018-05-17 Last updated: 2018-05-17Bibliographically approved
Fako, E., Dobrota, A. S., Pasti, I. A., Lopez, N., Mentus, S. V. & Skorodumova, N. V. (2018). Lattice mismatch as the descriptor of segregation, stability and reactivity of supported thin catalyst films. Physical Chemistry, Chemical Physics - PCCP, 20(3), 1524-1530
Open this publication in new window or tab >>Lattice mismatch as the descriptor of segregation, stability and reactivity of supported thin catalyst films
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2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 3, p. 1524-1530Article in journal (Refereed) Published
Abstract [en]

The increasing demand and high prices of advanced catalysts motivate a constant search for novel active materials with reduced contents of noble metals. The development of thin films and core-shell catalysts seems to be a promising strategy along this path. Using density functional theory we have analyzed a number of surface properties of supported bimetallic thin films with the composition A(3)B (where A = Pt and Pd, and B = Cu, Ag and Au). We focus on the surface segregation, dissolution stability and surface electronic structure. We also address the chemisorption properties of Pd3Au thin films supported by different substrates, by probing the surface reactivity with CO. We find a strong influence of the support in the case of mono- and bilayers, while the surface strain seems to be the predominant factor in determining the surface properties of supported trilayers and thicker films. In particular, we show that the studied properties of the supported trilayers can be predicted from the lattice mismatch between the overlayer and the support. Namely, if the strain dependence of the corresponding quantities for pure strained surfaces is known, the properties of strained supported trilayers can be reliably estimated. The obtained results can be used in the design of novel catalysts and predictions of the surface properties of supported ultrathin catalyst layers.

National Category
Chemical Sciences
Identifiers
urn:nbn:se:uu:diva-343672 (URN)10.1039/c7cp07276g (DOI)000423019600021 ()29260157 (PubMedID)
Funder
Swedish Research Council, 348-2012-6196, 2014-5993Carl Tryggers foundation
Available from: 2018-03-05 Created: 2018-03-05 Last updated: 2018-03-08Bibliographically approved
Nilsson, J. O., Leetmaa, M., Wang, B., Zguns, P. A., Pasti, I., Sandell, A. & Skorodumova, N. V. (2018). Modeling Kinetics of Water Adsorption on the Rutile TiO2 (110) Surface: Influence of Exchange-Correlation Functional. Physica status solidi. B, Basic research, 255(3), Article ID 1700344.
Open this publication in new window or tab >>Modeling Kinetics of Water Adsorption on the Rutile TiO2 (110) Surface: Influence of Exchange-Correlation Functional
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2018 (English)In: Physica status solidi. B, Basic research, ISSN 0370-1972, E-ISSN 1521-3951, Vol. 255, no 3, article id 1700344Article in journal (Refereed) Published
Abstract [en]

The accuracy of the theoretical description of materials properties in the framework of density functional theory (DFT) inherently depends on the exchange-correlation (XC) functional used in the calculations. Here we investigate the influence of the choice of a XC functional (PBE, RPBE, PW91, and PBE0) on the kinetics of the adsorption, diffusion and dissociation of water on the rutile TiO2(110) surface using a combined Kinetic Monte Carlo (KMC) - DFT approach, where the KMC simulations are based on the barriers for the aforementioned processes calculated with DFT. We also test how the adsorption energy of intact and dissociated water molecules changes when dispersion interactions are included into the calculations. We consider the beginning of the water layer formation varying coverage up to 0.2 monolayer (ML) at temperatures up to 180K. We demonstrate that the dynamics of the simulated water-titania system is extremely sensitive to the choice of the XC functional.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH, 2018
Keywords
density functional theory, kinetic Monte Carlo simulations, rutile, surfaces, TiO2, water
National Category
Theoretical Chemistry Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-350888 (URN)10.1002/pssb.201700344 (DOI)000427260100018 ()
Funder
Swedish Research Council, 2014-5993]Swedish Energy Agency, 35515-1
Available from: 2018-05-21 Created: 2018-05-21 Last updated: 2018-05-21Bibliographically approved
Žguns, P. A., Ruban, A. V. & Skorodumova, N. V. (2018). Phase diagram and oxygen–vacancy ordering in the CeO2–Gd2O3 system: a theoretical study. Physical Chemistry, Chemical Physics - PCCP, 20(17), 11805-11818
Open this publication in new window or tab >>Phase diagram and oxygen–vacancy ordering in the CeO2–Gd2O3 system: a theoretical study
2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 17, p. 11805-11818Article in journal (Refereed) Published
Abstract [en]

We present the phase diagram of Ce1-xGdxO2-x/2 (CGO), calculated by means of a combined Density Functional Theory (DFT), cluster expansion and lattice Monte Carlo approach. We show that this methodology gives reliable results for the whole range of concentrations (x ≡ xGd ≤ 1). In the thermodynamic equilibrium, we observe two transitions: the onset of oxygen-vacancy (O-Va) ordering at ca. 1200-3300 K for concentrations xGd = 0.3-1, and a phase separation into CeO2 and C-type Gd2O3 occurring below ca. 1000 K for all concentrations. We also model 'quenched' systems, with cations immobile below 1500 K, and observe that the presence of random-like cation configurations does not prevent C-type vacancy ordering. The obtained transition temperatures for Va ordering agree rather well with existing experimental data. We analyse the effect of vacancy ordering and composition on the lattice parameters and relaxation pattern of cations.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
National Category
Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-353404 (URN)10.1039/c8cp01029c (DOI)000431824000034 ()29658037 (PubMedID)
Funder
Swedish Research Council, VR 348-2012-6196 2015-05538EU, European Research Council
Available from: 2018-06-12 Created: 2018-06-12 Last updated: 2018-09-03
Migas, D. B., Bogorodz, V. O., Filonov, A. B., Borisenko, V. E. & Skorodumova, N. V. (2018). Quasi-2D silicon structures based on ultrathin Me2Si (Me = Mg, Ca, Sr, Ba) films. Surface Science, 670, 51-57
Open this publication in new window or tab >>Quasi-2D silicon structures based on ultrathin Me2Si (Me = Mg, Ca, Sr, Ba) films
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2018 (English)In: Surface Science, ISSN 0039-6028, E-ISSN 1879-2758, Vol. 670, p. 51-57Article in journal (Refereed) Published
Abstract [en]

By means of ab initio calculations with hybrid functionals we show a possibility for quasi-2D silicon structures originated from semiconducting Mg2Si, Ca2Si, Sr2Si and Ba2Si silicides to exist. Such a 2D structure is similar to the one of transition metal chalcogenides where silicon atoms form a layer in between of metal atoms aligned in surface layers. These metal surface atoms act as pseudo passivation species stabilizing crystal structure and providing semiconducting properties. Considered 2D Mg2Si, Ca2Si, Sr2Si and Ba2Si have band gaps of 1.14 eV, 0.69 eV, 0.33 eV and 0.19 eV, respectively, while the former one is also characterized by a direct transition with appreciable oscillator strength. Electronic states of the surface atoms are found to suppress an influence of the quantum confinement on the band gaps. Additionally, we report Sr2Si bulk in the cubic structure to have a direct band gap of 0.85 eV as well as sizable oscillator strength of the first direct transition.

Place, publisher, year, edition, pages
ELSEVIER SCIENCE BV, 2018
Keywords
2D materials, Semiconducting silicides, Surface passivation, Structural optimization, Band structure
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-350483 (URN)10.1016/j.susc.2017.12.017 (DOI)000426232100007 ()
Funder
Swedish Research Council, 2014-5993
Available from: 2018-05-17 Created: 2018-05-17 Last updated: 2018-05-17Bibliographically approved
Jovanovic, A., Dobrota, A. S., Rafailovic, L. D., Mentus, S. V., Pasti, I. A., Johansson, B. & Skorodumova, N. V. (2018). Structural and electronic properties of V2O5 and their tuning by doping with 3d elements - modelling using the DFT plus U method and dispersion correction. Physical Chemistry, Chemical Physics - PCCP, 20(20), 13934-13943
Open this publication in new window or tab >>Structural and electronic properties of V2O5 and their tuning by doping with 3d elements - modelling using the DFT plus U method and dispersion correction
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2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 20, p. 13934-13943Article in journal (Refereed) Published
Abstract [en]

New electrode materials for alkaline-ion batteries are a timely topic. Among many promising candidates, V2O5 is one of the most interesting cathode materials. While having very high theoretical capacity, in practice, its performance is hindered by its low stability and poor conductivity. As regards the theoretical descriptions of V2O5, common DFT-GGA calculations fail to reproduce both the electronic and crystal structures. While the band gap is underestimated, the interlayer spacing is overestimated as weak dispersion interactions are not properly described within GGA. Here we show that the combination of the DFT+U method and semi-empirical D2 correction can compensate for the drawbacks of the GGA when it comes to the modelling of V2O5. When compared to common PBE calculations, with a modest increase in the computational cost, PBE+U+D2 fully reproduced the experimental band gap of V2O5, while the errors in the lattice parameters are only a few percent. Using the proposed PBE+U+D2 methodology we studied the doping of V2O5 with 3d elements (from Sc to Zn). We show that both the structural and electronic parameters are affected by doping. Most importantly, a significant increase in conductivity is expected upon doping, which is of great importance for the application of V2O5 in metal-ion batteries.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:uu:diva-357738 (URN)10.1039/c8cp00992a (DOI)000433262300026 ()29744500 (PubMedID)
Funder
Swedish Research Council, 2014-5993
Available from: 2018-08-30 Created: 2018-08-30 Last updated: 2018-08-30Bibliographically approved
Lazarevic-Pasti, T., Anicijevic, V., Baljozovic, M., Anicijevic, D. V., Gutic, S., Vasic, V., . . . Pasti, I. A. (2018). The impact of the structure of graphene-based materials on the removal of organophosphorus pesticides from water. ENVIRONMENTAL SCIENCE-NANO, 5(6), 1482-1494
Open this publication in new window or tab >>The impact of the structure of graphene-based materials on the removal of organophosphorus pesticides from water
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2018 (English)In: ENVIRONMENTAL SCIENCE-NANO, ISSN 2051-8153, Vol. 5, no 6, p. 1482-1494Article in journal (Refereed) Published
Abstract [en]

The wide use of pesticides in modern agriculture and other areas results in an urgent need for their efficient removal from the environment. Adsorption of pesticides is one of the most commonly used strategies for this task. Here we analyze the adsorption of two organophosphorus pesticides, dimethoate (DMT) and chlorpyrifos (CPF), on graphene-based materials. The adsorption was found to be very sensitive to the structure of the adsorbents used. In particular, aliphatic DMT was found to prefer hydrophilic oxidized graphene surfaces. The CPF molecule, which contains an aromatic moiety, prefers adsorption on the surface of a graphene basal plane with high structural order and preserved electron system. The toxicity of pesticide solutions is reduced after adsorption, suggesting that there is no oxidation of DMT and CPF to more toxic oxo forms. We emphasize that the combination of structural properties of adsorbents and adsorbates defines the adsorption of organophosphorus pesticides on graphene-based materials, while the specific surface area of adsorbents is not the major factor.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY, 2018
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-358537 (URN)10.1039/c8en00171e (DOI)000435355700016 ()
Funder
Swedish Research Council, 2014-5993Carl Tryggers foundation
Available from: 2018-08-30 Created: 2018-08-30 Last updated: 2018-08-30Bibliographically approved
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