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Skorodumova, Natalia V.
Alternative names
Publications (10 of 90) 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
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
Pasti, I. A., Johansson, B. & Skorodumova, N. V. (2018). Tunable reactivity of supported single metal atoms by impurity engineering of the MgO(001) support. Physical Chemistry, Chemical Physics - PCCP, 20(9), 6337-6346
Open this publication in new window or tab >>Tunable reactivity of supported single metal atoms by impurity engineering of the MgO(001) support
2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 9, p. 6337-6346Article in journal (Refereed) Published
Abstract [en]

Development of novel materials may often require a rational use of high price components, like noble metals, in combination with the possibility to tune their properties in a desirable way. Here we present a theoretical DFT study of Au and Pd single atoms supported by doped MgO(001). By introducing B, C and N impurities into the MgO(001) surface, the interaction between the surface and the supported metal adatoms can be adjusted. Impurity atoms act as strong binding sites for Au and Pd adatoms and can help to produce highly dispersed metal particles. The reactivity of metal atoms supported by doped MgO(001), as probed by CO, is altered compared to their counterparts on pristine MgO(001). We find that Pd atoms on doped MgO(001) are less reactive than on perfect MgO(001). In contrast, Au adatoms bind CO much more strongly when placed on doped MgO(001). In the case of Au on N-doped MgO(001) we find that charge redistribution between the metal atom and impurity takes place even when not in direct contact, which enhances the interaction of Au with CO. The presented results suggest possible ways for optimizing the reactivity of oxide supported metal catalysts through impurity engineering.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-352729 (URN)10.1039/c7cp08370j (DOI)000429280100034 ()29435542 (PubMedID)
Funder
Swedish Research Council, 2014-5993Carl Tryggers foundation
Available from: 2018-06-07 Created: 2018-06-07 Last updated: 2018-06-07Bibliographically approved
Dobrota, A. S., Pasti, I. A., Mentus, S. V. & Skorodumova, N. V. (2017). A DFT study of the interplay between dopants and oxygen functional groups over the graphene basal plane - implications in energy-related applications. Physical Chemistry, Chemical Physics - PCCP, 19(12), 8530-8540
Open this publication in new window or tab >>A DFT study of the interplay between dopants and oxygen functional groups over the graphene basal plane - implications in energy-related applications
2017 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 12, p. 8530-8540Article in journal (Refereed) Published
Abstract [en]

Understanding the ways graphene can be functionalized is of great importance for many contemporary technologies. Using density functional theory calculations we investigate how vacancy formation and substitutional doping by B, N, P and S affect the oxidizability and reactivity of the graphene basal plane. We find that the presence of these defects enhances the reactivity of graphene. In particular, these sites act as strong attractors for OH groups, suggesting that the oxidation of graphene could start at these sites or that these sites are the most difficult to reduce. Scaling between the OH and H adsorption energies is found on both reduced and oxidized doped graphene surfaces. Using the O-2 molecule as a probe we show that a proper modelling of doped graphene materials has to take into account the presence of oxygen functional groups.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY, 2017
National Category
Physical Chemistry Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-320039 (URN)10.1039/c7cp00344g (DOI)000397860900045 ()28288218 (PubMedID)
Funder
Swedish Research Council, 348-2012-6196 2014-5993
Available from: 2017-04-13 Created: 2017-04-13 Last updated: 2017-11-29Bibliographically approved
Gutic, S. J., Dobrota, A. S., Leetmaa, M., Skorodumova, N. V. V., Mentus, S. V. & Pasti, I. A. (2017). Improved catalysts for hydrogen evolution reaction in alkaline solutions through the electrochemical formation of nickel-reduced graphene oxide interface. Physical Chemistry, Chemical Physics - PCCP, 19(20), 13281-13293
Open this publication in new window or tab >>Improved catalysts for hydrogen evolution reaction in alkaline solutions through the electrochemical formation of nickel-reduced graphene oxide interface
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2017 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 20, p. 13281-13293Article in journal (Refereed) Published
Abstract [en]

H-2 production via water electrolysis plays an important role in hydrogen economy. Hence, novel cheap electrocatalysts for the hydrogen evolution reaction ( HER) are constantly needed. Here, we describe a simple method for the preparation of composite catalysts for H-2 evolution, consisting in simultaneous reduction of the graphene oxide film, and electrochemical deposition of Ni on its surface. The obtained composites (Ni@rGO), compared to pure electrodeposited Ni, show an improved electrocatalytic activity towards HER in alkaline media. We found that the activity of the Ni@rGO catalysts depends on the surface composition ( Ni vs. C mole ratio) and on the level of structural disorder of the rGO support. We suggest that HER activity is improved via H-ads spillover from the Ni particles to the rGO support, where quick recombination to molecular hydrogen is favored. A deeper insight into such a mechanism of H-2 production was achieved by kinetic Monte-Carlo simulations. These simulations enabled the reproduction of experimentally observed trends under the assumption that the support can act as a Hads acceptor. We expect that the proposed procedure for the production of novel HER catalysts could be generalized and lead to the development of a new generation of HER catalysts by tailoring the catalyst/support interface.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY, 2017
National Category
Materials Chemistry
Identifiers
urn:nbn:se:uu:diva-326228 (URN)10.1039/c7cp01237c (DOI)000402072100072 ()28492661 (PubMedID)
Funder
Swedish Research Council, 2014-5993
Available from: 2017-07-05 Created: 2017-07-05 Last updated: 2017-07-05Bibliographically approved
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