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Author Vladimirova, N.V.; Frolov, A.S.; Sanchez-Barriga, J.; Clark, O.J.; Matsui, F.; Usachov, D.Y.; Muntwiler, M.; Callaert, C.; Hadermann, J.; Neudachina, V.S.; Tamm, M.E.; Yashina, L.V.
Title Occupancy of lattice positions probed by X-ray photoelectron diffraction : a case study of tetradymite topological insulators Type A1 Journal article
Year (down) 2023 Publication Surfaces and interfaces Abbreviated Journal
Volume 36 Issue Pages 102516-10
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Occupancy of different structural positions in a crystal lattice often seems to play a key role in material prop-erties. Several experimental techniques have been developed to uncover this issue, all of them being mostly bulk sensitive. However, many materials including topological insulators (TIs), which are among the most intriguing modern materials, are intended to be used in devices as thin films, for which the sublattice occupancy may differ from the bulk. One of the possible approaches to occupancy analysis is X-ray Photoelectron Diffraction (XPD), a structural method in surface science with chemical sensitivity. We applied this method in a case study of Sb2(Te1-xSex)3 mixed crystals, which belong to prototypical TIs. We used high-angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) as a reference method to verify our analysis. We revealed that the XPD data for vacuum cleaved bulk crystals are in excellent agreement with the reference ones. Also, we demonstrate that the anion occupancy near a naturally formed surface can be rather different from that of the bulk. The present results are relevant for a wide range of compositions where the system remains a topological phase, as we ultimately show by probing the transiently occupied topological surface state above the Fermi level by ultrafast photoemission.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000901694900001 Publication Date 2022-11-28
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2468-0230 ISBN Additional Links UA library record; WoS full record
Impact Factor 6.2 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 6.2; 2023 IF: NA
Call Number UA @ admin @ c:irua:193502 Serial 7327
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Author Volykhov, A.A.; Frolov, A.S.; Neudachina, V.S.; Vladimirova, N.V.; Gerber, E.; Callaert, C.; Hadermann, J.; Khmelevsky, N.O.; Knop-Gericke, A.; Sanchez-Barriga, J.; Yashina, L.V.
Title Impact of ordering on the reactivity of mixed crystals of topological insulators with anion substitution: Bi₂SeTe₂ and Sb₂SeTe₂ Type A1 Journal article
Year (down) 2021 Publication Applied Surface Science Abbreviated Journal Appl Surf Sci
Volume 541 Issue Pages 148490
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Three-dimensional topological insulators are exotic materials with unique properties. Tetradymite type binary chalcogenides of bismuth and antimony, as well as their mixed crystals, belong to prototypical TIs. Potential device applications of these materials require in-depth knowledge of their stability in the ambient atmosphere and other media maintained during their processing. Here we investigated the reactivity of mixed crystals with anion substitution, Bi-2(Se1-xTex)(3) and Sb2(Se1-xTex)(3), towards molecular oxygen using both in situ and ex situ X-ray photoelectron spectroscopy. The results indicate that, in contrast to cation substitution, partial substitution of tellurium by selenium atoms leads to anomalously high surface reactivity, which even exceeds that of the most reactive binary constituent. We attribute this effect to anion ordering that essentially modifies the bond geometry, especially the respective bond angles as modeled by DFT.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000608492900003 Publication Date 2020-11-18
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 0169-4332 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 3.387 Times cited Open Access Not_Open_Access
Notes Approved Most recent IF: 3.387
Call Number UA @ admin @ c:irua:176067 Serial 6728
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Author Frolov, A.S.; Sanchez-Barriga, J.; Callaert, C.; Hadermann, J.; Fedorov, A., V; Usachov, D.Y.; Chaika, A.N.; Walls, B.C.; Zhussupbekov, K.; Shvets, I., V.; Muntwiler, M.; Amati, M.; Gregoratti, L.; Varykhalov, A.Y.; Rader, O.; Yashina, L., V.
Title Atomic and electronic structure of a multidomain GeTe crystal Type A1 Journal article
Year (down) 2020 Publication Acs Nano Abbreviated Journal Acs Nano
Volume 14 Issue 12 Pages 16576-16589
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Renewed interest in the ferroelectric semi-conductor germanium telluride was recently triggered by the direct observation of a giant Rashba effect and a 30-year-old dream about a functional spin field-effect transistor. In this respect, all-electrical control of the spin texture in this material in combination with ferroelectric properties at the nanoscale would create advanced functionalities in spintronics and data information processing. Here, we investigate the atomic and electronic properties of GeTe bulk single crystals and their (111) surfaces. We succeeded in growing crystals possessing solely inversion domains of similar to 10 nm thickness parallel to each other. Using HAADF-TEM we observe two types of domain boundaries, one of them being similar in structure to the van der Waals gap in layered materials. This structure is responsible for the formation of surface domains with preferential Te-termination (similar to 68%) as we determined using photoelectron diffraction and XPS. The lateral dimensions of the surface domains are in the range of similar to 10-100 nm, and both Ge- and Te-terminations reveal no reconstruction. Using spin-ARPES we establish an intrinsic quantitative relationship between the spin polarization of pure bulk states and the relative contribution of different terminations, a result that is consistent with a reversal of the spin texture of the bulk Rashba bands for opposite configurations of the ferroelectric polarization within individual nanodomains. Our findings are important for potential applications of ferroelectric Rashba semiconductors in nonvolatile spintronic devices with advanced memory and computing capabilities at the nanoscale.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000603308800022 Publication Date 2020-11-02
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1936-0851 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 17.1 Times cited Open Access OpenAccess
Notes Approved Most recent IF: 17.1; 2020 IF: 13.942
Call Number UA @ admin @ c:irua:175027 Serial 6716
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Author Sirotina, A.P.; Callaert, C.; Volykhov, A.A.; Frolov, A.S.; Sanchez-Barriga, J.; Knop-Gericke, A.; Hadermann, J.; Yashina, L.V.
Title Mechanistic studies of gas reactions with multicomponent solids : what can we learn by combining NAP XPS and atomic resolution STEM/EDX? Type A1 Journal article
Year (down) 2019 Publication The journal of physical chemistry: C : nanomaterials and interfaces Abbreviated Journal J Phys Chem C
Volume 123 Issue 43 Pages 26201-26210
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Abstract Rapid development of experimental techniques has enabled real time studies of solid gas reactions at the level reaching the atomic scale. In the present paper, we focus on a combination of atomic resolution STEM/EDX, which visualizes the reaction zone, and near ambient pressure (NAP) XPS, which collects information for a surface layer of variable thickness under reaction conditions. We compare the behavior of two affined topological insulators, Bi2Te3 and Sb2Te3. We used a simple reaction with molecular oxygen occurring at 298 K, which is of practical importance to avoid material degradation. Despite certain limitations, a combination of in situ XPS and ex situ cross-sectional STEM/EDX allowed us to obtain a self-consistent picture of the solid gas reaction mechanism for oxidation of Sb2Te3 and Bi2Te3 crystals, which includes component redistribution between the oxide and the subsurface layer and Te segregation with formation of a thin ordered layer at the interface. The process is multistep in case of both compounds. At the very beginning of the oxidation process the reactivity is determined by the energy benefit of the corresponding element oxygen bond formation. Further in the oxidation process, the behavior of these two compounds becomes similar and features component redistribution between the oxide and the subsurface layer.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000493865700019 Publication Date 2019-10-03
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1932-7447; 1932-7455 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.536 Times cited Open Access
Notes Approved Most recent IF: 4.536
Call Number UA @ admin @ c:irua:164664 Serial 6310
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Author Sanchez-Barriga, J.; Aguilera, I.; Yashina, L., V; Tsukanova, D.Y.; Freyse, F.; Chaika, A.N.; Callaert, C.; Abakumov, A.M.; Hadermann, J.; Varykhalov, A.; Rienks, E.D.L.; Bihlmayer, G.; Blugel, S.; Rader, O.
Title Anomalous behavior of the electronic structure of (Bi1-xInx)2Se3across the quantum phase transition from topological to trivial insulator Type A1 Journal article
Year (down) 2018 Publication Physical review B Abbreviated Journal
Volume 98 Issue 23 Pages 235110
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract Using spin- and angle-resolved photoemission spectroscopy and relativistic many-body calculations, we investigate the evolution of the electronic structure of (Bi1-xInx)(2)Se-3)(2)Se-3 bulk single crystals around the critical point of the trivial to topological insulator quantum-phase transition. By increasing x, we observe how a surface gap opens at the Dirac point of the initially gapless topological surface state of Bi2Se3, leading to the existence of massive fermions. The surface gap monotonically increases for a wide range of x values across the topological and trivial sides of the quantum-phase transition. By means of photon-energy-dependent measurements, we demonstrate that the gapped surface state survives the inversion of the bulk bands which occurs at a critical point near x = 0.055. The surface state exhibits a nonzero in-plane spin polarization which decays exponentially with increasing x, and which persists in both the topological and trivial insulator phases. Our calculations reveal qualitative agreement with the experimental results all across the quantum-phase transition upon the systematic variation of the spin-orbit coupling strength. A non-time-reversal symmetry-breaking mechanism of bulk-mediated scattering processes that increase with decreasing spin-orbit coupling strength is proposed as explanation.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000452322800003 Publication Date 2018-12-05
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2469-9969; 2469-9950 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited Open Access
Notes Approved no
Call Number UA @ admin @ c:irua:156240 Serial 7462
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Author Volykhov, A.A.; Sanchez-Barriga, J.; Batuk, M.; Callaert, C.; Hadermann, J.; Sirotina, A.P.; Neudachina, V.S.; Belova, A.I.; Vladimirova, N.V.; Tamm, M.E.; Khmelevsky, N.O.; Escudero, C.; Perez-Dieste, V.; Knop-Gericke, A.; Yashina, L.V.
Title Can surface reactivity of mixed crystals be predicted from their counterparts? A case study of (Bi1-xSbx)2Te3 topological insulators Type A1 Journal article
Year (down) 2018 Publication Journal of materials chemistry C : materials for optical and electronic devices Abbreviated Journal J Mater Chem C
Volume 6 Issue 33 Pages 8941-8949
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract The behavior of ternary mixed crystals or solid solutions and its correlation with the properties of their binary constituents is of fundamental interest. Due to their unique potential for application in future information technology, mixed crystals of topological insulators with the spin-locked, gapless states on their surfaces attract huge attention of physicists, chemists and material scientists. (Bi1-xSbx)(2)Te-3 solid solutions are among the best candidates for spintronic applications since the bulk carrier concentration can be tuned by varying x to obtain truly bulk-insulating samples, where the topological surface states largely contribute to the transport and the realization of the surface quantum Hall effect. As this ternary compound will be evidently used in the form of thin-film devices its chemical stability is an important practical issue. Based on the atomic resolution HAADF-TEM and EDX data together with the XPS results obtained both ex situ and in situ, we propose an atomistic picture of the mixed crystal reactivity compared to that of its binary constituents. We find that the surface reactivity is determined by the probability of oxygen attack on the Te-Sb bonds, which is directly proportional to the number of Te atoms bonded to at least one Sb atom. The oxidation mechanism includes formation of an amorphous antimony oxide at the very surface due to Sb diffusion from the first two quintuple layers, electron tunneling from the Fermi level of the crystal to oxygen, oxygen ion diffusion to the crystal, and finally, slow Te oxidation to the +4 oxidation state. The oxide layer thickness is limited by the electron transport, and the overall process resembles the Cabrera-Mott mechanism in metals. These observations are critical not only for current understanding of the chemical reactivity of complex crystals, but also to improve the performance of future spintronic devices based on topological materials.
Address
Corporate Author Thesis
Publisher Place of Publication Editor
Language Wos 000443279300007 Publication Date 2018-07-20
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2050-7526; 2050-7534 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 5.256 Times cited 3 Open Access Not_Open_Access
Notes ; The authors acknowledge financial support within the bilateral program "Russian-German Laboratory at BESSY II''. We thank Helmholtz-Zentrum Berlin for granting access to the beamlines RGBL, UE112-PGM2a and ISISS. Support of ALBA staff during measurements at the CIRCE beamline is gratefully acknowledged. We thank Dr Ivan Bobrikov for support in the XRD measurements and Daria Tsukanova for the participation in crystal preparation and XPS measurements. A. Volykhov thanks RSF (grant 18-73-00248) for financial support. A. I. Belova acknowledges support from the G-RISC Centre of Excellence. The work was supported by Helmholtz Gemeinschaft (Grant No. HRJRG-408) and RFBR (grant 14-03-31518). J. H. and C. C. acknowledge support from the University of Antwerp through the BOF grant 31445. ; Approved Most recent IF: 5.256
Call Number UA @ lucian @ c:irua:153647 Serial 5080
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Author Sanchez-Barriga, J.; Ogorodnikov, I.I.; Kuznetsov, M.V.; Volykhov, A.A.; Matsui, F.; Callaert, C.; Hadermann, J.; Verbitskiy, N.I.; Koch, R.J.; Varykhalov, A.; Rader, O.; Yashina, L.V.
Title Observation of hidden atomic order at the interface between Fe and topological insulator Bi2Te3 Type A1 Journal article
Year (down) 2017 Publication Physical chemistry, chemical physics Abbreviated Journal Phys Chem Chem Phys
Volume 19 Issue 45 Pages 30520-30532
Keywords A1 Journal article; Electron microscopy for materials research (EMAT)
Abstract <script type='text/javascript'>document.write(unpmarked('To realize spintronic devices based on topological insulators (TIs), well-defined interfaces between magnetic metals and TIs are required. Here, we characterize atomically precisely the interface between the 3d transition metal Fe and the TI Bi2Te3 at different stages of its formation. Using photoelectron diffraction and holography, we show that after deposition of up to 3 monolayers Fe on Bi2Te3 at room temperature, the Fe atoms are ordered at the interface despite the surface disorder revealed by our scanning-tunneling microscopy images. We find that Fe occupies two different sites: a hollow adatom deeply relaxed into the Bi2Te3 quintuple layers and an interstitial atom between the third (Te) and fourth (Bi) atomic layers. For both sites, our core-level photoemission spectra and density-functional theory calculations demonstrate simultaneous chemical bonding of Fe to both Te and Bi atoms. We further show that upon deposition of Fe up to a thickness of 20 nm, the Fe atoms penetrate deeper into the bulk forming a 2-5 nm interface layer containing FeTe. In addition, excessive Bi is pushed down into the bulk of Bi2Te3 leading to the formation of septuple layers of Bi3Te4 within a distance of similar to 25 nm from the interface. Controlling the magnetic properties of the complex interface structures revealed by our work will be of critical importance when optimizing the efficiency of spin injection in TI-based devices.'));
Address
Corporate Author Thesis
Publisher Place of Publication Cambridge Editor
Language Wos 000416054400023 Publication Date 2017-10-24
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 1463-9076; 1463-9084 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 4.123 Times cited 4 Open Access OpenAccess
Notes ; The authors acknowledge financial support within the bilateral program “Russian-German Laboratory at BESSY II” and thank Helmholtz Zentrum Berlin for granting access to the beamlines RGBL, UE112-PGM2a and U49-PGM1. The Supercomputing Center of Lomonosov Moscow State University is gratefully acknowledged for granting access to the “Lomonosov” supercomputer. The work was partially supported by DFG priority program SPP 1666, Impuls- und Vernetzungsfonds der Helmholtz-Gemeinschaft (Grant No. HRJRG-408) and Russian Foundation for Basic Research (Grants No. 13-02-91327 and No. 16-29-06410). C. C. acknowledges support from the University of Antwerp through the BOF grant 31445. The authors thank Dr Vera Neudachina, Daria Tsukanova, Dr Elmar Kataev and Dr Maria Batuk for their support during the XPS and TEM experiments. ; Approved Most recent IF: 4.123
Call Number UA @ lucian @ c:irua:147659 Serial 4888
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Author Varykhalov, A.; Marchenko, D.; Sanchez-Barriga, J.; Scholz, M.R.; Verberck, B.; Trauzettel, B.; Wehling, T.O.; Carbone, C.; Rader, O.
Title Intact dirac cones at broken sublattice symmetry : photoemission study of graphene on Ni and Co Type A1 Journal article
Year (down) 2012 Publication Physical review X Abbreviated Journal Phys Rev X
Volume 2 Issue 4 Pages 041017-10
Keywords A1 Journal article; Condensed Matter Theory (CMT)
Abstract The appearance of massless Dirac fermions in graphene requires two equivalent carbon sublattices of trigonal shape. While the generation of an effective mass and a band gap at the Dirac point remains an unresolved problem for freestanding extended graphene, it is well established by breaking translational symmetry by confinement and by breaking sublattice symmetry by interaction with a substrate. One of the strongest sublattice-symmetry-breaking interactions with predicted and measured band gaps ranging from 400 meV to more than 3 eV has been attributed to the interfaces of graphene with Ni and Co, which are also promising spin-filter interfaces. Here, we apply angle-resolved photoemission to epitaxial graphene on Ni (111) and Co(0001) to show the presence of intact Dirac cones 2.8 eV below the Fermi level. Our results challenge the common belief that the breaking of sublattice symmetry by a substrate and the opening of the band gap at the Dirac energy are in a straightforward relation. A simple effective model of a biased bilayer structure composed of graphene and a sublattice-symmetry-broken layer, corroborated by density-functional-theory calculations, demonstrates the general validity of our conclusions.
Address
Corporate Author Thesis
Publisher Place of Publication College Park, Md Editor
Language Wos 000312703200001 Publication Date 2012-12-22
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2160-3308; ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 12.789 Times cited 86 Open Access
Notes ; A. V. acknowledges helpful discussions with N. Sandler. This work was supported by SPP 1459 of the Deutsche Forschungsgemeinschaft. B. V. acknowledges support from the Research Foundation Flanders (FWO-Vlaanderen). B. T. and T. O. W. would like to thank the KITP at Santa Barbara for hospitality during the completion of this work. ; Approved Most recent IF: 12.789; 2012 IF: 6.711
Call Number UA @ lucian @ c:irua:105964 Serial 1677
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