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The contribution of sulphuric acid to atmospheric particle formation and growth: A comparison between boundary layers in Northern and Central Europe

2005, Fiedler, V., Dal Maso, M., Boy, M., Aufmhoff, H., Hoffmann, J., Schuck, T., Birmili, W., Hanke, M., Uecker, J., Arnold, F., Kulmala, M.

Atmospheric gaseous sulphuric acid was measured and its influence on particle formation and growth was investigated building on aerosol data. The measurements were part of the EU-project QUEST and took place at two different measurement sites in Northern and Central Europe (Hyytiälä, Finland, March-April 2003 and Heidelberg, Germany, March-April 2004). From a comprehensive data set including sulphuric acid, particle number size distributions and meteorological data, particle growth rates, particle formation rates and source rates of condensable vapors were inferred. Growth rates were determined in two different ways, from particle size distributions as well as from a so-called timeshift analysis. Moreover, correlations between sulphuric acid and particle number concentration between 3 and 6 nm were examined and the influence of air masses of different origin was investigated. Measured maximum concentrations of sulphuric acid were in the range from 1x106 to 16x106cm-3. The gaseous sulphuric acid lifetime with respect to condensation on aerosol particles ranged from 2 to 33min in Hyytiälä and from 0.5 to 8 min in Heidelberg. Most calculated values (growth rates, formation rates, vapor source rates) were considerably higher in Central Europe (Heidelberg), due to the more polluted air and higher preexistent aerosol concentrations. Close correlations between H2SO4 and nucleation mode particles (size range: 3-6 nm) were found on most days at both sites. The percentage contribution of sulphuric acid to particle growth was below 10% at both places and to initial growth below 20%. An air mass analysis indicated that at Heidelberg new particles were formed predominantly in air advected from southwesterly directions.

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Huge impact of compressive strain on phase transition temperatures in epitaxial ferroelectric KxNa1-xNbO3 thin films

2019, Von Helden, L., Bogula, L., Janolin, P.-E., Hanke, M., Breuer, T., Schmidbauer, M., Ganschow, S., Schwarzkopf, J.

We present a study in which ferroelectric phase transition temperatures in epitaxial KxNa1-xNbO3 films are altered systematically by choosing different (110)-oriented rare-earth scandate substrates and by variation of the potassium to sodium ratio. Our results prove the capability to continuously shift the ferroelectric-to-ferroelectric transition from the monoclinic MC to orthorhombic c-phase by about 400 °C via the application of anisotropic compressive strain. The phase transition was investigated in detail by monitoring the temperature dependence of ferroelectric domain patterns using piezoresponse force microscopy and upon analyzing structural changes by means of high resolution X-ray diffraction including X-ray reciprocal space mapping. Moreover, the temperature evolution of the effective piezoelectric coefficient d33,f was determined using double beam laser interferometry, which exhibits a significant dependence on the particular ferroelectric phase. © 2019 Author(s).

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Lattice matched Volmer–Weber growth of Fe3Si on GaAs(001) - the influence of the growth rate

2019, Jenichen, B., Cheng, Z., Hanke, M., Herfort, J., Trampert, A.

We investigate the formation of lattice matched single-crystalline Fe3Si/GaAs(001) ferromagnet/semiconductor hybrid structures by Volmer-Weber island growth, starting from the epitaxial growth of isolated Fe3Si islands up to the formation of continuous films as a result of island coalescence. We find coherent defect-free layers exhibiting compositional disorder near the Fe3Si/GaAs - interface for higher growth rates, whereas they are fully ordered for lower growth rates. © 2019 IOP Publishing Ltd.

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Diffraction at GaAs/Fe3Si core/shell nanowires: The formation of nanofacets

2016, Jenichen, B., Hanke, M., Hilse, M., Herfort, J., Trampert, A., Erwin, S.C.

GaAs/Fe3Si core/shell nanowire structures were fabricated by molecular-beam epitaxy on oxidized Si(111) substrates and investigated by synchrotron x-ray diffraction. The surfaces of the Fe3Si shells exhibit nanofacets. These facets consist of well pronounced Fe3Si{111} planes. Density functional theory reveals that the Si-terminated Fe3Si{111} surface has the lowest energy in agreement with the experimental findings. We can analyze the x-ray diffuse scattering and diffraction of the ensemble of nanowires avoiding the signal of the substrate and poly-crystalline films located between the wires. Fe3Si nanofacets cause streaks in the x-ray reciprocal space map rotated by an azimuthal angle of 30° compared with those of bare GaAs nanowires. In the corresponding TEM micrograph the facets are revealed only if the incident electron beam is oriented along [1 1 ̄ 0] in accordance with the x-ray results. Additional maxima in the x-ray scans indicate the onset of chemical reactions between Fe3Si shells and GaAs cores occurring at increased growth temperatures.

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SO2 oxidation products other than H2SO4 as a trigger of new particle formation. Part 2: Comparison of ambient and laboratory measurements, and atmospheric implications

2008, Laaksonen, A., Kulmala, M., Bernd, T., Stratmann, F., Mikkonen, S., Ruuskanen, A., Lehtinen, K.E.J., Dal Maso, M., Aalto, P., Petäjä, T., Riipinen, I., Sihto, S.-L., Janson, R., Arnold, F., Hanke, M., Ücker, J., Umann, B., Sellegri, K., O'Dowd, C.D., Viisanen, Y.

Atmospheric new particle formation is generally thought to occur due to homogeneous or ion-induced nucleation of sulphuric acid. We compare ambient nucleation rates with laboratory data from nucleation experiments involving either sulphuric acid or oxidized SO2. Atmospheric nucleation occurs at H2SO4 concentrations 2–4 orders of magnitude lower than binary or ternary nucleation rates of H2SO4 produced from a liquid reservoir, and atmospheric H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We hypothesize these features to be due to the formation of free HSO5 radicals in pace with H2SO4 during the SO2 oxidation. We suggest that at temperatures above ~250 K these radicals produce nuclei of new aerosols much more efficiently than H2SO4. These nuclei are activated to further growth by H2SO4 and possibly other trace species. However, at lower temperatures the atmospheric relative acidity is high enough for the H2SO4–H2O nucleation to dominate.

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Structural properties of Co2TiSi films on GaAs(001)

2016, Jenichen, B., Herfort, J., Hanke, M., Jahn, U., Kong, X., Dau, M.T., Trampert, A., Kirmse, H., Erwin, S.C.

Co2TiSi films were grown by molecular beam epitaxy on GaAs(001) and analyzed using reflection high-energy electron diffraction, and electron microscopy. In addition, X-ray diffraction was combined with lattice parameter calculations by density functional theory comparing the L21 and B2 structures and considering the influence of non-stoichiometry. Columnar growth is found and attributed to inhomogeneous epitaxial strain from non-random alloying. In films with thicknesses up to 13 nm, these columns may be the origin of perpendicular magnetization with the easy axis perpendicular to the sample surface. We found L21 and B2 ordered regions, however the [Co]/[Ti]-ratio is changing in dependence of the position in the film. The resulting columnar structure is leading to anisotropic B2-ordering with the best order parallel to the axes of the columns.

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Structural investigation of nanocrystalline graphene grown on (6√3 × 6√3)R30°-reconstructed SiC surfaces by molecular beam epitaxy

2013, Schumann, T., Dubslaff, M., Oliveira, M.H., Hanke, M., Fromm, F., Seyller, T., Nemec, L., Blum, V., Scheffler, M., Lopes, J.M.J.

Growth of nanocrystalline graphene films on (6√3 × 6√3)R30°-reconstructed SiC surfaces was achieved by molecular beam epitaxy, enabling the investigation of quasi-homoepitaxial growth. The structural quality of the graphene films, which is investigated by Raman spectroscopy, increases with growth time. X-ray photoelectron spectroscopy proves that the SiC surface reconstruction persists throughout the growth process and that the synthesized films consist of sp2-bonded carbon. Interestingly, grazing incidence x-ray diffraction measurements show that the graphene domains possess one single in-plane orientation, are aligned to the substrate, and offer a noticeably contracted lattice parameter of 2.450 Å. We correlate this contraction with theoretically calculated reference values (all-electron density functional calculations based on the van der Waals corrected Perdew–Burke–Ernzerhof functional) for the lattice parameter contraction induced in ideal, free-standing graphene sheets by: substrate-induced buckling, the edges of limited-size flakes and typical point defects (monovacancies, divacancies, Stone–Wales defects).