TY - GEN A1 - Tallarida, Massimo A1 - Adelmann, Christoph A1 - Delabie, Annelies A1 - Elshocht, Sven van A1 - Caymax, Matty A1 - Schmeißer, Dieter T1 - III-V/Oxide Interfaces Investigated with Synchrotron Radiation Photoemission Spectroscopy T2 - ECS Transactions N2 - We used synchrotron radiation photoemission spectroscopy (SR-PES) to investigate the surface of GaAs and other III-V semiconductors after tri-methyl-aluminum (TMA) pulses performed at 250{degree sign}C. We observed the removal of native oxide and the growth of Al-oxide upon measuring the As3d, Ga3d, Al2p and VB spectra. After seven TMA pulses we performed one water pulse. As3d and Ga3d peaks showed almost no lineshape change, but a decrease of intensity due to the water adsorption. The valence band shows a change in the secondary electron cut-off and the decrease of work function. We conclude that water mostly adsorbs molecularly and induces the work function decrease. The molecular absorption of water indicates that the seven TMA pulses produce a passivated surface only partially terminated with OH groups. KW - Interfaces KW - III/V KW - Synchrotron Photoemission Spectroscopy Y1 - 2013 U6 - https://doi.org/10.1149/05004.0123ecst SN - 1938-6737 VL - 50 IS - 4 SP - 123 EP - 128 ER - TY - GEN A1 - Müller, Klaus A1 - Fleige, Michael A1 - Rachow, Fabian A1 - Schmeißer, Dieter T1 - Sabatier based CO2-methanation of flue gas emitted by conventional power plants T2 - Energy Procedia N2 - The hydrogenation CO2+ 4H2 ->CH4 + 2H2O discovered by Paul Sabatier nowadays is discussed as "Power-to-approach" to utilize excess energy from renewable electricity generation. In a laboratory scale, we investigate the Sabatier process in a simulated flue gas atmosphere of conventional base load power plants. The reaction is investigated with regard to conversion rates, yield, selectivity and long-term stability. Using a catalyst based on nickel,we extract selectivities near 100% with a conversion around 85%. Beside the influence of oxygen, we investigate further typical contaminations like NO2 and SO2. KW - Power to gas KW - CO2 -Methanation KW - Sabatier-reaction KW - flue gas Y1 - 2013 U6 - https://doi.org/10.1016/j.egypro.2013.08.028 SN - 1876-6102 VL - 40 SP - 240 EP - 248 ER - TY - CHAP A1 - Mai, Andreas A1 - Dauderstädt, Ulrike A1 - Pahner, D. A1 - Krellmann, M. A1 - Schmeißer, Dieter A1 - Wagner, M. T1 - In situ determination of laser induced degradation of micro-mirror arrays T2 - International Students and Young Scientists Workshop Photonics and Microsystems, Cottbus, Germany, 8 - 10 June 2011 N2 - The Fraunhofer Institute for Photonic Microsystems (Fraunhofer IPMS) develops spatial light modulators (SLMs) based on arrays of tiltable micro mirrors on a semiconductor chip. Typical applications are pattern generation for deepUV-laser mask writing or structured illumination in microscopy. Development and optimization of such SLMs requires detailed knowledge of the device behaviour under operating conditions. Here, the flatness of each single mirror effects the image resolution and contrast of the generated pattern and is amongst others a characteristic property of SLMs. In this context a surface topography measurement under laser exposure (in situ) was designed. The interferometric setup uses the phase-shift principle and allows a resolution in z-direction in the single-digit nanometer range. During irradiation with UV-laser light at 248 nm (KrF) and energy densities of up to 20 mJ/cm2 the change in single micro-mirrors topography was detected in situ. Measurementswith varying pulse energies were carried out to identify an impacton the device performance. In general, the setup is neither limited to a specific illumination wavelength nor to micro-mirrors as structures under test. KW - micro-mirror arrays KW - laser induced degradation Y1 - 2011 SN - 978-1-4577-1651-5 U6 - https://doi.org/10.1109/STYSW.2011.6155850 SP - 84 EP - 88 PB - IEEE CY - Piscataway, NJ ER - TY - GEN A1 - Barreca, Davide A1 - Carraro, Giorgio A1 - Gasparotto, Alberto A1 - Maccato, Chiara A1 - Rossi, Francesca A1 - Salviati, Giancarlo A1 - Tallarida, Massimo A1 - Das, Chittaranjan A1 - Fresno, Fernando A1 - Korte, Dorota A1 - Štangar, Urška Lavrenčič A1 - Franko, Mladen A1 - Schmeißer, Dieter T1 - Surface Functionalization of Nanostructured Fe2O3 Polymorphs: From Design to Light-Activated Applications T2 - ACS Applied Materials & Interfaces N2 - Nanostructured iron(III) oxide deposits are grown by chemical vapor deposition (CVD) at 400−500 °C on Si(100) substrates from Fe(hfa)2TMEDA (hfa = 1,1,1,5,5,5-hexafluoro-2,4-pentanedionate; TMEDA = N,N,N′N′-tetramethylethylenediamine), yielding the selective formation of α-Fe2O3or the scarcely studiedε-Fe2O3 polymorphs under suitably optimized preparative conditions. By using Ti(OPr i)4(OPri= iso-propoxy) and water asatomic layer deposition (ALD) precursors, we subsequently functionalized the obtained materials at moderate temperatures (<300°C) by an ultrathin titanomagnetite (Fe3−xTixO4) overlayer. An extensive multitechnique character-ization, aimed at elucidating the system structure, morphology, composition and optical properties, evidenced that the photoactivated hydrophilic and photocatalytic behavior of the synthesized materials is dependent both on iron oxide phase composition and ALD surface modification. The proposed CVD/ALD hybrid synthetic approach candidates itself as a powerful tool for a variety of applications where semiconductor-based nanoarchitectures can benefit from the coupling with an ad hoc surface layer. KW - chemical vapor deposition KW - atomic layer deposition KW - iron oxide KW - titanomagnetite KW - photoactivated properties Y1 - 2013 U6 - https://doi.org/10.1021/am401475g SN - 1944-8252 VL - 5 IS - 15 SP - 7130 EP - 7138 ER - TY - GEN A1 - Adelmann, Christoph A1 - Cuypers, Daniel A1 - Tallarida, Massimo A1 - Rodriguez, Leonard A1 - De Clercq, Astrid A1 - Friedrich, Daniel A1 - Conard, Thierry A1 - Delabie, Annelies A1 - Seo, Jin Won A1 - Locquet, Jean-Pierre A1 - De Gendt, Stefan A1 - Schmeißer, Dieter A1 - Elshocht, Sven van A1 - Caymax, Matty T1 - Surface Chemistry and Interface Formation during the Atomic Layer Deposition of Alumina from Trimethylaluminum and Water on Indium Phosphide T2 - Chemistry of Materials N2 - The surface chemistry and the interface formation during the initial stages of the atomic layer deposition (ALD) of Al2O3 from trimethylaluminum (TMA) and H2O on InP(100)were studied by synchrotron radiation photoemission spectroscopy and scanning tunneling microscopy. The effect of the ex situ surface cleaning by either H2SO4 or (NH4)2S was examined. It is shown that the native oxide on the InP surface consisted mainly of indium hydrogen phosphates with a P enrichment at the interface with InP. After a (NH4)2S treatment, S was present on the surface as a sulfide in both surface and subsurface sites. Exposure to TMA led to the formation of a thin AlPO4 layer, irrespective of the surface cleaning. The surface Fermi level of p-type InP was found to be pinned close to midgap after H2SO4 cleaning and moved only slightly further toward the conduction band edge upon TMA exposure, indicating that the AlPO4/InP interface was rather defective. (NH4)2S passivation led to a Fermi level position of p-type InP close to the conduction band edge. Hence, the InP surface was weakly inverted, which can be attributed to surface doping by S donors. TMA exposure was found to remove surface S, which was accompanied by a shift of the Fermi level to midgap, consistent with the removal of (part of) the S donors in combination with a defective AlPO4/InP interface. Further TMA/H2O ALD did not lead to any detectable changes of the AlPO4/InP interface and suggested simple overgrowth with Al2O3. Y1 - 2013 U6 - https://doi.org/10.1021/cm304070h SN - 1520-5002 VL - 25 IS - 7 SP - 1078 EP - 1091 ER - TY - GEN A1 - Rossi, Francesca A1 - Fabbri, Filippo A1 - Tallarida, Massimo A1 - Schmeißer, Dieter A1 - Modreanu, Mircea A1 - Attolini, Giovanni A1 - Salviati, Giancarlo T1 - Structural and luminescence properties of HfO2 nanocrystals grown by atomic layer deposition on SiC/SiO2 core/shell nanowires T2 - Scripta Materialia N2 - In this work we report the morphological, structural and luminescence properties of HfO2 nanocrystals grown on the surface of SiC/SiO2 core/shell nanowires by atomic layer deposition. All the studies are carried out in comparison with HfO2 nanocrystal aggregates grown on planar oxidized silicon substrates. The structural analyses reveal that HfO2has monoclinic structure with dif-ferent orientations. The cathodoluminescence emission shows the main components at 2.7 and 2.3 eV, deeply influenced by the arrangement and aggregation of the nanocrystals. KW - Silicon carbide KW - Silicon dioxide KW - Nanowires KW - Hafnium oxide KW - Nanocrystals Y1 - 2013 U6 - https://doi.org/10.1016/j.scriptamat.2013.08.017 SN - 1359-6462 VL - 69 IS - 10 SP - 744 EP - 747 ER - TY - GEN A1 - Haeberle, Jörg A1 - Henkel, Karsten A1 - Gargouri, Hassan A1 - Naumann, Franziska A1 - Gruska, Bernd A1 - Arens, Michael A1 - Tallarida, Massimo A1 - Schmeißer, Dieter T1 - Ellipsometry and XPS comparative studies of thermal and plasma enhanced atomic layer deposited Al2O3-films T2 - Beilstein Journal of Nanotechnology N2 - We report on results on the preparation of thin (<100 nm) aluminum oxide (Al2O3) films on silicon substrates using thermal atomic layer deposition (T-ALD) and plasma enhanced atomic layer deposition (PE-ALD) in the SENTECH SI ALD LL system. The T-ALD Al2O3layers were deposited at 200 °C, for the PE-ALD films we varied the substrate temperature range between room temperature (rt) and 200 °C. We show data from spectroscopic ellipsometry (thickness, refractive index, growth rate) over 4” wafers and correlatethem to X-ray photoelectron spectroscopy (XPS) results. The 200°C T-ALD and PE-ALD processes yield films with similar refractive indices and with oxygen to aluminum elemental ratios very close to the stoichiometric value of 1.5. However, in both also fragments of the precursor are integrated into the film. The PE-ALD films show an increased growth rate and lower carbon contaminations. Reducing the deposition temperature down to rt leads to a higher content of carbon and CH-species. We also find a decrease of the refractive index and of the oxygen to aluminum elemental ratio as well as an increase of the growth rate whereas the homogeneity of the film growth is not influenced significantly. Initial state energy shifts in all PE-ALD samples are observed which we attribute to a net negative charge within the films. KW - Al2O3 KW - ALD KW - ellipsometry KW - PE-ALD KW - XPS Y1 - 2013 U6 - https://doi.org/10.3762/bjnano.4.83 SN - 2190-4286 VL - 2013 IS - 4 SP - 732 EP - 742 ER - TY - CHAP A1 - Cuypers, Daniel A1 - Dorp, Dennis H. von A1 - Tallarida, Massimo A1 - Brizzi, Simone A1 - Rodriguez, Leonard A1 - Conard, Thierry A1 - Arnauts, Sophia A1 - Schmeißer, Dieter A1 - Adelmann, Christoph A1 - De Gendt, Stefan T1 - Study of InP Surfaces After Wet Chemical Treatments T2 - Meeting Abstracts-Electrochemical Society, San Francisco, 2013 KW - Synchrotron Radiation Photoelectron Spectroscopy KW - InP KW - Wet chemical treatment Y1 - 2013 UR - http://ma.ecsdl.org/content/MA2013-02/30/2132.full.pdf+html N1 - MA2013-02(30) SP - S. 2132 PB - The Electrochemical Society ER - TY - GEN A1 - Cuypers, Daniel A1 - Dorp, Dennis H. von A1 - Tallarida, Massimo A1 - Brizzi, Simone A1 - Rodriguez, Leonard A1 - Conard, Thierry A1 - Arnauts, Sophia A1 - Schmeißer, Dieter A1 - Adelmann, Christoph A1 - De Gendt, Stefan T1 - Study of InP Surfaces after Wet Chemical Treatments T2 - ECS Transactions N2 - In this work synchrotron radiation photoemission spectroscopy (SRPES) is used to study InP surfaces after different wet chemical treatments. All results are compared to a typical fingerprint of surface components present on an as received InP sample. It is shown that acidified (HCl and H₂SO₄) treatments efficiently remove the native phosphate, although components like Pᴼ, Inᴼ and P(2±∆)+ remain present. In alkaline solution (NH₄OH) oxide remains present at the surface. As an alternative treatment, the immersion into (NH₄)₂S was studied. This passivation treatment results in fewer surface components which suggests that a higher quality surface is obtained. KW - Synchrotron Radiation Photoelectron Spectroscopy KW - InP KW - Wet chemical treatment Y1 - 2013 U6 - https://doi.org/10.1149/05806.0297ecst SN - 1938-6737 SN - 1938-5862 VL - 58 IS - 6 SP - 297 EP - 303 ER - TY - GEN A1 - Cuypers, Daniel A1 - Dorp, Dennis H. von A1 - Tallarida, Massimo A1 - Brizzi, Simone A1 - Conard, Thierry A1 - Rodriguez, Leonard A1 - Mees, M. A1 - Arnauts, Sophia A1 - Schmeißer, Dieter A1 - Adelmann, Christoph A1 - De Gendt, Stefan T1 - Study of InP Surfaces after Wet Chemical Treatments T2 - ECS Journal of Solid State Science and Technology N2 - The influence of different wet chemical treatments (HCl, H₂SO₄, NH₄OH) on the composition of InP surfaces is studied by using synchrotron radiation photoemission spectroscopy (SRPES). It is shown that a significant amount of oxide remains present after immersion in a NH₄OH solution which is ascribed to the insolubility of In³⁺ at higher pH values. Acidic treatments efficiently remove the native oxide, although components like Pᴼ, Inᴼ and P(2±Δ)+ suboxides are observed. Alternatively, the influence of a passivation step in (NH₄)₂S solution on the surface composition was investigated. The InP surface after immersion into (NH₄)₂S results in fewer surface components, without detection of Pᴼ and P(2±Δ)+ suboxides. Finally, slight etching of InP surfaces in HCl/H₂O₂ solution followed by a native oxide removal step, showed no significant effect on the surface composition. KW - Synchrotron Radiation Photoelectron Spectroscopy KW - Scanning Tunneling Microscopy KW - InP KW - Wet chemical treatment Y1 - 2014 U6 - https://doi.org/10.1149/2.005401jss SN - 2162-8777 SN - 2162-8769 VL - 3 IS - 1 SP - N3016 EP - N3022 ER - TY - GEN A1 - Müller, Klaus A1 - Städter, Matthias A1 - Rachow, Fabian A1 - Hoffmannbeck, David A1 - Schmeißer, Dieter T1 - Sabatier-based CO2-methanation by catalytic conversion T2 - Environmental Earth Sciences N2 - The catalytic conversion of CO2is an important component for the reintegration of secondary products like CO2 or H2 into the energy supply. An example is the "power to gas’" concept with a conversion of CO2 into CH4. The CO2 is transferred into a carrier of chemical energy, with the possibility to feed the produced CH4 into the existing network of natural gas. At temperatures of around 350 °C, hydrogenation of CO2 to CH4 is possible by the Sabatier reaction CO2+4H2->CH4+H2O. One prerequisite for efficient kinetics of the Sabatier reaction is the application and optimization of catalysts. The focus of catalyst development is given to their performance under the conditions to be expected in the special application. As a part of the project Geoenergy-Research (GeoEn), we address questions related to the catalytic utilization of CO2 produced in the course of the oxyfuel combustion of lignite. In this contribution, we report on the experimental setup in laboratory scale, which enables an advanced characterization of the catalytic performance, including thermodesorption measurements at atmospheric pressure in order to determine the amount of adsorbed CO2 under real conditions. We also show data for activation energies, the catalytic performance as function of temperature and the long time stability of a commercial Ru-based catalyst. KW - CO2 KW - Sabatier reaction KW - Catalysis KW - RuO2 Y1 - 2013 U6 - https://doi.org/10.1007/s12665-013-2609-3 SN - 1866-6280 VL - 70 IS - 8 SP - 3771 EP - 3778 ER - TY - GEN A1 - Das, Chittaranjan A1 - Tallarida, Massimo A1 - Schmeißer, Dieter T1 - Linear dichroism in ALD layers of TiO₂ T2 - Environmental Earth Sciences N2 - We prepare TiO₂film by ALD and study their electronic properties by soft X-ray absorption spectroscopy (XAS) and photoelectron spectroscopy. We focus on XAS and X-ray linear dichroism to indentify band onset and learn about local distortion of the Ti–O octahedral atomic and about defects which cause Ti-based electronic states within the band gap. KW - Anatase KW - Dichroism KW - Amorphous Y1 - 2013 U6 - https://doi.org/10.1007/s12665-013-2836-7 SN - 1866-6280 VL - 70 IS - 8 SP - 3785 EP - 3795 ER - TY - GEN A1 - Städter, Matthias A1 - Müller, Klaus A1 - Rachow, Fabian A1 - Richter, Matthias A1 - Schmeißer, Dieter T1 - Ambient pressure thermal desorption spectroscopy (AP-TDS) of NiO/SiO2 catalysts T2 - Environmental Earth Sciences N2 - The Sabatier reaction is a key process in the "power-to-gas" application which is considered to con-tribute to future chemical energy storage systems. In this contribution we focus on the catalytic active sites of a NiO catalyst supported on SiO2(NiO/SiO2) which is commonly used in the Sabatier reaction. A novel technique for the characterization of the active sites is presented and dis-cussed using thermal desorption spectroscopy at ambient pressure. This analytical tool is operated under reaction conditions and allows element specific measurements during the catalytic process of CO2 reforming towards methane. Beside the desorption experiments, XPS and XAS measurements of pristine and catalytically used samples are performed to determine the influence of the Sabatier reaction conditions on the surface structure of the catalyst. KW - CO2 KW - NiO KW - TDS KW - XAS KW - XPS Y1 - 2013 U6 - https://doi.org/10.1007/s12665-013-2835-8 SN - 1866-6280 VL - 70 IS - 8 SP - 3779 EP - 3784 ER - TY - GEN A1 - Scheck-Wenderoth, Magdalena A1 - Schmeißer, Dieter A1 - Mutti, Maria A1 - Kolditz, Olaf A1 - Huenges, Ernst A1 - Schultz, Hans-Martin A1 - Liebscher, Axel A1 - Bock, Michaela T1 - Geoenergy: new concepts for utilization of geo-reservoirs as potential energy sources T2 - Environmental Earth Sciences KW - Geothermal technologies KW - capturing and storing and utilizing CO2 KW - hydraulic fracturing Y1 - 2013 U6 - https://doi.org/10.1007/s12665-013-2877-y SN - 1866-6280 VL - 70 IS - 8 SP - 3427 EP - 3431 ER - TY - GEN A1 - Gerlich, Lukas A1 - Ohsiek, Susanne A1 - Klein, Christoph A1 - Geiß, Mario A1 - Friedemann, Michael A1 - Kücher, Peter A1 - Schmeißer, Dieter T1 - Interface engineering for the TaN/Ta barrier film deposition process to control Ta-crystal growth T2 - Microelectronic Engineering N2 - As a consequence of device shrinking the resistivity of the widely used TaN/Ta double barrier layer becomes an increasingly important parameter for device speed beyond the 32 nm technology node. In this study we describe the optimization of the deposition of TaN/Ta stacks in such a way that tantalum nitride layer thickness is minimized and tantalum grows in the favorable conducting alpha-phase. In the first part of the study we usedin situ ARXPS to investigate the growth of different tantalum nitride layers on SiO2 and SiOCH as a function of deposition time, nitrogen flow and deposition power. In the second part we analyzed the crystalline phase of a 20 nm thick tantalum layer deposited on top of the same series of tantalum nitride layers characterized in the growth study. The main findings are the appearance of tan-talum carbide and tantalum silicide as interface species for the deposition on SiOCH and only tantalum silicide for the deposition on SiO2. We found that alpha-tantalum grows preferably on tantalum carbide and nitrogen rich intermediate layers whereas silicide at the interface promotes the growth of beta-tantalum. To verify these findings we studied two additional modifications of the interface. A lower bias power for a deposition of tantalum nitride on SiO2 was used to confirm the role of tantalum silicide and a thermal treatment of a thin tantalum layer on SiOCH was applied to confirm the role of tantalum carbide. Finally, the contact resistance in via chains on patterned wafers for four selected processes showed the same trends as the sheet resistance of the corresponding barrier films on blanket wafer experiments. KW - Tantalum KW - in situ XPS KW - Ta-phase KW - TaNx KW - Barrier KW - Interface Y1 - 2013 U6 - https://doi.org/10.1016/j.mee.2013.01.017 VL - Vol. 106 SP - 63 EP - 68 ER - TY - GEN A1 - Henkel, Karsten A1 - Gargouri, Hassan A1 - Gruska, Bernd A1 - Arens, Michael A1 - Tallarida, Massimo A1 - Schmeißer, Dieter T1 - Capacitance and conductance versus voltage characterization of Al2O3 layers prepared by PE-ALD at 25°C ≤ T ≤ 200°C T2 - Journal of Vacuum Science and Technology A N2 - In this work, plasma enhanced atomic layer deposited (PE-ALD) samples were prepared at substrate temperatures in the range between room temperature (RT) and 200 °C and investigated by capacitance–voltage and conductance–voltage recordings. The measurements are compared to standard thermal atomic layer deposition (T-ALD) at 200 °C. Very low interface state density (D it) ~1011 eV−1 cm−2 could be achieved for the PE-ALD process at 200 °C substrate temperature after postdeposition anneal (PDA) in forming gas at 450 °C. The PDA works very effectively for both the PE-ALD and T-ALD at 200 °C substrate temperature delivering also similar values of negative fixed charge density (N fix) around −2.5 × 1012 cm−2. At the substrate temperature of 150 °C, highest N fix (−2.9 × 1012 cm−2) and moderate D it (2.7 × 1011 eV−1 cm−2) values were observed. The as deposited PE-ALD layer at RT shows both low D it in the range of (1 to 3) × 1011 eV−1 cm−2 and low N fix (−4.4 × 1011 cm−2) at the same time. The dependencies of N fix, D it, and relative permittivity on the substrate temperatures and its adjustability are discussed. KW - Atomic layer deposition (ALD) KW - Al2O3 KW - dielectric properties KW - interface state density KW - fixed oxide charge KW - permittivity Y1 - 2014 UR - http://link.aip.org/link/?JVA/32/01A107&aemail=author U6 - https://doi.org/10.1116/1.4831897 VL - 1 IS - 32 SP - 01A107-1 EP - 01A107-10 ER - TY - GEN A1 - Richter, Matthias A1 - Starke, Ulrich A1 - Schmeißer, Dieter T1 - Multiple Auger processes in Graphene T2 - Journal of Electron Spectroscopy and Related Phenomena N2 - Resonant Auger decay processes have been studied by resonant photoemission spectroscopy (resPES) and X-ray absorption spectroscopy (XAS) in Graphene systems. The pi*-resonance is used to identify the degree of localization of the lowest pi*-orbitals in the conduction band. Localization and lifetime of the photo-excited intermediate state cause the formation of multiple Auger processes. For the Graphene systems we identify two novel Auger decay combinations with a four hole final state: the (S+S) and the(S+S)* decay. We demonstrate that these processes are sensitive for interlayer coupling and interactions with the metallic free electrons of the substrate. KW - Graphene KW - X-Ray absorption spectroscopy KW - XAS KW - resonant photoemission spectroscopy KW - resPES KW - multiple hole Auger Y1 - 2014 U6 - https://doi.org/10.1016/j.elspec.2013.12.009 SN - 0368-2048 IS - Vol. 192 SP - 1 EP - 6 ER - TY - GEN A1 - Tallarida, Massimo A1 - Das, Chittaranjan A1 - Schmeißer, Dieter T1 - Quantum size effects in TiO2 thin films grown by atomic layer deposition T2 - Beilstein Journal of Nanotechnology N2 - We study the atomic layer deposition of TiO2 by means of X-ray absorption spectroscopy. The Ti precursor, titanium isopropoxide, was used in combination with H2O on Si/SiO2 substrates that were heated at 200 °C. The low growth rate (0.15 Å/cycle) and the in situ characterization permitted to follow changes in the electronic structure of TiO2 in the sub-nanometer range, which are influenced by quantum size effects. The modified electronic properties may play an important role in charge carrier transport and separation, and increase the efficiency of energy conversion systems. KW - atomic layer deposition (ALD) KW - charge transfer multiplet KW - covalency KW - energy conversion KW - quantum size effects KW - titanium dioxide (TiO2) KW - water splitting KW - X-ray absorption spectroscopy (XAS) Y1 - 2014 U6 - https://doi.org/10.3762/bjnano.5.7 SN - 2190-4286 IS - 5 SP - 77 EP - 82 ER - TY - GEN A1 - Richter, Matthias A1 - Friedrich, Daniel A1 - Schmeißer, Dieter T1 - Interlayer-exciton mediated three-hole-Auger-decay in the pi-band of highly oriented pyrolytic graphite T2 - Physica E N2 - Resonant photoemission spectroscopy(resPES) is used to probe the occupied pi- and unoccupied pi*-bands of carbon thin films with particular focus on the Auger decay. Highly Oriented Pyrolytic Graphite (HOPG) is studied at the C1s edge. We find strong resonant features at 285.5 eV and 292 eV in the resPES diagram. The normal two-hole Auger decay proceeds under constant kinetic energy (451)only in the sigma*-region. In the pi*-region, however, it proceeds under 67.5° in terms of a Ebind(w) diagram. We attribute this to a multiple Auger decay with a net three hole final state. For this novel decay process we propose a model.We discuss the long lifetime of the first resonant excitation and conclude that it arises from the strong excitonic character of the first resonant state. We use HOPG as a reference system and suggest that this novel process is a tool to identify interlayer–substrate interaction of the carbon layers involved. KW - resonant excitation KW - three hole Auger decay KW - X-ray photoelectron spectroscopy KW - HOPG Y1 - 2014 U6 - https://doi.org/10.1016/j.physe.2013.01.015 SN - 1386-9477 VL - Vol. 56 SP - 441 EP - 446 ER - TY - GEN A1 - Haeberle, Jörg A1 - Richter, Matthias A1 - Galazka, Zbigniew A1 - Janowitz, Christoph A1 - Schmeißer, Dieter T1 - Resonant Photoemission at the O1s threshold to characterize In2O3 single crystals T2 - Thin Solid Films N2 - We report on spectroscopic investigations on In2O3 single crystals. We focus on the detailed analysis of the O1s resonance profile by resonant photoelectron spectroscopy. We analyze the electronic structure and assign the O2p to build the valence band and both, O2p and In5s5p states to contribute to the conduction band (CB). We determine the partial density of states for the valence and CBs and find a strong hybridization of O2p and In5s states. This is deduced from constant final state spectra on the O-KLL-Auger over the O K-edge and In M4,5-edge and a comparison to the corresponding X-ray absorption spectroscopy data.We also identify several types of defects. A broad band of oxygen derived defects is identified that extends throughout the gap. These are attributed to small polarons which cause an anti-resonance in the valence states around the O1s threshold. In addition, a separate Auger decay at resonance indicates the existence of localized charge transfer states which involves localized In5s5p states. KW - In2O3 KW - TCO KW - X-ray spectroscopy KW - Small polaron KW - Charge transfer Y1 - 2014 U6 - https://doi.org/10.1016/j.tsf.2013.03.036 SN - 0040-6090 SN - 1879-2731 VL - 2014 IS - 555 SP - 53 EP - 56 ER - TY - GEN A1 - Kramm, Ulrike Ingrid A1 - Herrmann-Geppert, Iris A1 - Fiechter, Sebastian A1 - Zehl, Gerald A1 - Zizak, Ivo A1 - Dorbandt, Iris A1 - Schmeißer, Dieter A1 - Bogdanoff, Peter T1 - Effect of iron carbide formation on the number of active sites in Fe-N-C catalysts for the oxygen reduction reaction in acidic media T2 - Journals of materials chemistry A KW - Oxygen reduction reaction (ORR) KW - Fe-N-C catalyst KW - acidic media KW - high-temperature X-ray diffraction (HT-XRD) KW - thermogravimetry coupled with mass-spectroscopy (TG-MS) Y1 - 2014 U6 - https://doi.org/10.1039/c3ta13821f SN - 2050-7488 SN - 2050-7496 IS - 8 SP - 2663 EP - 2670 ER - TY - GEN A1 - Kramm, Ulrike Ingrid A1 - Lefèvre, Michel A1 - Larouche, Nicholas A1 - Schmeißer, Dieter A1 - Dodelet, Jean-Pol T1 - Correlations between Mass Activity and Physicochemical Properties of Fe/N/C Catalysts for the ORR in PEM Fuel Cell via 57 Fe Mössbauer Spectroscopy and Other Techniques T2 - Journal of the American Chemica Society N2 - The aim of this work is to clarify the origin of the enhanced PEM-FC performance of catalysts prepared by the procedures described in Science 2009, 324, 71 and Nat. Commun. 2011, 2, 416. Catalysts were characterized after a first heat treatment in argon at 1050 °C (Ar) and a second heat treatment in ammonia at 950 °C (Ar + NH3). For the NC catalysts a variation of the nitrogen precursor was also implemented. 57Fe Mössbauer spectroscopy, X-ray photoelectron spectroscopy, neutron activation analysis, and N2 sorption measurements were used to characterize all catalysts. The results were correlated to the mass activity of these catalysts measured at 0.8 V in H2/O2 PEM-FC. It was found that all catalysts contain the same FeN4-like species already found in INRS Standard (Phys. Chem. Chem. Phys. 2012, 14, 11673). Among all FeN4-like species, only D1 sites, assigned to FeN4/C, and D3, assigned to N-FeN2+2 /C sites, were active for the oxygen reduction reaction (ORR). The difference between INRS Standard and the new catalysts is simply that there are many more D1 and D3 sites available in the new catalysts. All (Ar + NH3)-type catalysts have a much larger porosity than Ar-type catalysts, while the maximum number of their active sites is only slightly larger after a second heat treatment in NH3. The large difference in activity between the Ar-type catalysts and the Ar + NH3 ones stems from the availability of the sites to perform ORR, as many sites of the Ar-type catalysts are secluded in the material, while they are available at the surface of the Ar + NH3-type catalysts. KW - Fe-N-C catalyst KW - 57 Fe Mössbauer Spectroscopy KW - X-ray photo-electron spectroscopy KW - neutron activation analysis KW - nitrogen sorption measurements KW - oxygen reduction reaction (ORR) KW - PEM Fuel Cell Y1 - 2014 U6 - https://doi.org/10.1021/ja410076f SN - 0002-7863 SN - 1520-5126 VL - 136 IS - 3 SP - 978 EP - 985 ER - TY - GEN A1 - Adelmann, Christoph A1 - Schram, Tom A1 - Chew, Soon Aik A1 - Woicik, J. C. A1 - Brizzi, Simone A1 - Tallarida, Massimo A1 - Schmeißer, Dieter A1 - Horiguchi, Naoto A1 - Elshocht, Sven van A1 - Ragnarsson, Lars-Åke T1 - On the scalability of doped hafnia thin films T2 - Applied Physics Letters N2 - The scaling behavior of Gd- and Al-doped HfO2 films as gate dielectrics in metal-oxide-semiconductor (MOS) capacitors was studied. For equivalent oxide thicknesses (EOTs) in the range of 10 Å, crystallized Gd:HfO2 showed higher leakage current densities than crystallized Al:HfO2, with undoped HfO2 in between. Ultimately, the scalability of Al:HfO2 was limited by the ability to crystallize the films at a given thermal budget. As a result, for post-deposition annealing at 800 °C, the EOT of Al:HfO2 based MOS capacitors was limited to ∼8 Å. However, for such an EOT, leakage current densities were reduced by about 100× with respect to HfO2. This demonstrates the high potential of Al:HfO2 for low-standby-power MOS devices. KW - scalability KW - hafnia thin films KW - Al:HfO2 KW - Gd:HfO2 KW - EXAFS KW - equivalent oxide thickness (EOT) KW - leakage current KW - X-ray absorption spectroscopy (XAS) Y1 - 2014 U6 - https://doi.org/10.1063/1.4870075 SN - 0003-6951 SN - 1077-3118 IS - 104 SP - 122906-1 EP - 122906-4 ER -