@inproceedings{TallaridaMichlingDasetal., author = {Tallarida, Massimo and Michling, Marcel and Das, Chittaranjan and Friedrich, Daniel and St{\"a}dter, Matthias and Schmeißer, Dieter}, title = {Role of substrate chemistry in ALD revealed by in-situ techniques}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {We show recent results of our in-situ investigations where the role of substrate chemistry in ALD is outlined. While the usual strategy to develop new properties of ALD films is to find new precursors or new procedures, the influence of substrate chemistry on the growth properties of ALD films has been often underestimated. This has principally a technical reason, as the usual characterization methods (QMS, FTIR, ellipsometry) are only weakly sensitive to the substrate, and a characterization of substrates before ALD is often not possible. Thanks to the use of in-situ characterization methods, including photoemission and X-ray absorption spectroscopy with synchrotron radiation, we are able to determine chemical properties of substrates before ALD and after either half or complete ALD cycles. The substrate chemistry influences the standard Al2O3 ALD with TMA and water [1,2], as well as the TiO2 ALD with TTIP and either water, O2 or O2-plasma. [1] M. Tallarida, K. Kukli, M. Michling, M. Ritala, M. Leskel{\"a} and D. Schmeisser, Chem. Mater. 23, 3159 (2011); [2] M. Tallarida, C. Adelmann, A. Delabie, S. van Elshocht, M. Caymax, and D. Schmeisser, Appl. Phys. Lett. 92, 042906 (2011).}, language = {en} } @inproceedings{FischerRohrbeckWehneretal., author = {Fischer, Christian B. and Rohrbeck, Magdalena and Wehner, Stefan and Richter, Matthias and Schmeißer, Dieter}, title = {Diamond-Like Carbon Coatings on Selected Plastic Materials}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {The manufacturing of synthetic materials and their wide range of use for daily life is accompanied by essential requirements. Besides the basic performance of materials such as flexibility, elasticity, fracture strength and chemical resistance, further determinants are long term stability or biocompatibility. To overcome mismatches in surface characteristics of optimal parent material they can be customized for their intended use resulting in suitable coatings for profitable applications. The determining factor for such modifications is the preservation of basic material performance in addition to the benefit of further advantages like changed adhesive, improved repellent or antibacterial behavior. Protective coatings of selected plastic materials have been realized by depositing a few layers of diamond-like carbon (DLC). The assembly of soft plastic material and robust DLC coating is important for the resulting material characteristics. The detailed understanding of materials interphasing between these unequal materials and the conjunction of carbon centers in chemically different neighborhood is part of the presented work. Results will be transferable to other plastic materials with diverse needs, e.g. energy storage devices, water treatments and coatings for everyday commodities or industrial parts.}, language = {en} } @inproceedings{RohrbeckFischerWehneretal., author = {Rohrbeck, Magdalena and Fischer, Christian B. and Wehner, Stefan and Richter, Matthias and Schmeißer, Dieter}, title = {Diamond-Like Carbon Coatings on Industrial Polyethylene Surfaces}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Bd. 47}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {Synthetic materials are used in a wide variety of fields. Depending on the intended application the plastic material must meet specific requirements. Since the material always interacts with its environment, particular attention is required regarding the surface. Possible damage of the plastic material and further risks could be caused by the adhesion of bacteria, biofilm formation and encrustations. Therefore, bacteria-repellent coatings and surface-modified materials that allow for an effective removal of adhered bacteria are of extremely high interest for many applications. In this study Polyethylene (PE) is chosen as simplest model for relevant plastic materials. Surface modification of PE samples is accomplished by plasma-deposited diamond-like carbon (DLC) coatings to achieve increased abrasion strength and bacterial resistance. Two types of nanometer-scaled DLC films with different layer thicknesses are compared by multiscale microscopic analysis. Further spectroscopic measurements with synchrotron radiation are performed. These results will provide an enhanced understanding of layer formation at the interface between the basic plastic material and the DLC coating and will possibly lead to optimal parameters for the surface coating to achieve improved product characteristics.}, language = {en} } @misc{DasTallaridaSchmeisser, author = {Das, Chittaranjan and Tallarida, Massimo and Schmeißer, Dieter}, title = {Si microstructures laminated with a nanolayer of TiO2 as long-term stable and effective photocathodes in PEC devices}, series = {Nanoscale}, journal = {Nanoscale}, number = {7}, issn = {2040-3364}, doi = {10.1039/C5NR00764J}, pages = {7726 -- 7733}, abstract = {Photoelectrochemical (PEC) water splitting is one of the most emerging fields for green energy generation and storage. Here we show a study of microstructured Si covered by a TiO2 nano-layer. The microstructures are prepared by galvanostatic selective etching of Si. The TiO2 nano-layer was deposited by atomic layer deposition (ALD) to protect the microstructured photocathode against corrosion. The obtained microstructured photocathode showed a shift in the onset potential of 400 mV towards the anodic direction compared to bare Si. The Si microstructures laminated with a nano-layer of TiO2 show stability over 60 hours of measurement.}, language = {en} } @inproceedings{HenkelDasSowinskaetal., author = {Henkel, Karsten and Das, Chittaranjan and Sowinska, Małgorzata and Tallarida, Massimo and Schmeißer, Dieter and Gargouri, Hassan and K{\"a}rkk{\"a}nen, Irina and Schneidewind, Jessica and Gruska, Bernd and Arens, Michael}, title = {Charakterisierung von TiO2-ALD-Schichten und deren Nutzung f{\"u}r die Passivierung von Si-Photokathoden}, series = {Tagungsband Photovoltaik-Meeting: Anwendungen-Qualit{\"a}t-Perspektiven, Senftenberg, 15.04.2015}, booktitle = {Tagungsband Photovoltaik-Meeting: Anwendungen-Qualit{\"a}t-Perspektiven, Senftenberg, 15.04.2015}, editor = {Gl{\"u}ck, B. K. and Schmidt, S. and Stein, E. and Raschke, J{\"o}rg-Uwe and Richter, H.}, publisher = {BTU Cottbus-Senftenberg}, address = {Senftenberg}, pages = {3 -- 8}, abstract = {Wir berichten zun{\"a}chst {\"u}ber den Einfluss der Methode der Atomlagenabscheidung auf die TiO2-Schichteigenschaften. Insbesondere wird der Zusammenhang zwischen Ti3+- sowie Interbandzust{\"a}nden mit elektrischen Kennlinien und deren Einfluss auf funktionale Schichteigenschaften diskutiert. Anschließend werden Mikrostrukturierung, Grenzfl{\"a}chen-Engineering und konforme Abscheidung einer TiO2-ALD-Schutzschicht effektiv zur Performance-Steigerung von p-Si-Photokathoden angewendet.}, language = {de} } @misc{NourbakhshAdelmannSongetal., author = {Nourbakhsh, Amirhasan and Adelmann, Christoph and Song, Yi and Lee, Chang Seung and Asselberghs, Inge and Huyghebaert, Cedric and Brizzi, Simone and Tallarida, Massimo and Schmeißer, Dieter and Elshocht, Sven van and Heyns, Marc and Kong, Jing and Palacios, Tom{\´a}s and De Gendt, Stefan}, title = {Graphene oxide monolayers as atomically thin seeding layers for atomic layer deposition of metal oxides}, series = {Nanoscale}, volume = {2015}, journal = {Nanoscale}, number = {7}, issn = {2040-3364}, doi = {10.1039/C5NR01128K}, pages = {10781 -- 10789}, abstract = {Graphene oxide (GO) was explored as an atomically-thin transferable seed layer for the atomic layer deposition (ALD) of dielectric materials on any substrate of choice. This approach does not require specific chemical groups on the target surface to initiate ALD. This establishes GO as a unique interface which enables the growth of dielectric materials on a wide range of substrate materials and opens up numerous prospects for applications. In this work, a mild oxygen plasma treatment was used to oxidize graphene monolayers with well-controlled and tunable density of epoxide functional groups. This was confirmed by synchrotron-radiation photoelectron spectroscopy. In addition, density functional theory calculations were carried out on representative epoxidized graphene monolayer models to correlate the capacitive properties of GO with its electronic structure. Capacitance-voltage measurements showed that the capacitive behavior of Al2O3/GO depends on the oxidation level of GO. Finally, GO was successfully used as an ALD seed layer for the deposition of Al2O3 on chemically inert single layer graphene, resulting in high performance top-gated field-effect transistors.}, language = {en} } @misc{TamangGhoshGarainetal., author = {Tamang, Abiral and Ghosh, Sujoy Kumar and Garain, Samiran and Alam, Md. Mehebub and Haeberle, J{\"o}rg and Henkel, Karsten and Schmeißer, Dieter and Mandal, Dipankar}, title = {DNA-Assisted β‑phase Nucleation and Alignment of Molecular Dipoles in PVDF Film: A Realization of Self-Poled Bioinspired Flexible Polymer Nanogenerator for Portable Electronic Devices}, series = {ACS Applied Materials \& Interfaces}, journal = {ACS Applied Materials \& Interfaces}, number = {7}, issn = {1944-8244}, doi = {10.1021/acsami.5b04161}, pages = {16143 -- 16147}, abstract = {A flexible nanogenerator (NG) is fabricated with a poly(vinylidene fluoride) (PVDF)film, where deoxyribonu-cleic acid (DNA) is the agent for the electroactive β-phase nucleation. Denatured DNA is co-operating to align the molecular-CH2/-CF2 dipoles of PVDF causing piezo- electricity without electrical poling. The NG is capable of harvesting energy from a variety of easily accessible mechanical stress such as human touch, machine vibration, football juggling, and walking. The NG exhibits high piezoelectric energy conversion efficiency facilitating the instant turn-on of several green or blue light-emitting diodes. The generated energy can be used to charge capacitors providing a wide scope for the design of self-powered portable devices.}, language = {en} } @misc{SchmeisserHaeberleRichteretal., author = {Schmeißer, Dieter and Haeberle, J{\"o}rg and Richter, Matthias and Brazda, Petr}, title = {Spin State and Satellite Structures of ε-Fe₂O₃ as determined by Resonant Photoelectron Spectroscopy}, series = {Nuclear Instruments and Methods in Physics Research B}, volume = {2015}, journal = {Nuclear Instruments and Methods in Physics Research B}, number = {364}, issn = {0168-583X}, doi = {10.1016/j.nimb.2015.08.062}, pages = {127 -- 131}, abstract = {We use resonant photoelectron spectroscopy at the Fe2p and the O1s absorption edges to report on spectroscopic investigation of Fe-oxides nanoparticles. We discuss the spectroscopic details like multiple Auger decays, satellite emission in the X-ray absorption process and the core level data. We explain these data by a novel mechanism in which the resonant excitation between Fe3d and Fe4s states are involved. This mechanism is observed when the photo-excited electron becomes polarized by the electron-hole pairs existing in the conduction and valence bands.}, language = {en} } @misc{AlbertonCorreaBrizziSchmeisser, author = {Alberton Corr{\^e}a, Silma and Brizzi, Simone and Schmeißer, Dieter}, title = {Spectroscopic investigation of the electronic structure of thin atomic layer deposition HfO2 films}, series = {Journal of Vacuum Science \& Technology A}, volume = {34}, journal = {Journal of Vacuum Science \& Technology A}, number = {1}, issn = {0734-2101}, doi = {10.1116/1.4935338}, pages = {01A117-1 -- 01A117-8}, abstract = {The electronic structure of HfO2 thin films is investigated employing resonant photoelectron spectroscopy (resPES). The detailed analysis of the O1s resonance profile enables the determination of the partial density of states for the valence and the conduction bands as well as the electronic band gap to be 6.2 eV. The position of the charge neutrality level is evaluated. Thereby, it is demonstrated that the resPES data are able to combine information both for the valence as well as for the conduction band states. In addition, evidences for intrinsic in-gap states attributed to polaronic and charge transfer states are given. Electronic charges within the atomic layer deposition-HfO2films are identified, pointing out that the amount of charges is essential to determine the accurate position of the surface potentials.}, language = {en} } @misc{SowińskaHenkelSchmeisseretal., author = {Sowińska, Małgorzata and Henkel, Karsten and Schmeißer, Dieter and K{\"a}rkk{\"a}nen, Irina and Schneidewind, Jessica and Naumann, Franziska and Gruska, Bernd and Gargouri, Hassan}, title = {Plasma-enhanced atomic layer deposition of titanium oxynitrides films: A comparative spectroscopic and electrical study}, series = {Journal of Vacuum Science and Technology A}, journal = {Journal of Vacuum Science and Technology A}, number = {34}, issn = {0734-2101}, doi = {10.1116/1.4936227}, pages = {01A127-1 -- 01A127-9}, abstract = {The process parameters' impact of the plasma-enhanced atomic layer deposition (PE-ALD) method on the oxygen to nitrogen (O/N) ratio in titanium oxynitride (TiOxNy) films was studied. Titanium(IV)isopropoxide in combination with NH3 plasma and tetrakis(dimethylamino) titanium by applying N2 plasma processes were investigated. Samples were characterized by the in situ spectroscopic ellipsometry, x-ray photoelectron spectroscopy, and electrical characterization (current-voltage: I-V and capacitance-voltage: C-V) methods. The O/N ratio in the TiOxNy films is found to be very sensitive for their electric properties such as conductivity, dielectric breakdown, and permittivity. Our results indicate that these PE-ALD film properties can be tuned, via the O/N ratio, by the selection of the process parameters and precursor/coreactant combination.}, language = {en} } @misc{PitthandosReisAlbertonCorreaetal., author = {Pitthan, E. and dos Reis, R. and Alberton Corr{\^e}a, Silma and Schmeißer, Dieter and Boudinov, H. I. and Stedile, F. C.}, title = {Influence of CO annealing in metal-oxide-semiconductor capacitors with SiO2 films thermally grown on Si and on SiC}, series = {Journal of Applied Physics}, journal = {Journal of Applied Physics}, number = {119}, issn = {0021-8979}, doi = {10.1063/1.4939836}, pages = {025307-1 -- 025307-6}, abstract = {Understanding the influence of SiC reaction with CO, a by-product of SiC thermal oxidation, is a key point to elucidate the origin of electrical defects in SiC metal-oxide-semiconductor (MOS) devices. In this work, the effects on electrical, structural, and chemical properties of SiO2/Si and SiO2/SiC structures submitted to CO annealing were investigated. It was observed that long annealing times resulted in the incorporation of carbon from CO in the Si substrate, followed by deterioration of the SiO2/Si interface, and its crystallization as SiC. Besides, this incorporated carbon remained in the Si surface (previous SiO2/Si region) after removal of the silicon dioxide film by HF etching. In the SiC case, an even more defective surface region was observed due to the CO interaction. All MOS capacitors formed using both semiconductor materials presented higher leakage current and generation of positive effective charge after CO annealings. Such results suggest that the negative fixed charge, typically observed in SiO2/SiC structures, is not originated from the interaction of the CO by-product, formed during SiC oxidation, with the SiO2/SiC interfacial region.}, language = {en} } @misc{SchmeisserHaeberle, author = {Schmeißer, Dieter and Haeberle, J{\"o}rg}, title = {Intrinsic localized gap states in IGZO and its parent single crystalline TCOs}, series = {Thin Solid Films}, journal = {Thin Solid Films}, number = {603}, issn = {0040-6090}, doi = {10.1016/j.tsf.2016.02.010}, pages = {206 -- 211}, abstract = {We report on the X-ray absorption data for Indium-Gallium-Zink-Oxide thin films, amorphous ZnO films, amorphous SnOx films, and single crystalline In2O3, Ga2O3, ZnO, and SnO2 data. These absorption data probe the empty conduction band states explicitly. Also they allow for an elemental assignment using resonant excitation to derive the contributions of each metal ion. We find that the lowest states appear right at the Fermi energy and result from configuration interaction induced charge transfer states which we consider as intrinsic gap states.}, language = {en} } @inproceedings{AlbertonCorreaBrizziTallaridaetal., author = {Alberton Corr{\^e}a, Silma and Brizzi, Simone and Tallarida, Massimo and Schmeißer, Dieter}, title = {Charging effect in HfO2 films deposited on SiO2/Si by atomic layer deposition}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {Thin films of hafnium oxide (HfO2) deposited by atomic layer deposition (ALD) have been studied extensively as a high-k replacement for the SiO2 gate in field effect transistors. The use of ALD process allows one to grow homogeneous thin films at low temperatures with a precise control of thickness [1]. Some important electrical considerations for the application of a high-k dielectric include the presence of fixed charge (Qf) and charge trapping in the dielectric. For instance, in the case of Al2O3 thin films deposited on Si, the thickness of the interfacial SiO2 layer was identified as a key fundamental parameter determining Qf [2]. A similar trend can be also expected in HfO2/Si structures. Therefore, in this work, we proposed an in situ evaluation of photon induced charge trapping in HfO2 films deposited on SiO2/Si structures. For that, tetrakis-di-methyl-amino-hafnium (TDMAHf) and H2O were employed as precursors to deposit HfO2 films on SiO2/Si samples with variable thickness of the SiO2 interlayer. Measurements were performed by Synchrotron Radiation Photoemission Spectroscopy (SR-PES). Results indicated that the charging process is dependent on the thickness of the SiO2 interlayer and on the quality of the HfO2 film. [1] M. Leskel{\"a} and M. Ritala, Thin Solid Films 409, 138 (2002). [2] G. Dingemans et al., J. Appl. Phys. 110, 093715 (2011).}, language = {en} } @inproceedings{BrizziTallaridaAdelmannetal., author = {Brizzi, Simone and Tallarida, Massimo and Adelmann, Christoph and Ragnarsson, Lars-{\AA}ke and Elshocht, Sven van and Schmeißer, Dieter}, title = {Structural changes in HfO2 thin films: thickness and doping dependence}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {In this work we show results regarding MOCVD and ALD HfO2 as well as Al-doped HfO2. We use Synchrotron Radiation Photoemission Spectroscopy (SRPES) to determine Hf/O atomic ratios and X-ray Absorption Spectroscopy (XAS) to investigate the electronic properties related to their crystallization. MOCVD films are synthesized at temperatures ranging from ambient to 400∘C and show structures from completely amorphous to monoclinic. ALD films are amorphous as deposited, and can crystallize after post-deposition anneal depending on the percentage of Al-doping. We discuss PES results in order to determine how close to stoichiometry the Hf/O atomic ratios of the films are, as well as the doping level. From XAS data, instead, we can point out how orbital hybridizations are related to structural and physical properties.}, language = {en} } @inproceedings{DasTallaridaSchmeisser, author = {Das, Chittaranjan and Tallarida, Massimo and Schmeißer, Dieter}, title = {X-ray linear dichroism in atomic layer deposited Titanium dioxide layers}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {Among the various metal oxides TiO2 has been investigated because of its wide range of applications in various fields such as self-cleaning, photocatalysis, solar cell, water splitting, bio-implants. In order to increase its efficiency in water splitting and solar cell energy conversion, it is necessary to understand the crystal structure and electronic properties of thin films. Generally the process of synthesis may modify the electronic properties of TiO2. In the present work we show X-ray linear dichroism (XLD) measurements of TiO2 thin films of different polymorphs. Titania thin films were produced by atomic layer deposition (ALD) and were characterized in-situ with X-ray photoelectron and absorption spectroscopy at synchrotron radiation center BESSY-II. We found that that all titania phases show XLD at Ti-L and O-K edges, but the intensity of XLD is different for different phases. We discuss our data in terms of the partial density of states.}, language = {en} } @inproceedings{DasTallaridaSchmeisser, author = {Das, Chittaranjan and Tallarida, Massimo and Schmeißer, Dieter}, title = {Control of thickness of SiO2 interfacial layer for photocatalytic water splitting on Si photocathodes}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {Silicon with a band gap of 1.1eV is an excellent candidate for visible photocatalytic water splitting. But p-type Si has a low quantum yield and are less efficient for water splitting [1]. It has been shown that preventing oxidation of Si surface can shift the onset potential for water reduction by about 300mV towards more positive [2]. We investigated in detail the influence of the SiO2 layer thickness on the onset potential for water splitting on Si photocathodes: we used p-type Si substrates covered with SiO2 layers of varying thickness. Then, we deposited a thin TiO2 film on using atomic layer deposition (ALD) to inhibit Si oxidation during the electrochemical experiment. In this way we could shift the onset potential up to 200mV, depending on the SiO2 thickness. [1]E. L. Warren, S. W. Boettcher, M. G. Walter, H. A. Atwater, and N. S. Lewis: J. Phys. Chem. C 115 (2011) 594. [2]B. Seger, Anders B. Laursen, P. C. K. Vesborg, T. Pedersen, O. Hansen, S. Dahl, I. Chorkendorff, Angew. Chem. Int. Ed. 2012, 51, 9128}, language = {en} } @inproceedings{HaeberleGasparBarquinhaetal., author = {Haeberle, J{\"o}rg and Gaspar, Diana and Barquinha, Pedro and Machulik, Stephan and Janowitz, Christoph and Galazka, Zbigniew and Schmeißer, Dieter}, title = {A spectroscopic comparison of AOS thin films and TCO single crystals}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, abstract = {Amorphous oxide semiconductors (AOS) and transparent conductive oxides (TCO) are today one of most attractive fields of research in many industrial products, like e.g. high definition, low cost, transparent, and flexible displays. We got the unique possibility to measure a-GIZO and a-SnOx thin films and compare their electronic properties with those of In2O3, Ga2O3, ZnO, and SnO2 single crystals. We use resPES to study the electronic properties. We report on the core levels, the VB PES data, partial Integrated Yield (pIY) and the XAS absorption data. From these we are able to derive the elemental ratio, the pDOS as well as the band scheme. At the O1s resonance we observe multiple Auger processes from which we deduce that a band of localized defect states is located between the Fermi energy and the CBM. The resonant profiles taken at the corresponding metal edges indicate that metal states are involved in the DOS.}, language = {en} } @inproceedings{TallaridaHenkelGargourietal., author = {Tallarida, Massimo and Henkel, Karsten and Gargouri, Hassan and Haeberle, J{\"o}rg and Gruska, Bernd and Arens, Matthias and Schmeißer, Dieter}, title = {New opportunities with Plasma enhanced atomic layer deposition (PE-ALD) of oxides}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {Thermal Atomic layer deposition (T-ALD) of oxides is obtained by the pulsed alternation of a metal precursor and an oxygen source, typically H2O or O3, and the reactions leading to ALD are thermally activated. With plasma enhanced ALD (PE-ALD), instead, the oxygen source is represented by an oxygen-containing plasma. The higher reactivity of the plasma-generated species extend the capabilities of ALD: improved film quality and increased flexibility in process conditions, such as growth at low temperature, are typical advantages of PE-ALD over T-ALD. We report on results on the preparation of thin (<100 nm) aluminum oxide (Al2O3) films on silicon substrates using T-ALD and PE-ALD in the SENTECH SI ALD LL system. Films were deposited in the temperature range between room temperature (RT) and 200∘C. We characterized the films with spectroscopic ellipsometry (thickness, refractive index, growth rate) over 4" wafers and with X-ray photoelectron spectroscopy. All films resulted in a high degree of homogeneity, independent of the deposition temperature. Investigations with capacitance-voltage and conductance-voltage measurements showed a very low interface states density for the PE-ALD films.}, language = {en} } @inproceedings{RoeskenRohrbeckCatenaetal., author = {R{\"o}sken, Liz M. and Rohrbeck, Magdalena and Catena, Alberto and Wehner, Stefan and Fischer, Christian B. and Richter, Matthias and St{\"a}dter, Matthias and Schmeißer, Dieter}, title = {Characterization of diamond-like carbon (DLC) coatings on industrial polyethylene and polyoxymethylene by SEM, AFM and NEXAFS}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, abstract = {Diamond-like carbon (DLC) coatings are often utilized to change the base properties of raw materials, e. g. to gain robust or chemically inert surfaces. Here the deposition of hard DLC layers on soft polymers is tested. The common industrial polymers polyethylene (PE) and polyoxymethylene (POM) serve as model substrates in the present work. In order to examine the effect of the carbonaceous layers on PE and POM thin diamond-like carbon films were realized via PECVD. The topography of the different coatings was detected by AFM and SEM uncovering the different influence of the substrate material, e. g. interlayer formation for PE. The composition of the surface structures were analyzed in more detail by NEXAFS, showing the hybridization of carbon atoms in chemical different surroundings from the pure polymer to the carbon coating. The comparison of carbon coated PE- and POM-composites enables valuable insights into the interaction between soft substrates and hard coatings. For the chosen settings in PECVD, POM showed incomplete coating, while on PE a very stable and robust composite has formed.}, language = {en} } @inproceedings{AlbertonCorreaBrizziTallaridaetal., author = {Alberton Corr{\^e}a, Silma and Brizzi, Simone and Tallarida, Massimo and Schmeißer, Dieter}, title = {Spectroscopic investigation of the electronic structure of HfO2 thin films}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 211}, abstract = {HfO2 is of current interest as a material for memristive and ferroelectric devices. In this work, we used spectroscopic techniques to evaluate the electronic structure and defects mechanisms in thin HfO2 films deposited by atomic layer deposition and by metal-organic chemical vapour deposition. The partial density of states for the valence and the conduction bands was determined by the detailed analysis of the O1s resonance profile by resonant photoelectron spectroscopy. From the relative contributions we find a CNL 6.5 eV referred to Evac. We also find that the positions of valence band maximum and conduction band minimum, the excitation range for the polaronic states and the range of charge transfer band were not influenced by the preparation conditions. All films exhibit a band gap of 6.2 eV. However, the Fermi level position was found to vary within about 1.2 eV depending on the preparation conditions, which we argue that is due to the presence of charges within the films. This explains why the position of the Fermi level depends on the individual preparation parameters.}, language = {en} } @inproceedings{DasTallaridaSchmeisser, author = {Das, Chittaranjan and Tallarida, Massimo and Schmeißer, Dieter}, title = {Determination of charge neutrality level in TiO2 films from res-PES measurements}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 415}, abstract = {Titanium dioxide is one of the metal oxides which have versatile application in different fields. The applications of TiO2 are in the field of cosmetics, electronics (memory resistive switching), dye, photonics and photocatalysis. In the present paper we study the resPES data of TiO2 films prepared by atomic layer deposition. The measurements are done in in-situ system at beam line U49/2-PGM2 in BESSY-II. The density of state in valence band and conduction band is obtained from the resonance photo electron spectroscopy (res-PES) of the O1s and the Ti2p edge. The data allow to determine the position of the VBM and CBM with respect to the Fermi energy. Also the existence of localized O2p and Ti2p derived states is deduced which appear in the gap. In addition we determine the charge neutrality level (CNL).The CNL is the position where the weight of the density of state from valence band and conduction band are equal. This is an important quantity for the discussion of interface properties.}, language = {en} } @inproceedings{HaeberleGasparBarquinhaetal., author = {Haeberle, J{\"o}rg and Gaspar, Diana and Barquinha, Pedro and Pereira, Lu{\´i}s and Martins, Rodrigo and Fortunato, Elvira and Machulik, Stephan and Janowitz, Christoph and Manzke, Recardo and Schmeißer, Dieter}, title = {The Electronic Structure of amorphuos SnOx thin films and SnO2 single crystals}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 271}, abstract = {We compare the electronic properties of amorphous p-type SnOx thin film grown by rf magnetron sputtering with those of n-type SnO2 single crystals grown by cvt. We use resPES to study the electronic band structure. We measure the core levels, the VB PES data, partial Integrated Yield (pIY) and the XAS absorption data. From the resPES data recorded at the O1s and the Sn3d edges we derive the VB pDOS and the CB pDOS . The differences are most pronounced in the position of the VBM as for the a-SnOx films there appears a band closer to the Fermi energy. In addition for the SnOx we find in the XAS and pIY data a significant peak that appears right at the Fermi energy. This peak is absent in the single crystalline data. We attribute this to a change in the configuration of the Sn4d states to form a 4d8 configuration instead of 4d9 and 4d10 configurations which are identified in the single crystalline data.}, language = {en} } @inproceedings{IsraelRachowSchwiertzetal., author = {Israel, Johannes and Rachow, Fabian and Schwiertz, Carola and Charlafti, Evgenia and M{\"u}ller, Klaus and Schmeißer, Dieter}, title = {Self restriction oft the Sabatier reaction in large scale}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, abstract = {A main goal for a sustainable energy supply is a long term energy storage system. One opportunity in this research field is the power to gas concept, where the produced gas can be fed in the existing network of natural gas. Here we show in a technical scale how the direct CO2 conversion to methane according the Sabatier reaction, CO2 + 4 H2 → CH4 + 2H2O , is self organized. At a certain limit of gas flow, a steady state equilibrium of exothermic heat production and thermal flow is reached and the reaction needs no further external annealing. We find for the maximum volume rate at the steady state equilibirum a shift of around 250 ∘C above the optimized temperature of the catalytic supported chemical equilibrium. It is shown that also with this setup the used catalyst works with a stable conversion higher than 80 \% under the reached temperature and given pressure conditions.}, language = {en} } @inproceedings{MandalHenkelSchmeisser, author = {Mandal, Dipankar and Henkel, Karsten and Schmeißer, Dieter}, title = {A polymer nanogenerator based on silver nanoparticles doped electrospun P(VDF-HFP) nanofibers}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 208}, abstract = {The rising energy demand within the increasing mobility of human society has driven the development of new alternative power sources for portable devices with ultra-low electric power consumption. Based on its piezoelectric properties poly-vinylidene fluoride (PVDF) is a good candidate for mechanical energy harvesting for such devices. Moreover the copolymer poly(vinylidene fluoride-hexafluoropropylene) [P(VDF-HFP)] offers better film flexibility and cost-effectiveness than pure PVDF. We report on a polymer nanogenerator (PNG) based on electrospun P(VDF-HFP) nanofibers doped with silver nanoparticles (Ag-NPs). The electrospun fibers were characterized by FTIR, XPS, SEM and pressure imparting probe. It has been found that the yield of the piezoelectric phase is increased by the addition of Ag-NPs due to an interaction between surface charges of Ag-NPs and the molecular dipoles. Furthermore, defects in the P(VDF-HFP) electrospun fibers are removed. Accordingly, a significant enhancement in the output power of the PNG was found. Similar trends were also observed with Pd-NPs.}, language = {en} } @inproceedings{RachowIsraelSchwiertzetal., author = {Rachow, Fabian and Israel, Johannes and Schwiertz, Carola and Charlafti, Evgenia and M{\"u}ller, Klaus and Schmeißer, Dieter}, title = {CO2 Methanation with different gas mixtures}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 539}, abstract = {A key issue in the Energiewende in Germany is the storage of excess energy, as it enables energy management systems to react to fluctuating sources and enhances the flexibility of an energy mix. Power to Gas may be the most reasonable approach to store the energy in the form of hydrogen or synthetic natural gas. We study the direct conversion of CO2 by the Sabatier reaction to gain a methane based mixture which can replace natural gas in CHP plants and gas motors and can help to partially reduce the CO2 emission. In laboratory scale we investigated the performance (with IR and QMS) of Ni-based catalyst for different sources of CO2 like clean CO2, CO2 emitted as flue gas from an Oxyfuel power plant or a synthetic mixture with O2, N2 and SO2 in concentration typical for conventional power plants. Measurements from an up-scaled system are also presented, showing data important for a technical application. Here, we are able to convert more than 200kg CO2/day with conversion rates up to 90\%.}, language = {en} } @inproceedings{RouissiTallaridaSchmeisser, author = {Rouissi, Zied and Tallarida, Massimo and Schmeißer, Dieter}, title = {Study of atomic layer deposition with scanning tunneling microscopy}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 401}, abstract = {We present a work concerning the study of the initial steps of atomic layer deposition (ALD) with scanning tunneling microscopy (STM). We focus on the role of the substrates which has been often neglected.However, the detailed knowledge of precursor-substrate reactions is important for the understanding of how ALD proceeds. We report on the reaction of the Al-precursor, trimethyl-Al (TMA), on nanostructured surfaces such as Ag nanoclusters and nanostripes prepared by thermal evaporation on HOPG. We characterized the surface before and after one TMA adsorption pulse at room temperature, observing that the morphology of step edges changes after TMA creating a new terraces with a width of 7-10 nm, translated in the direction of the TMA deposition. This shows that, in case of a regular stepped surface, the substrate morphology would keep the same regularity with the translation in a direction privileged by the precursor absorption.}, language = {en} } @inproceedings{RouissiBrizziAlbertonCorreaetal., author = {Rouissi, Zied and Brizzi, Simone and Alberton Corr{\^e}a, Silma and Tallarida, Massimo and Schmeißer, Dieter}, title = {Comparison of charge neutrality level of Cu/CuO/HfO2 and Si/SiO2/HfO2}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {208}, abstract = {Copper Oxide (CuO) is a promising metal oxide semiconductor, which can be used in different applications, such as catalysis, solar energy conversion, and water splitting. In this work, we use resonance photoemission spectroscopy (ResPES) to analyse the electronics properties of HfO2 films deposited on Cu/CuO and Si/SiO2. For that, we deposited 10 cycles of HfO2 by atomic layer deposition (ALD) on Cu/CuO and Si/SiO2 samples and investigated the density states for the valence and conduction bands which were determined by the detailed analysis of the O1s resonance profile obtained by ResPES. We compared the positions of valence band maximum and conduction band minimum, the excitation range for the polaronic states and the range of charge transfer band in Cu/CuO/HfO2 and Si/SiO2/HfO2. Also, we determined the band gap and the charge neutrality level (CNL).}, language = {en} } @misc{KrammZanaVoschetal., author = {Kramm, Ulrike Ingrid and Zana, Alessandro and Vosch, Tom and Fiechter, Sebastian and Arenz, Matthias and Schmeißer, Dieter}, title = {On the structural composition and stability of Fe-N-C catalysts prepared by an intermediate acid leaching}, series = {Journal of Solid State Electrochemistry}, volume = {20}, journal = {Journal of Solid State Electrochemistry}, number = {4}, issn = {1432-8488}, doi = {10.1007/s10008-015-3060-z}, pages = {969 -- 981}, abstract = {The development of highly active and stable non-noble metal catalysts (NNMC) for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEM-FC) becomes of importance in order to enable cost reduction. In this work, we discuss the structural composition as derived from Fe-57M{\"o}ßbauer spectroscopy and X-ray diffraction, catalytic performance determined by a rotating (ring)disk electrode (RRDE) technique and stability evaluation of our Fe-N-C catalysts prepared by an intermediate acid leaching (IAL). The advantage of this IAL is given by a high density of active sites within the catalyst, as even without sulphur addition, an iron carbide formation and related disintegration of active sites are inhibited. In addition, our accelerated stress tests illustrate better stability of the sulphur-free IAL catalyst in comparison to the sulphur-added one.}, language = {en} }