@misc{KotŁobazaNaumannetal., author = {Kot, Małgorzata and Łobaza, Justyna and Naumann, Franziska and Gargouri, Hassan and Henkel, Karsten and Schmeißer, Dieter}, title = {Long-term ambient surface oxidation of titanium oxynitride films prepared by plasma-enhanced atomic layer deposition: An XPS study}, series = {Journal of Vacuum Science and Technology A}, volume = {36}, journal = {Journal of Vacuum Science and Technology A}, number = {1}, issn = {0734-2101}, doi = {10.1116/1.5003356}, abstract = {The surface oxidation of a titanium oxynitride (TiOxNy) film after long-time storage of 25 month in ambient conditions is investigated. The TiOxNy film is prepared by plasma-enhanced atomic layer deposition using etrakis(dimethylamino)titanium and nitrogen plasma, and the film is characterized by Ar+ ion sputtering of the film surface in combination with x-ray photoelectron spectroscopy (XPS) as well as by angle-resolved XPS. The total thickness of an oxygen-enriched layer at the surface of the TiOxNy films is found to be about 0.7 nm and it consists of a sequence of a 0.4 nm thick TiON/TiO2 enriched layer followed by a 0.3 nm thick TiO2 enriched layer underneath compared to the bulk composition of the film which shows constant values of 29\% TiN, 29\% TiO2, and 42\% TiON. The results suggest that the TiON enrichment takes place initially at the surface followed by a surface and subsurface oxidation.}, language = {en} } @misc{SchmeisserHenkel, author = {Schmeißer, Dieter and Henkel, Karsten}, title = {Intrinsic defects and multiple-atom processes in the oxidic semiconductor Ga₂O₃}, series = {Journal of Applied Physics}, volume = {123}, journal = {Journal of Applied Physics}, number = {16}, issn = {0021-8979}, doi = {10.1063/1.5010740}, pages = {161596-1 -- 161596-9}, abstract = {We report on the electronic structure of gallium oxide (Ga₂O₃) single crystals as studied by resonant photoelectron spectroscopy (resPES). We identify intrinsic electronic defects that are formed by mixed-atomic valence states. We differentiate three coexisting defect states that differ in their electronic correlation energy and their spatial localization lengths. Their relative abundance is described by a fractional ionicity with covalent and ionic bonding contributions. For Ga₂O₃, our analyses of the resPES data enable us to derive two main aspects: first, experimental access is given to determine the ionicity based on the original concepts of Pauling and Phillips. Second, we report on multi-atomic energy loss processes in the Ga2p core level and X-ray absorption data. The two experimental findings can be explained consistently in the same context of mixed-atomic valence states and intrinsic electronic defects.}, language = {en} } @misc{KotWojciechowskiSnaithetal., author = {Kot, Małgorzata and Wojciechowski, Konrad and Snaith, Henry J. and Schmeißer, Dieter}, title = {Evidence of Nitrogen Contribution to the Electronic Structure of the CH₃NH₃PbI₃ Perovskite}, series = {Chemistry - A European Journal}, volume = {24}, journal = {Chemistry - A European Journal}, number = {14}, issn = {0947-6539}, doi = {10.1002/chem.201705144}, pages = {3539 -- 3544}, abstract = {Despite fast development of hybrid perovskite solar cells, there are many fundamental questions related to the perovskite film which remain open. For example, there are contradicting theoretical reports on the role of the or-ganic methylammonium cation (CH₃NH₃+)in the methylam-monium lead triiodide (CH₃NH₃PbI₃)perovskite film. From one side it is reported that the organic cation does not contribute to electronic structure of the CH₃NH₃PbI₃ film. From the other side, valence band maximum fluctuations, dependent on the CH₃NH₃+ rotation, have been theoretically predicted. The resonant X-ray photoelectron spectroscopy results reported here show experimental evidence of nitrogen contribution to the CH₃NH₃PbI₃ electronic structure. Moreover,the observed strong resonances of nitrogen with the I 5s and the Pb 5d-6s levels indicate that the CH₃NH₃PbI₃ valence band is extended up to ~18 eV below the Fermi energy, and therefore one should also consider these shallow core levels while modeling its electronic structure.}, language = {en} } @misc{JanowitzSchmeisser, author = {Janowitz, Christoph and Schmeißer, Dieter}, title = {Significance of out-of-plane electronic contributions in Bi-cuprates studied by resonant photoelectron spectroscopy at the Cu2p-edge}, series = {Superconductor Science and Technology}, volume = {31}, journal = {Superconductor Science and Technology}, number = {4}, issn = {0953-2048}, doi = {10.1088/1361-6668/aaadf6}, pages = {11}, abstract = {In high-temperature superconductors with a layered crystal structure, the copper-oxygen planes are commonly considered to dominate the electronic properties around the Fermi energy. As a consequence, out-of-plane contributions are often neglected in the description of these materials. Here we report on a resonant photoemission study of Pb₀,4Bi1,₆Sr₂,₀CaCu₂0₈ ((Pb, Bi)-2212) and Pb₀,₆Bi₁,₄Sr₁.5La₀.5Cu0₆ ((Pb, Bi)-2201)) single crystals to unravel the resonant decay mechanisms at the Cu2p absorption edge. We find evidence for a pronounced polarization dependence caused by two different Auger processes for in-plane and out-of-plane orientations. We deduce that the lowest energy valence state—which is involved in the two Auger processes—consists of three-dimensional contributions by admixed out-of-plane Sr, Bi, and 02p states. It also suggests that the doping-induced charge density is dynamic, fluctuating within the Cu-0 plane, and spills out perpendicular to it. This suggests that out-of-plane electronic degrees of freedom should be included in future consistent theoretical models of these materials.}, language = {en} } @inproceedings{GarainHenkelMandaletal., author = {Garain, Samiran and Henkel, Karsten and Mandal, Dipankar and Schmeißer, Dieter}, title = {One-Pot Synthesis of Copper Oxide Nanowires and PVDF/CuO Composite Films for Piezoelectric Energy Harvesting Application}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Band 53,3}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Band 53,3}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 135}, abstract = {Copper oxide (CuO) is an attractive p-type oxide semiconductor with narrow band gap that has intriguing properties such as non-toxicity, chemical stability, electrocatalytic activity, abundant availability and low production cost. Polymeric materials have attracted great interest owing to their high flexibility, light weight, low cost production and high resistance against corrosion. Poly(vinylidene fluoride) (PVDF) is a commonly used piezoelectric polymer due to its excellent flexibility and piezoelectric properties. In this work, we adopted a one-pot synthesis of CuO nanowires by facile and selective chemical etching process of Cu substrate. XPS, XRD, SEM data ascribed the formation of polycrystalline CuO nanowires over the entire Cu surface. It has been observed that the uniformity, shape and size of the nanowires could be conveniently controlled by etching time and etchant concentration. We have also prepared piezoelectric nanogenerator based on the flexible PVDF/CuO composite film, where the traditional electrical poling treatment was avoided. In addition, dielectric properties have been studied to demonstrate the role of interfacial polarization.}, language = {en} } @inproceedings{KotNaumannGarainetal., author = {Kot, Małgorzata and Naumann, Franziska and Garain, Samiran and Po{\'{z}}arowska, Emilia and Gargouri, Hassan and Henkel, Karsten and Schmeißer, Dieter}, title = {Aluminum nitride films prepared by plasma atomic layer deposition using different plasma sources}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Band 53,3}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Band 53,3}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 170}, abstract = {Aluminum nitride (AlN) thin films are promising for versatile applications in optoelectronics, electronics, piezoelectrics, and acoustics due to their remarkable properties such as wide band gap, high dielectric constant, low electrical conductivity, good piezoelectric coefficient and high ultrasonic velocity. We present a comparative study of AlN films grown by plasma-enhanced atomic layer deposition at 350°C silicon wafers in the SENTECH SI ALD LL system using TMA and NH3 where either a capacitively coupled plasma (CCP) or a direct PTSA (planar triple spiral antenna) source was applied. The films were characterized by ellipsometry, XPS and electrical measurements. The layer properties are discussed concerning the varied ALD process parameters. In general, the process using the direct PTSA source delivered films with higher refractive index and better homogeneity over the wafer achieving also higher growth rates per cycle (GPC) in reduced total cycle durations. Films with refractive index in the range of 2.05 and permittivity around 8 could be realized with a GPC of 1.54 {\AA}/cycle.}, language = {en} } @inproceedings{KotKegelmannKusetal., author = {Kot, Małgorzata and Kegelmann, Lukas and Kus, Peter and Tsud, Nataliya and Matol{\´i}nov{\´a}, Iva and Albrecht, Steve and Matolin, Vladimir and Schmeißer, Dieter}, title = {Room temperature atomic layer deposition for perovskite solar cells}, series = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Band 53,3}, booktitle = {Verhandlungen der Deutschen Physikalischen Gesellschaft, Reihe 6, Band 53,3}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {S. 174}, abstract = {After few years of efficiency driven research on perovskite solar cells, the focus now is shifting to understand the underlying processes governing the high efficiency and also to obtain long-term stable devices. Among various deposition methods, atomic layer deposition (ALD) may represent one of the best options, being possible to coat substrates in a very efficient way and at very low temperatures. In our previous work [1] we reported that the efficiency of the solar cell containing aged perovskite film can be enhanced twice while covering the perovskite with a thin ALD alumina film at room temperature. In this work, the chemical, electronic and morphological properties of the fresh perovskite film treated by ALD pulses of the trimethylaluminium and water at room temperature investigated using X-ray Photoelectron Spectroscopy and Field Emission Scanning Electron Microscopy will be discused and correlated with the solar cells performance and stability. [1] M. Kot et al., ChemSusChem 2016, 9, 3401.}, language = {en} } @misc{GarainSenHenkeletal., author = {Garain, Samiran and Sen, Shrabanee and Henkel, Karsten and Schmeißer, Dieter and Mandal, Dipankar}, title = {Enhancement of Electroactive β-phase and Superior Dielectric Properties in Cerium Based Poly(vinylidene fluoride) Composite Films}, series = {Materials Today: proceedings}, volume = {5}, journal = {Materials Today: proceedings}, number = {3 part 3}, issn = {2214-7853}, doi = {10.1016/j.matpr.2017.11.003}, pages = {10084 -- 10090}, abstract = {In this work we report on the preparation of poly(vinylidene fluoride) (PVDF) films with various mass fractions (wt\%) of hydrated rare earth metal salt [(NH4)4Ce(SO4)4.2H2O] (CAS) and its electroactive phase (β- and γ-phase) formation. It was found that CAS can yield high amount of electroactive phases in PVDF. Compared to the neat PVDF film, a significantly increment of dielectric constant (ε ∼ 41) and a low loss factor (tan δ ∼ 0.8) were observed in the PVDF-CAS composite films. Thus the PVDF-CAS composite films with high electroactive phase and superior dielectric properties may meet the requirements of next generation electronic components.}, language = {en} } @incollection{HenkelKotRichteretal., author = {Henkel, Karsten and Kot, Małgorzata and Richter, Matthias and Tallarida, Massimo and Schmeißer, Dieter}, title = {An (In Situ)² Approach: ALD and resPES Applied to Al₂O₃, HfO₂, and TiO₂ Ultrathin Films}, series = {Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry, Vol. 3.1}, booktitle = {Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry, Vol. 3.1}, editor = {Wandelt, Klaus}, publisher = {Elsevier}, address = {Oxford}, isbn = {978-0-12-809739-7}, doi = {10.1016/B978-0-12-409547-2.13852-1}, pages = {18 -- 26}, abstract = {Oxide surface coatings are of importance in tailoring interface properties with respect to surface passivation, adjustment of surface potentials, or providing active centers for surface reactions. In this contribution, we report about surface coatings prepared by the atomic layer deposition (ALD) method. ALD is known for its conformal growth of ultrathin, dense films which exhibit a low concentration of pinholes.}, language = {en} } @incollection{SchmeisserKotCorreaetal., author = {Schmeißer, Dieter and Kot, Małgorzata and Corr{\^e}a, Silma Alberton and Das, Chittaranjan and Henkel, Karsten}, title = {Interface Potentials, Intrinsic Defects, and Passivation Mechanisms in Al₂O₃, HfO₂, and TiO₂ Ultrathin Films}, series = {Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry, vol. 3.1}, booktitle = {Encyclopedia of Interfacial Chemistry: Surface Science and Electrochemistry, vol. 3.1}, editor = {Wandelt, Klaus}, publisher = {Elsevier}, address = {Oxford}, isbn = {978-0-12-809739-7}, doi = {10.1016/B978-0-12-409547-2.14119-8}, pages = {162 -- 171}, abstract = {We study the electronic structure of ultrathin Al₂O₃, HfO₂, and TiO₂ ALD films by resonant photoelectron spectroscopy. We identify intrinsic defects which are responsible for the active sites in interface reactions, for the incorporation of intrinsic charges, and for the formation of local dipole momenta. All of these features determine the surface potentials and the reactivity of the surface of the atomic layer deposition coated systems. We give examples of charges and dipoles in Al₂O₃, on a study of the surface potentials in HfO₂, and relate the intrinsic defects in TiO₂ to their electrochemical relevance.}, language = {en} } @misc{SchmeisserHenkelJanowitz, author = {Schmeißer, Dieter and Henkel, Karsten and Janowitz, Christoph}, title = {Ionicity of ZnO - a key system for transparent conductive oxides}, series = {epl : a letters journal exploring the frontiers of physics}, volume = {123}, journal = {epl : a letters journal exploring the frontiers of physics}, number = {2}, issn = {1286-4854}, doi = {10.1209/0295-5075/123/27003}, pages = {27003-p1 -- 27003-p7}, abstract = {The electronic structure of ZnO is dominated by coexisting electron and ionic states/bonds caused by charge polarization and self-trapping phenomena of the valence charges. Their interplay manifests itself in intrinsic electronic defects which have different degree of spatial localization and electronic correlation. The relative abundance of intrinsic defects can be determined by the ionicity factor fi and its value can be derived from three independent experimental procedures in a consistent way. This approach also explains the complex satellite features in the XPS and XAS data. Ionicity and satellite formation are two experimental findings which can be explained consistently in the same context of mixed-atomic valence states and intrinsic electronic defects.}, language = {en} } @misc{KotKegelmannDasetal., author = {Kot, Małgorzata and Kegelmann, Lukas and Das, Chittaranjan and Kus, Peter and Tsud, Nataliya and Matol{\´i}nov{\´a}, Iva and Albrecht, Steve and Matolin, Vladimir and Schmeißer, Dieter}, title = {Room temperature atomic layer deposited Al₂O₃ improves perovskite solar cells efficiency over time}, series = {ChemSusChem}, volume = {11}, journal = {ChemSusChem}, number = {20}, issn = {1864-5631}, doi = {10.1002/cssc.201801434}, pages = {3640 -- 3648}, abstract = {Electrical characterisation of perovskite solar cells consisting of room-temperature atomic-layer-deposited aluminium oxide (RT-ALD-Al₂O₃) film on top of a methyl ammonium lead triiodide (CH₃NH₃PbI₃) absorber showed excellent stability of the power conversion efficiency (PCE) over along time. Under the same environmental conditions (for 355 d), the average PCE of solar cells without the ALD layer decreased from 13.6 to 9.6 \%, whereas that of solar cells containing 9 ALD cycles of depositing RT-ALD-Al₂O₃on top of CH₃NH₃PbI₃ increased from 9.4 to 10.8 \%. Spectromicroscopic investigations of the ALD/perovskite interface revealed that the maximum PCE with the ALD layer is obtained when the so-called perovskite cleaning process induced by ALD precursors is complete. The PCE enhancement over time is probably related to a self-healing process induced by the RT-ALD-Al₂O₃ film. This work may provide a new direction for further improving the long-term stability and performance of perovskite solar cells.}, language = {en} } @incollection{HenkelHaeberleMuelleretal., author = {Henkel, Karsten and Haeberle, J{\"o}rg and M{\"u}ller, Klaus and Janowitz, Christoph and Schmeißer, Dieter}, title = {Preparation, properties and electronic structure of SnO₂}, series = {Single Crystals of Electronic Materials}, booktitle = {Single Crystals of Electronic Materials}, editor = {Fornari, Robert}, publisher = {Elsevier, Woodhead Publishing}, address = {Duxford}, isbn = {978-0-08-102096-8}, pages = {547 -- 572}, abstract = {This chapter reports about tin oxide (SnO₂), a material which belongs to the transparent conducting oxide family and is best characterized by its high conductivity, high carrier mobility, and the ability to form p-type conductivity. We correlate these properties in terms of localized intrinsic electronic defect states which are resolved by resonant photoelectron spectroscopy measurements. We describe SnO₂ in terms of an inhomogeneous, mixed-ionic-covalent semiconductor in which these intrinsic electronic defects state are stabilized.}, language = {en} } @misc{MaityGarainHenkeletal., author = {Maity, Kuntal and Garain, Samiran and Henkel, Karsten and Schmeißer, Dieter and Mandal, Dipankar}, title = {Natural Sugar-Assisted, Chemically Reinforced, Highly Durable Piezoorganic Nanogenerator with Superior Power Density for Self-Powered Wearable Electronics}, series = {ACS Applied Materials \& Interfaces}, volume = {10}, journal = {ACS Applied Materials \& Interfaces}, issn = {1944-8244}, doi = {10.1021/acsami.8b15320}, pages = {44018 -- 44032}, abstract = {Natural piezoelectric materials are of increasing interest, particularly for applications in biocompatible, implantable, and flexible electronic devices. In this paper, we introduce a cost-effective, easily available natural piezoelectric material, that is, sugar in the field of wearable piezoelectric nanogenerators (PNGs) where low electrical output, biocompatibility, and performance durability are still critical issues. We report on a high-performance piezoorganic nanogenerator (PONG) based on the hybridization of sugar-encapsulated polyvinylidenefluoride (PVDF) nanofiber webs (SGNFW). We explore the crucial role of single-crystal sugar having a fascinating structure along with the synergistic enhancement of piezoelectricity during nanoconfinement of sugar-interfaced macromolecular PVDF chains. As a consequence, the SGNFW-based PONG exhibits outstanding electricity generation capability (e.g.,∼100 V under 10 kPa human finger impact and maximum power density of 33 mW/m2) in combination with sensitivity to abundantly available different mechanical sources (such as wind flow, vibration, personal electronics, and acoustic vibration). Consequently, it opens up suitability in multifunctional self-powered wearable sensor designs for realistic implementation. In addition, commercially available capacitors are charged up effectively by the PONG because of its rapid energy storage capability. The high performance of the PONG not only offers"battery-free"energy generation (several portable units of light-emitting diodes and a liquid crystal display screen are powered up without using external storage) but also promises its use in wireless signal transmitting systems, which widens the potential in personal health care monitoring. Furthermore, owing to the geometrical stress confinement effect, the PONG is proven to be a highly durable power-generating device validated by stability test over 10 weeks. Therefore, the organic nanogenerator would be a convenient solution for portable personal electronic devices that are expected to operate in a self-powered manner.}, language = {en} } @misc{BiswasGarainMaityetal., author = {Biswas, Anirban and Garain, Samiran and Maity, Kuntal and Henkel, Karsten and Schmeißer, Dieter and Mandal, Dipankar}, title = {Influence of In situ Synthesized Bismuth Oxide Nanostructures in Self-poled PVDF-based Nanogenerator for Mechanical Energy Harvesting Application}, series = {Polymer Composites}, volume = {40}, journal = {Polymer Composites}, number = {S1}, issn = {0272-8397}, doi = {10.1002/pc.24628}, pages = {E265 -- E274}, abstract = {A self-poled piezoelectric nanogenerator (NG) based on bismuth oxide (Bi2O3) nanostructures (BNS)-doped poly(vinylidene fluoride) (PVDF) is demonstrated. The in-situ formation of BNS incorporated in the PVDF matrix is realized through a simple solution casting technique that favors the nucleation and stabilization of 99.6\% of the electroactive phase in PVDF (i.e., beta/gamma-phases). The enhancement of the output voltage (3.6 V) and current (2.4mA) of the NG based on a nonelectrically poled BNS containing PVDF composite film is achieved and demonstrated by simple repeated human finger imparting. The improvement of the output performance is influenced by the generation of the electroactive polar beta-phase in PVDF, due to the electrostatic interactions between the -CH2-/-CF2- dipoles of PVDF and the surface charge of the BNS. The NGs are able to charge up capacitors demonstrating that the power generation from such a hybrid device structure can be utilized for powering various portable devices.}, language = {en} } @misc{KotHenkelNaumannetal., author = {Kot, Małgorzata and Henkel, Karsten and Naumann, Franziska and Gargouri, Hassan and Tarnawska, Lidia Lupina and Wilker, Viola and Kus, Peter and Pożarowska, Emilia and Garain, Samiran and Rouissi, Zied and Schmeißer, Dieter}, title = {Comparison of plasma-enhanced atomic layer deposition AlN films prepared with different plasma sources}, series = {Journal of Vacuum Science and Technology A}, volume = {37}, journal = {Journal of Vacuum Science and Technology A}, number = {2}, issn = {0734-2101}, doi = {10.1116/1.5079628}, pages = {11}, abstract = {A comparative study of thin aluminum nitride (AlN) films deposited by plasma-enhanced atomic layer deposition in the SENTECH SI ALD LL system applying either a direct inductively coupled plasma (ICP) or an indirect capacitively coupled plasma (CCP) source is presented. The films prepared with the ICP source (based on a planar triple spiral antenna) exhibit improved properties concerning the growth rate per cycle, total cycle duration, homogeneity, refractive index, fixed and mobile electrical charges, and residual oxygen content compared to the CCP source, where the comparison is based on the applied plasma power of 200 W. The increase of the plasma power to 600 W in the ICP process significantly reduces the residual oxygen content and enhances the electrical breakdown field. The AlN layers grown under these conditions, with a growth rate per cycle of 1.54 {\AA}/cycle, contain residual oxygen and carbon concentrations of about 10\% and 4\%, respectively, and possess a refractive index of 2.07 (at 632.8 nm).}, language = {en} } @misc{KotwicaDomaradzkiWojcieszaketal., author = {Kotwica, Tomasz and Domaradzki, Jarosław and Wojcieszak, Damian and Sikora, Andrzej and Kot, Małgorzata and Schmeißer, Dieter}, title = {Analysis of surface properties of Ti-Cu-Ox gradient thin films using AFM and XPS investigations}, series = {Materials Science-Poland}, volume = {36}, journal = {Materials Science-Poland}, number = {4}, issn = {0137-1339}, doi = {10.2478/msp-2018-0100}, pages = {761 -- 768}, abstract = {The paper presents results of investigations on surface properties of transparent semiconducting thin films based on (Ti-Cu)oxide system prepared using multi-magnetron sputtering system. The thin films were prepared using two programmed profiles of pulse widt hmodulation coefficient, so called V- and U-shape profiles. The applied powering profiles allowed fabrication of thin films with gradient distribution of Ti and Cu elements over the thickness of deposited layers. Optical investigations allowed determination of transparency of prepared films that reached up to 60 \% in the visible part of optical radiation, which makes them attractive for the transparent electronics domain. Surface properties investigations showed that the surface of mixed (Ti-Cu)oxides was sensitive to adsorption, in particular to carbon dioxide and water vapor. Soft etching with argon ions resulted in surface cleaning from residuals, however, deoxidation of Cu-oxide components was also observed.}, language = {en} } @misc{JanowitzSchmeisser, author = {Janowitz, Christoph and Schmeißer, Dieter}, title = {Out-of-plane electronic contributions in Bi-cuprates studied by resonant photoelectron spectroscopy at the Cu 2p edge}, series = {Verhandlungen der DPG}, journal = {Verhandlungen der DPG}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {403 -- 403}, abstract = {In high-temperature superconductors with a layered crystal structure out-of-plane contributions are often neglected, while the copper-oxygen planes are commonly considered to dominate the electronic properties around the Fermi energy. Here we report on a resonant photoemission study of (Pb,Bi)2201 and (Pb,Bi)2212 single crystals to unravel the resonant decay mechanisms at the Cu 2p absorption edge. We demonstrate a pronounced polarization dependence caused by two different Auger processes for in-plane and out-of-plane orientations. We deduce that the lowest energy valence state being involved in the two Auger processes, consists of three-dimensional contributions by admixed out-of-plane Sr, Bi, and O 2p states. It also suggests that the doping-induced charge density is dynamic, fluctuating within the Cu-O plane, and spills out perpendicular to it. C. Janowitz and D. Schmeißer, Supercond. Sci. Technol. 31, 045006 (2018)}, language = {en} } @misc{MahmoodinezhadPożarowskaHenkeletal., author = {Mahmoodinezhad, Ali and Pożarowska, Emilia and Henkel, Karsten and Schmeißer, Dieter and Flege, Jan Ingo}, title = {Depth profiling of PEALD-AlN films based on Al2p XPS peak decomposition}, series = {Verhandlungen der DPG}, journal = {Verhandlungen der DPG}, publisher = {Deutsche Physikalische Gesellschaft}, address = {Bad Honnef}, issn = {0420-0195}, pages = {157 -- 157}, abstract = {AlN has remarkable properties (wide band gap, low electrical and thermal conductivity, high dielectric constant, piezoelectricity) and is attractive for (opto)electronic and sensor applications. However, high oxygen content within nitride films is always a critical issue due to the thermodynamically favorable oxidation against nitridation resulting in deteriorated materials properties. In order to clarify whether the oxidation is a surface-limited or a bulk process elemental depth profiling is essential. In this work XPS in combination with Ar+ sputtering is applied to carry out depth profiling of AlN films prepared by plasma-enhanced atomic layer deposition using different parameters (plasma source, power and pulse duration). Particularly, the Al2p core levels are analyzed where the signals are decomposed into four components, representing weaker contributions of pure AlN and aluminum oxide phases as well as stronger signals of mixed oxygen-rich and nitrogen-rich phases. After sputtering (providing access to the deeper part of the film) the pure AlN phase content increases while the pure aluminum oxide content stays relatively constant. These issues are discussed with regard to the preparation parameters employed and accompanying XRD and electrical measurements.}, language = {en} } @misc{RoyGhoshSultanaetal., author = {Roy, Krittish and Ghosh, Sujoy Kumar and Sultana, Ayesha and Garain, Samiran and Xie, Mengying and Bowen, Christopher Rhys and Henkel, Karsten and Schmeißer, Dieter and Mandal, Dipankar}, title = {A Self-Powered Wearable Pressure Sensor and Pyroelectric Breathing Sensor Based on GO Interfaced PVDF Nanofibers}, series = {ACS Applied Nano Materials}, volume = {2}, journal = {ACS Applied Nano Materials}, number = {4}, issn = {2574-0970}, doi = {10.1021/acsanm.9b00033}, pages = {2013 -- 2025}, abstract = {This paper reports a self-powered,flexible, piezo- and pyro-electric hybrid nanogenerator (NG) device that can be fixed on different locations of human skin for detecting static and dynamic pressure variations and can also monitor temperature fluctuations during the respiration process. An efficient and cost-effective fabrication strategy has been developed to create electrospun poly(vinylidene fluoride) (PVDF)/graphene oxide (GO) nanofibers, which are used to create a highly sensitive wearable pressure sensor and pyroelectric breathing sensor. The sensor can accurately and rapidly detect pressures as low as 10 Pa with a high sensitivity (4.3 V/kPa), a key performance indicator for wearable sensors. Importantly, the sensor exhibits a high sensitivity to bending and stretching by finger, wrist, and elbow. The pressure sensor is also highly sensitive to vocal vibrations when attached to the human throat. The device can generate a maximum output power density of∼6.2 mW/m2 when subjected to a compressive stress, which enhances its range of applications. Moreover, it is demonstrated that doping with GO improves the pyroelectric energy harvesting and sensing performance of the device under repeated temperature fluctuations. The PVDF/GO-based nanogenerator has a maximum pyroelectric output power density of∼1.2 nW/m2 and can sense temperature changes during respiration, which makes it promising as a pyroelectric breathing sensor. It is demonstrated that processing of the PVDF-GO self-powered multifunctional pressure and pyroelectric breathing sensor can be up-scaled for fabricating compact and high-performance electronic skins for application in health monitoring, motion detection, and portable electronics.}, language = {en} } @misc{ObstarczykKaczmarekWojcieszaketal., author = {Obstarczyk, Agata and Kaczmarek, Danuta and Wojcieszak, Damian and Mazur, Michał and Domaradzki, Jarosław and Kotwica, Tomasz and Pastuszek, Roman and Schmeißer, Dieter and Mazur, Piotr and Kot, Małgorzata}, title = {Tailoring optical and electrical properties of thin-film coatings based on mixed Hf and Ti oxides for optoelectronic application}, series = {Materials and Design}, volume = {175}, journal = {Materials and Design}, issn = {0264-1275}, doi = {10.1016/j.matdes.2019.107822}, pages = {15}, abstract = {In this work multi-magnetron sputtering stand was used for the deposition of the mixed oxides thin films based on HfO2 and TiO2. In order to obtain various material composition the power released to each magnetron (containing metallic hafnium and titanium targets) was precisely selected. Structural, surface, optical, electrical and mechanical properties of as-deposited coatings were analyzed. Depending on the hafnium content in the deposited thin films various types of the microstructure was obtained, i.e. HfO2-monoclinic, amorphous and TiO2-rutile. Increase of Ti content above 28 at. \% in the as-prepared mixed oxides coatings caused their amorphization. It was found that with an increase of Ti content in prepared coatings their surface roughness and simultaneously water contact angle decreased. Performed measurements of electrical properties revealed that the lowest leakage current density in the range of 10-7 - 10-8 A/cm2 was obtained for amorphous coatings. Moreover, the tailoring of the dielectric constant was possible by a proper selection of material composition and microstructure of the deposited thin films. Average transparency in the visible wavelength region was in the range of ca. 79-86\%. The influence of material composition and structure on shifting of the fundamental absorption edge and optical bandgap energy was also observed. The refractive index increased with an increase of Ti content, while extinction coefficient was the lowest for amorphous coatings. Additionally, hardness values were dependent on the material composition and optical packing density and were in the range from 7.6 GPa to 10.1 GPa.}, language = {en} } @misc{MuellerRachowGuentheretal., author = {M{\"u}ller, Klaus and Rachow, Fabian and G{\"u}nther, Vivien and Schmeißer, Dieter}, title = {Methanation of Coke Oven Gas with Nickel-based catalysts}, series = {International Journal of Environmental Science}, journal = {International Journal of Environmental Science}, number = {4}, issn = {2367-8941}, pages = {73 -- 79}, abstract = {For a complete transition from fossil to CO₂ neutral energy supply new energy storage concepts are needed that allow energy supply in times of absence of regenerative power production as during dark doldrums. A promising renewable energy storage approach is the power to gas (to power) technique based on the production of synthetic natural gas (also called e-methane) by methanation of CO₂ with H₂. The latter is usually produced by electrolysis. In any power to gas concept, electrolysis is a very critical part, due to its high costs, stability issues, or limited power of required electrolysers. As an alternative source of hydrogen, we investigate the methanation of coke oven gas (COG). COG is a byproduct of the carbon rich coke production from coal for the steel industry, with a high amount of hydrogen (~60vol\%). Coke oven gas furthermore contains CH₄(~25vol\%), CO (5-8vol\%), and CO₂(1-3vol\%), making it an attractive feedstock for the production of synthetic energy carriers like methane. In the present study, the authors investigate the direct conversion of CO and CO₂ from COG into e-methane. Compared to stoichiometric conversion, the COG hydrogen content is too high for catalytic methanation of CO₂. In order to achieve a higher methane yield, the addition of CO₂ from air, flue gas, or coal gasification can compensate the surplus of hydrogen in the coke oven gas. The process is evaluated by the conversion of CO and CO₂, the catalyst selectivity towards higher hydrocarbons for varying temperatures, and the CH₄ yield.}, language = {en} } @misc{SchmeisserHenkelPożarowskaetal., author = {Schmeißer, Dieter and Henkel, Karsten and Pożarowska, Emilia and Kegelmann, Lukas and Tsud, Nataliya and Kot, Małgorzata}, title = {Point Defect-Mediated Interface Formation and Appearance of a Cooper Minimum for AlOₓ Atomic-Layer-Deposited Films on CH₃NH₃PbI₃}, series = {The Journal of Physical Chemistry. C}, volume = {123}, journal = {The Journal of Physical Chemistry. C}, number = {38}, issn = {1932-7447}, doi = {10.1021/acs.jpcc.9b05282}, pages = {23352 -- 23360}, abstract = {We report on the interaction of CH₃NH₃PbI₃ substrates with AlOx films prepared by atomic layer deposition at room temperature. We use synchrotron radiation-based photoemission spectroscopy and study the Pb 4f, I 3d, and Al 2p core levels as well as the corresponding valence band states (Pb 5d and O 2p). A Cooper minimum is observed for both the Pb 5d and O 2p states, and it indicates that the bonding at the interface must be covalent. We focus on the electronic properties of the substrate and its interface and identify a delicate charge balance between polaronic and excitonic states in MAPI and AlOₓ. The perovskite vacancy sites, identified by changes in the core-level intensities, mediate the charge balance and covalent interaction.}, language = {en} } @misc{KotHenkelMuelleretal., author = {Kot, Małgorzata and Henkel, Karsten and M{\"u}ller, Klaus and Kegelmann, Lukas and Albrecht, Steve and Tsud, Nataliya and K{\´u}s, Peter and Matolinov{\´a}, Iva and Schmeißer, Dieter}, title = {Al2O3-Atomic Layer Deposited Films on CH3NH3PbI3 : Intrinsic Defects and Passivation Mechanisms}, series = {Energy Technology , The Journal of Physical Chemistry C}, volume = {7}, journal = {Energy Technology , The Journal of Physical Chemistry C}, number = {11}, issn = {2194-4288}, doi = {10.1002/ente.201900975}, pages = {10}, abstract = {The initial interaction of atomic layer deposited films of Al2O3 at room temperature on CH3NH3PbI3 (MAPI) films is studied. Synchrotron radiation-based photoelectron spectroscopy is applied to analyze the initial changes in the Al-derived features by comparing samples with different Al2O3 film thicknesses. It is found that polarons and excitons, both intrinsic defects of Al2O3, play a key role in the interface formation. The polaronic states uptake a charge from the MAPI substrate. This charge is transferred to and stabilized in the excitonic state of Al2O3 which is assigned to predominately tetrahedral coordinated Al sites. This charge transfer is initiated by vacancies present in the MAPI substrate and stabilizes a covalent bonding at the Al2O3-MAPI interface but also causes a roughening of the interface which may lead to the formation of grain boundaries. On top of the rough interface, 2D Al2O3 clusters with an increasing number of octahedrally coordinated Al—O bonds grow, and with increasing Al2O3 coverage, they introduce self-healing of the structural defects.}, language = {en} } @misc{MahmoodinezhadJanowitzNaumannetal., author = {Mahmoodinezhad, Ali and Janowitz, Christoph and Naumann, Franziska and Plate, Paul and Gargouri, Hassan and Henkel, Karsten and Schmeißer, Dieter and Flege, Jan Ingo}, title = {Low-temperature growth of gallium oxide thin films by plasma-enhanced atomic layer deposition}, series = {Journal of Vacuum Science and Technology A}, volume = {38}, journal = {Journal of Vacuum Science and Technology A}, number = {2}, issn = {0734-2101}, doi = {10.1116/1.5134800}, abstract = {Gallium oxide (Ga2O3) thin films were deposited by plasma-enhanced atomic layer deposition (PEALD) applying a capacitively coupled plasma source where trimethylgallium (TMGa) as the gallium precursor and oxygen (O2) plasma were used in a substrate temperature (Ts)in the range of 80-200 °C. TMGa exhibits high vapor pressure and therefore facilitates deposition at lower substrate temperatures. The Ga2O3 films were characterized by spectroscopic ellipsometry (SE), x-ray photoelectron spectroscopy (XPS), and capacitance-voltage (C-V) measurements. The SE data show linear thickness evolution with a growth rate of ∼0.66 {\AA} per cycle and inhomogeneity of ≤2\% for all samples. The refractive index of the Ga2O3 thin films is 1.86 ± 0.01 (at 632.8 nm) and independent of temperature, whereas the bandgap slightly decreases from 4.68 eV at Ts of 80 °C to 4.57 eV at 200 °C. XPS analysis revealed ideal stoichiometric gallium to oxygen ratios of 2:3 for the Ga2O3 layers with the lowest carbon contribution of ∼10\% for the sample prepared at 150 °C. The permittivity of the layers is 9.7 ± 0.2 (at 10 kHz). In addition, fixed and mobile oxide charge densities of 2-4E12 and 1-2E12 cm-2, respectively, were observed in the C-V characteristics. Moreover, the Ga2O3 films show breakdown fields in the range of 2.2-2.7 MV/cm. Excellent optical and electrical material properties are maintained even at low substrate temperatures as low as 80 °C. Hence, the TMGa/O2 PEALD process is suitable for electronic and optoelectronic applications where low-temperature growth is required.}, language = {en} }