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- X-ray photoelectron spectroscopy (XPS) (20)
- atomic layer deposition (18)
- resonant photoelectron spectroscopy (16)
- atomic layer deposition (ALD) (13)
- PVDF (12)
- X-ray photoelectron spectroscopy (12)
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- water splitting (9)
Institute
Metallic Single-Crystal CoSi Nanowires via Chemical Vapor Deposition of Single-Source Precursor
(2006)
Microscopic and spectroscopic characterization of interfaces and dielectric layers for OFET devices
(2009)
Ultra-thin homogeneous oxynitride films are prepared on Si(001). The Si surface is cleaned in UHV by heating (flashing) and is exposed to different pressures of N2Oat altered temperatures. Thus oxynitride layers of different thickness and different properties are grown depending on the N2O pressure and the Si temperature. This isillustrated by a schematic diagram. The properties of the different oxynitride layers were studied by a combined photoemission electron microscopy (PEEM) andphotoelectron spectroscopy (PES) investigation using highly monochromatic synchrotron radiation. The amount of oxygen and nitrogen incorporated in the oxynitridelayers is determined from the PES measurements. The typical surface morphology for different preparation conditions is shown in PEEM images.
Photo-Emission-Electron-Microscopy for Characterization of an Operating Organic Electronic Device
(2006)
In this contribution we report on investigations of the electronic structure and composition of regioregular poly(3-hexylthiophene) (P3HT) and phenyl-C61-butyric acid methyl ester (PCBM) based films by using Near Edge X-Ray Absorption Fine Structure (NEXAFS). The measurements were done at the U49/2-PGM2 beam line of BESSY II, Berlin using TEY (total electron yield) and TFY (total fluorescence yield) detection. The samples were produced by spin casting a mixture of P3HT (dissolved in chloroform) and PCBM (dissolved in chlorobenzene) on ITO (indium tin oxide) coated glass slides. Measurements of pure P3HT and PCBM show all typical excitations, whereas the blended system is a weighted superposition of the related peaks. Analyzing these weighted superposition, we observe in the surface sensitive TEY data an accumulation of P3HT, whereas in the bulk sensitive TFY signal an as expected mixture is found. We also show angular dependent NEXAFS measurements of the P3HT/PCBM blend in order to measure the orientation and distribution of the P3HT polymer. Additionally, we will show a new approach for organic solar cell application by introducing ferroelectric nanoparticles into the mixture.
Replacing Co by large amounts of Ni is considered to reduce costs in Li-Ion-Batteries while maintaining their performance. We are interested in whether this replacement causes changes in the valence band (VB) and conduction band (CB) states or not.
Samples were prepared as thin films from nitrate solutions on metal substrates and annealed in air and UHV. The Co to Ni ratio was varied from 50/50 over 40/60 and 30/70 up to 20/80. The results are compared to the pure Co-oxide. Experiments were carried out at the U49/2 beamline at BESSYII, Berlin.
XPS of the TM2p states reveals the existence of charge transfer ground states and different oxidation states. NEXAS at the Co2p, Ni2p and O1s edges projects the density of unoccupied states while resonant PES at these edges provides the related partial density of states (pDOS) and thus can be used to distinguish between the different contributions of TM3d and O2p states in the valence band region.
We find systematic variation of the VB structure, the valence band maximum and a shift at the O1s absorption edge while the TM2p XPS and absorption spectra do not seem to be affected by the mixing.
We investigated several layered perovskite derivatives of the family AnBnO3n+2, such as LaTiO3.41, CaNbO3.41 and SrNbO3.41, which can be considered as a stacking of blocks consisting of 5 perovskite layers. Electric transport across these layers takes place via intrinsic tunnelling. Mesa devices with a cross-sectional area of 50 to 200 µm2 and a height between 30 and 500 nm were fabricated by electron-beam lithography and ion-beam etching. Both dc I-V characteristics and pulsed current injection have shown switching between different resistive states in these materials. The resistive states have long-term stability, which makes them interesting for memory applications. The transport experiments suggest that switching and resistive memory are controlled by trapping and release of charge carriers. Furthermore, photoelectron and NEXAFS spectroscopy of cleaved LaTiO3.41 surfaces have been performed. The results are compared to recent correlated band theory (LDA+U) calculations.
Scanning Kelvin probe and photoemission electron microscopy of organic source-drain structures
(2004)
The TiO2 films are prepared by atomic layer deposition (ALD) method using titanium
isopropoxide precursors at 250 °C and analyzed using resonant photoemission spectroscopy (resPES). We report on the Ti2p and O1s core levels, on the valence band (VB) spectra and
x-ray absorption spectroscopy (XAS) data, and on the resonant photoelectron spectroscopy (resPES) profiles at the O1s and the Ti3p absorption edges. We determine the elemental
abundance, the position of the VB maxima, the partial density of states (PDOS) in the VB and in the conduction band (CB) and collect these data in a band scheme. In addition, we analyze the band-gap states as well as the intrinsic states due to polarons and charge-transfer
excitations. These states are found to cause multiple Auger decay processes upon resonant
excitation. We identify several of these processes and determine their relative contribution to the Auger signal quantitatively. As our resPES data allow a quantitative analysis of these defect states, we determine the relative abundance of the PDOS in the VB and in CB and also the charge neutrality level.
The anatase and rutile polymorphs of TiO2 are analyzed in the same way as the TiO2 ALD layer. The electronic properties of the TiO2ALD layer are compared with the anatase and rutile polymorphs of TiO2. In our comparative study, we find that ALD has its own
characteristic electronic structure that is distinct from that of anatase and rutile. However, many details of the electronic structure are comparable and we benefit from our spectroscopic
data and our careful analysis to find these differences. These can be attributed to a stronger hybridization of the O2p and Ti3d4s states for the ALD films when compared to the anatase and rutile polymorphs.
Wir haben CuInS2 (CIS) unterschiedlicher Herstellung (Koverdampfung, Sputtern, Pulsed Laser Deposition, CIS auf Kupferband aufgebracht) untersucht. Neben Tiefenprofilen (durch Sputtern) der Elementverteilung dieser Proben wurden der Einfluss der Temperatur, von aufgedampftem Kupfer und Indium, ebenfalls bei verschiedenen Temperaturen, auf das Verhalten der Stöchiometrie mit spektroskopischen Methoden (XPS, UPS) studiert. Parallel dazu wurde das Verhalten von im Vakuum aufgedampften ZnS und die entsprechenden Oberflächenreaktionen in Abhängigkeit von der Temperatur untersucht und charakterisiert, so dass Aussagen über die Optimierung und Anpassung von Präparationsbedingungen und Parametern zur Herstellung von erstens reinem CIS und zweitens von Mischkristallen des Typs Zn2-xCuxInxS2 möglich werden. Zwischen den beiden Endgliedern ZnS und CuInS2 besteht bis auf einen Phasenübergang bei etwa 80% CIS lückenlose Mischbarkeit gemäss Zn2-xCuxInxS2 (Bente: Chem.Erde (1991)). Die elektronische Bandlücke dieser Mischkristalle lässt sich im Vergleich zu reinem CuInS2 in einem Bereich von 3,67 eV (ZnS) bis 1,55 eV (CuInS2) variieren. Damit besteht die Möglichkeit, durch kontrollierte Änderung der Zusammensetzung der Schichten die Effizienz von Solarzellen aus diesem Material zu optimieren.
Due to the growing range of applications for organic materials considerable interest has been focused on the controlled growth of films on silicon substrates. Recently, it has been shown that ultra-thin oligimide films can be grown on Si(100)-2x1 with a direct Si-C linkage to the substrate. In this study, we have focused on the chemisorption of maleic anhydride (C4O3H2) on Si(100)-2x1. The combined HREELS data indicate that the adsorption of maleic anhydride on Si(100)-2x1 at low dosages occurs mainly through cycloaddition of the C=C bond to the dangling bonds of the Si-Si dimer analogous to the behaviour of ethene. The Si-Si dimer bonds are not involved in the chemisorption, as the continued observation of a 2x1 pattern in LEED shows. In the NEXAFS spectra, a π* resonance indicative of a C=C bond is absent upon exposure of the silicon substrate to maleic anhydride. At higher dosages, we observe chemisorbed maleic anhydride species, which are bonded to the Si surface atoms via a single Si-C linkage with preservation of the C=C double bond. In this case, the dissociated hydrogen bonds to one of the neighbouring Si atoms. Possible adsorption geometries will be discussed.
Es werden spektro-mikroskopische Untersuchungen an multikristallinem Silizium (mc-Si) vorgestellt, einem aussichtsreichen Material für die Herstellung preiswerter Solarzellen. Dazu wird ein Photoemissions- Elektronenmikroskop (PEEM) ausgestattet mit einem zusätzlichen Energieanalysator für Elektronen (µESCA) genutzt. Bei Verwendung eines Synchrotrons als Anregungsquelle ist es so möglich, sowohl Absorbtions-Spektren (NEXAFS) als auch Photoelektronen-Spektren (PES) mit Ortsauflösung zu erhalten.
Dabei wird gezeigt, dass das natürliche Oxid zur Untersuchung der morphologie-abhängigen Oberflächenpotentiale nicht entfernt werden muss. Des Weiteren wird die Verteilung von Ca- und Na-Ausscheidungen, die auf dem mc-Si gefunden wurden, durch ortsaufgelöstes NEXAFS bzw. PES dargestellt.
Für den Photoemissions-Prozess des mc-Si im PEEM wird ein Modell aufgestellt, welches Photoemission mit einer Quecksilberdampflampe (hνmax = 4,9 eV) erklärt.
Conducting Polypyrrole doped with Phthalocyaninesulfonates - new materials for chemical sensors
(2000)
Polypyrrole - a conducting polymer - is used as an active electrode of a quartz micro ballance and considered as a gate electrode in all-polymer field effect transistors used as chemical sensor. We use substituted phthalocyanines as dopants of polypyrrole as they offer the possibility to enhance the dopant concentration as well as to include functionalized groups. We studied these films by photoelectron spectroscopy, NEXAFS, PEEM, and TEM. These investigations revealed that the electronic structure as well as the morphology are highly dependent on the dopant’s structure. We suggest a new charge transport model for 5-ring heterocycle conductive polymers. Whereas in the standard model only the carbon backbone is considered for the charge transport, we found by NEXAFS investigations that the heteroatom has a considerable high participation in the gap states, which are responsible for the charge transport. The dopants π-interactions force the nitrogen lone pair wave functions to contribute to the conducting polymer π-system. This is a novel approach concerning the application as chemical sensors since the reversible interaction of the analyte modifies the dopant and not the matrix.
Es werden Untersuchungen an als Hochtemperatur-Sensoren arbeitenden Schottky-Dioden mit dem Aufbau Metall-Oxidschicht-Siliziumkarbid vorgestellt. Dazu wurden Tiefenprofile mit XPS durch abwechselndes Abtragen durch Sputtern und Messen erstellt. Die Messungen erfolgten an thermisch unterschiedlich vorbehandelten Proben. Dabei konnten dipol-bedingte Verschiebungen der Bindungsenergie von Rumpfniveaus beobachtet werden. Das dazu notwendige Dipol-Moment wird durch das Entstehen von mit einer Oxidschicht überzogenen Nanoteilchen erklärt. Die unterschiedlich ausgeprägten Dipol-Verschiebungen auf den einzelnen Proben erlaubten eine Erklärung der thermischen Vorbehandlung, die bei Weglassen zu „frischen“ und je nach Temperatur zu „aktivierten“ oder „toten“ Sensoren führte.
Untersuchungen des metallischen Kontaktes von Silber auf tosylat- und phthalocyanindotiertem Polypyrrol wurden mittels XPS- und µ-NEXAFS vorgenommen. Es wurde festgestellt, daß Silber mit dem Polypyrrol keine Verbindung eingeht. Daraus kann geschlossen werden, daß sowohl das leitfähige Polymer, als auch das Silber ihren Leitfähigkeitsmechanismus beibehalten. Es konnte gezeigt werden, daß bei steigender Silberbelegung die Intensität der Polaronenzustände des Polypyrrol in stärkerem Maße abnimmt, als die Intensität der unbesetzten Zustände. Das läßt darauf schließen, daß Silber die Grenzfläche stabilisiert.
Vorgestellt werden Arbeiten an dünnen WO3-Schichten, die durch Verdampfen aus einer Knudsenzelle im UHV präpariert wurden. Diese Filme sind im Rahmen der XPS-Analysen stöchiometrisch, ohne Gap-Zustände. Definierte Gap-Zustände bilden sich durch Relaxierung der Oberfläche: nach einigen Stunden im UHV, nach Heizen in Argon-Atmosphäre und nach Belegung mit Natrium. Die Charakterisierung dieser definierten Wolframoxid-Schichten erfolgt durch: 1.)XPS-Intensitäten 2.)detailierte Analyse der W4f-Rumpfniveaus durch Synchrotronstrahlung (Bessy, TGM 7) 3.)die Variation der Austrittsarbeit beim Heizen und bei Natrium-Belegung 4.)das Auftreten von Gap-Zuständen in der Bandlücke
Molybdänditellurid (MoTe2) gehört zu den Schichtgitterverbindung und ist im allgemeinen durch den Herstellungsprozeß n-dotiert. Proben dieses MoTe2 wurden im Ultrahochvakuum gespalten und die so erhaltenen sauberen (0001)-Spaltflächen mit einem Photoemissions-Elektronenmikroskop (PEEM) untersucht. Diese Untersuchung erbrachte nebeneinander auf den Proben- oberflächen liegende stark kontrastierte helle und dunkle Bereiche. Da das PEEM Austrittsarbeitsunterschiede als Kontrast darstellt, können diese hellen und dunklen Bereiche auf lokale Unterschiede in der Austrittsarbeit zurückgeführt werden. Weiterhin wird über den Versuch berichtet, eine Zuordnung zwischen dem Kontrast und dem Unterschied in der Austrittsarbeit mit Hilfe eines Elektronenenergie-Analysators (micro-ESCA) zu treffen.
Titanium oxynitride (TiON) films are interesting due to their remarkable optical and electronic properties which strongly depend on the O/N ratio. However, it is known that films containing Ti are prone to oxidation in contact with the air [1]. In this work, we study the thickness of a surface oxidation layer which is inherently formed on
the atomic layer deposition (ALD) grown TiON/TiN films on Si substrate. We use an Ar+
ion bombardment source and X-ray photoelectron spectroscopy (XPS) for this analysis. We calibrate the sputter rate by using substrate signal intensity decay (here Si 2p) in the XPS
spectra of the 5 nm thick TiON sample accordingly. This rate is assumed to be constant when films with a larger thickness are analyzed. We find that the surface oxidation layer is about 1 nm thick, independent on the detailed ALD parameters of the films. The TiN films found underneath are close to the stoichiometric values and have a residual O content below 5%. Finally, we compare these data to our previous
results collected with synchrotron-based radiation source [2,3].
References: [1] Sowinska et al., Applied Physics Letters 100, 233509
(2012). [2] M. Sowinska et al., Applied Surface Science 381, 42-47 (2016). [3] M. Sowińska et al., Journal of Vacuum Science and Tech-
nology A, 01A12734 (2016).
We report on a resonant photoemission (resPES) study of PbxBi2-xSr2-yLayCan-1CunO2n+4+d (BISCO) single
crystals to unravel the resonant decay mechanisms at the Cu2p absorption edge. The resPES studies on
superconducting BISCO are performed at Bessy U49/2. We investigated BISCO single crystals with different hole doping concentrations at temperatures between 300 K and 17 K. CuO films have been used as a reference. We focus on the resPES data recorded at the Cu2p absorption edge. We find a strong polarization dependence for in-plane and out-of-plane geometries (with respect to the Cu-O plane) in our data which are caused by two independent Auger processes. We also report on the influence of different doping concentrations. Our resPES data enable us to sort the individual resonant mechanisms at the Cu2p
edge in more detail than recently anticipated (Brookes et al., 2015). We discuss our data in the context of the recent discussion about the applicability of the Zhang-Rice model (Chen et al., 2013).
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.
Aluminum nitride films prepared by plasma atomic layer deposition using different plasma sources
(2018)
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 Å/cycle.
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.
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.
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.
Atomic Layer-Deposited Aluminum Oxide Hinders Iodide Migration and Stabilizes Perovskite Solar Cells
(2020)
Iodide migration causes degradation of the perovskite solar cells. Here,we observe the direct migration of iodide into the hole-transport
layer in a device. We demonstrate that ultrathin room temperature
atomic layer-deposited Al2O3 on the perovskite surface very effectively hinders the migration. The perovskite-Al2O3 interface enables charge transfer across the Al2O3 layer in the solar cells, without causing any drastic changes in the properties of the perovskite absorber. Furthermore, it helps to preserve the initial properties of the perovskite film during exposure to light and air under real operating conditions, and thus, improves the stability of the solar cells. The ultrathin Al2O3 layer deposited at room temperature significantly increases the lifetime of the perovskite solar cells, and we hope this may be a step toward the mass production of stable devices.
For several years, scientists have been trying to understand the mechanisms that reduce the long‐term stability of perovskite solar cells. In this work, we examined the effect of water and photon flux on the stability of CH3NH3PbI3 perovskite films and solar cells using in situ near‐ambient pressure X‐ray photoelectron spectroscopy (NAP‐XPS), field emission scanning electron microscopy (FESEM), and current density–voltage (J–V) characterization. The used amount of water vapor (up to 1 mbar) had a negligible impact on the perovskite film. The higher the photon flux, the more prominent were the changes in the NAP‐XPS and FESEM data; also, a faster decline in power conversion efficiency (PCE) and a more substantial hysteresis in the J‐V characteristics were observed. Based on our results, it can be concluded that the PCE decrease originates from the creation of Frenkel pair defects in the perovskite film under illumination. The stronger the illumination, the higher the number of Frenkel defects, leading to a faster PCE decline and more substantial hysteresis in the J‐V sweeps.
The design and development of intrinsically stretchable all-organic self-powered sensors concurrently perceiving temperature and pressure remain a challenge but deliver an exciting platform to realize environmentally friendly wearable electronics. In this approach, a biomimetic all-organic stretchable energy harvester is designed by a xylitol-added poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS/Xyl) film as a compatible overlay electrode with polyaniline-reinforced one-dimensional aligned poly(vinylidene fluoride) hybrid electroactive soft nanowires. The gradient of elastic modulus between the electrode and the active nanowire component enables the all-organic device to manifest excellent power-generating performance under external temperature fluctuation (∼3 μW/m2 under ΔT ∼ 92 K) and mechanical force (∼31 μW/cm2 at 30 N). Importantly, the device renders simultaneous energy scavenging of temperature and pressure changes under pressing and stretching conditions (∼20%). The excellent mechanosensitivity (∼100 mV/N), fast response time (∼1 ms), outstanding mechanical and thermal stability, and good temperature resolution <10 K enable the harvester to act as an epidermal sensor, which simultaneously detects and discriminates both subtle pressure and thermal deviations exposed to an epidermis surface. The real-time recording and wireless transferring of physiological signals to a smartphone indicate an effective way to realize remote healthcare monitoring for early intervention.
The photosensitive and rectifying properties of Ga2O3 are described by (n-type) intrinsic (π-) electrons. These polaronic screened multiatomic carriers populate the intrinsic defect states within the ionic gap; their spectroscopic evidence is based on resonant photoemission spectroscopy data that also provide the ionicity factor of Ga2O3 and the size of the ionic gap. The π-electron density depends on the internal potential and its photo- and field-induced dipole contributions, and it describes the observed combined ohmic-exponential carrier densities and current–voltage dependences. The π-electron dynamics is caused by pairing and dissociation dipoles in the bulk of Ga2O3. The material properties of the electrode contribute via external chemical potentials and define the criteria for ohmic and rectifying contacts. This quantitative and predictive concept not only convinces by perfect agreement with published experimental data but also points toward the achievable performance limits of UV absorbers and rectifying devices.
The interface region of friction-welded joints Al-Fe samples is investigated by scanning Auger Spectroscopy, Electron Probe Micro-analysis (EPMA), X-ray Photoelectron spectroscopy, and Photoemission Electron Microscopy, performed at the synchrotron light source (BESSY). We investigated polished samples cut to obtain a cross-section of the Al-Fe joints. At the Al-Fe interface there is a small number of Fe teeth protuding into the adjacent Al-matrix. Beside this mechanical interlock mechanism we identify an Fe-Al alloy which is formed in an almost homogeneous interface layer of approximately 80 micron thickness. We determine the valence band spectra within that layer and notice that the alloying formation is limited to the interface region. In addition, the profile of both, the Fe and O distribution within the Al next to that interface is determined. A model of the friction-welding mechanism is derived and discussed in terms of the ability of achieving low temperature Fe-Al joints.
The direct synthesis of methanol [CO2+3H2->CH3OH+H2O]
represent a possibility to reduce the global CO2-emission by recycling the CO2 and also to store excess energy from renewable energy sources into a common fuel or chemical feedstock (Power-to-Liquid). For an acceptable conversion rate of CO2 a catalyst is needed, together with
high temperatures (>200°C) and high pressure (50-200bar). Methanol is normally produced form synthesis gas, a mixture of CO and H2. By directly using CO2 for the exothermic reaction, we avoid the conversion of CO2 to CO by the reversed water gas shift reaction. We also present
new concepts for the conversion from CO2-rich flue gases, eliminating the need for a separation of the CO2. The concept is backed up by
measurements in laboratory scale. Here we use a Cu−ZnO
catalyst on a ZrO2 substrate prepared by impregnation and compare the results with commercially available catalysts. We achieved a conversion of around 7% and a selectivity of 60% at a temperature of 240°C and
45bar. The reaction is thermodynamically limited with a maximum conversion rate of 15% at 250°C and 50bar. The conversion and the
selectivity towards methanol is highly influenced by the catalyst used, the temperature, the pressure as well as the flow rate of the reactants.
Localized defect states and charge trapping in Al₂O₃ films prepared by atomic layer deposition
(2017)
The evaluation of the electronic structure and intrinsic defect mechanisms in Al₂O₃ thin films is essential for their effective use in applications with desired functionality such as surface passivation schemes for solar cells [1]. We present a comparative study of different Al₂O₃ films grown by atomic layer deposition (ALD) [2]. The layers were deposited on different substrates using the same aluminum precursor (TMA, trimethylalumium) and employing different process parameters (thermal-ALD, plasma-enhanced-ALD, substrate temperature). These films were characterized by resonant photoelectron spectroscopy and by electrical measurements (capacitance-voltage). For all films investigated intrinsic defect states within the electronic band gap were observed including excitonic, polaronic, and charge-transfer defect states, where their relative abundance is subject of the choice of ALD parameters and of the used substrate. The spectroscopic assigned in-gap defect states are related with electronic charges as determined in the electrical measurements. [1] G. Dingemans and W.M.M. Kessels, J. Vac. Sci. Technol. A 30, 040802 (2012). [2] K. Henkel, M. Kot, D. Schmeißer, J. Vac. Sci. Technol. A 35, (2017), accepted.
The use of electrochemistry, X-ray photoelectron spectroscopy, and resonant X-ray spectroscopy has unlocked the paradox of interfacial hole conduction through amorphous TiO2 (a-TiO2) to deposited Ni, Ir, and Au metal catalysts. Although electrocatalysts for the oxygen-evolution reaction derived from metallic Ir and Ni have mutually similar overpotentials in alkaline media, Si/a-TiO2/Ir interfaces exhibit higher overpotentials than Si/a-TiO2/Ni interfaces. The data allow formulation of full band energy diagrams for n-Si/a-TiO2/metal interfaces for M = Ni, Ir, or Au. Although both Ni and Ir produce band bending in a-TiO2 favoring hole conduction, only Ni creates multiple states within the a-TiO2 band gap at the a-TiO2/Ni interface, which produces a quasi-metallic interface at the a-TiO2/Ni junction. Au, however, produces a flat-band interface that limits hole conduction without any new band gap states.