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Das Fachgebiet der Kognitiven Technischen Systeme zeichnet sich durch einen hohen Grad an Interdisziplinarität (z. B. Kenntnisse auf den Gebieten Biologie, Psychologie, Informatik und den Ingenieurwissenschaften) aus. Nach wie vor besteht Bedarf an einer methodischen Darstellung des Fachgebietes, bei der die theoretische Durchdringung von Zusammenhängen zwischen den verschiedenen Wissensgebieten zusätzlich durch Anschaulichkeit unterstützt wird. Die vorliegende Arbeit stellt einen Fortschrittsbericht zur Realisierung eines Forschungs- und Experimentiersystems dar, mit dem wir dieses Anliegen unterstützen und über das wir erstmals konzeptionell in [1] berichtet haben. In diesem Beitrag folgen wir einem integrativen Ansatz zur Entwicklung einer kognitiven Architektur, mit der unter Verwendung repräsentationaler Datenstrukturen adaptives Verhalten auf verschiedenen Zeitskalen sowie zwei wichtige Verhaltensprogramme für das Problemlösen (Objektfindung, Exploration) auf der gemeinsamen Grundlage von Markov-Entscheidungsprozessen umgesetzt werden. Mit einem Kurzbericht zum Entwicklungsstand der physikalischen Experimentierumgebung und einer Zusammenfassung der bislang erreichten Ergebnisse beschließen wir den diesjährigen Beitrag.
Resonant Auger decay processes have been studied by resonant photoemission spectroscopy (resPES) and X-ray absorption spectroscopy (XAS) in Graphene systems. The pi*-resonance is used to identify the degree of localization of the lowest pi*-orbitals in the conduction band. Localization and lifetime of the photo-excited intermediate state cause the formation of multiple Auger processes. For the Graphene systems we identify two novel Auger decay combinations with a four hole final state: the (S+S) and the(S+S)* decay. We demonstrate that these processes are sensitive for interlayer coupling and interactions with the metallic free electrons of the substrate.
Resonant photoemission spectroscopy(resPES) is used to probe the occupied pi- and unoccupied pi*-bands of
carbon thin films with particular focus on the Auger decay. Highly Oriented Pyrolytic Graphite (HOPG) is
studied at the C1s edge. We find strong resonant features at 285.5 eV and 292 eV in the resPES diagram. The normal two-hole Auger decay proceeds under constant kinetic energy (451)only in the sigma*-region. In the pi*-region, however, it proceeds under 67.5° in terms of a Ebind(w) diagram. We attribute this to a multiple Auger decay with a net three hole final state. For this novel decay process we propose a model.We discuss
the long lifetime of the first resonant excitation and conclude that it arises from the strong excitonic character
of the first resonant state. We use HOPG as a reference system and suggest that this novel process is a tool to
identify interlayer–substrate interaction of the carbon layers involved.
The coating of materials with diamond-like carbon (DLC) is a very common way to change and improve their basic characteristics. Although DLC is used on several substrates, the chemical and physical properties throughout the coating process on plastics are yet sparsely investigated. Two types of protective
coatings one sp3-enriched (robust, r-type) and one with more sp2-centers (flexible, f-type) have been realized on polyethylene by PECVD deposition. SEM and AFM analysis of coated samples of DLC types revealed diverse surface topographies on different scales and images appeared even differently smoothed by the carbonaceous deposits. Grains of both DLC types are platelet-shaped and nearly double in size for the robust type indicating fundamental differences in the epitaxial DLC growth. NEXAFS spectroscopy showed significant details of carbon centers in chemically different neighborhood displaying a characteristic fingerprint behavior. Comparison of deposition models revealed a mechanism of interlayer formation which is discussed in detail. Interlayer formation is clearly the appropriate explanation of the process for the current carbon deposition between these two unequal materials. An improved understanding of hard DLC and soft polyethylene assembly is given in the presented work.
We use resonant photoemission at the C1s edge to study the
electronic structure of HOPG, graphene flakes and monolayer
graphene. We find remarkable differences in the profile of the Auger decay channels, which we attribute to an additional multiple-Auger with a three-hole final state. A prerequisite for the
appearance of this decay mechanism is the existence of localized excitonic states, which cause the appearance of the multiple Auger decay. We use those effects to identify the existence and the quantity of such defect states within the π*-band regime in carbon thin films, because the intensity of the three-hole Auger decay is varying with the defect density of the carbon films. We find that the appearance of the multiple Auger decay is different for multilayer and monolayer graphene. In particular the interaction of
impurities leads to broadening of the C1s core levels. The three-hole Auger decay spectroscopy is a new method to detect such
contaminations with a high sensitivity.
The electronic structure of Cobalt based catalysts used for photocatalytic water splitting in solar cells is analyzed using synchrotron radiation photoelectron spectroscopy. The catalyst
films are prepared by electrochemical deposition. We employ a X-ray photoelectron spectroscopy study to analyze the Co2p and O1s core levels,absorption edges and valence bands. We discuss our resonant data in terms of the partial density of states of the valence
and conduction band. We find a difference in the Co oxidation state as a function of film thickness (deposited charge). From the relative amount of Co, O, K and P we favor the molecular cobaltate cluster-like structure as the structural motif of the Co-PI
catalyst.
Cobalt based oxygen evolution catalysts (Co-PI, PI=electrodeposited from pH 7 phosphate) are studied by resonant photoemission spectroscopy at the Co L3 and O1s edge. For the individual Co3d states, we determine their configuration, their spin, and their energy level relative to the Fermi
energy. We identify the Co divalent high spin state and the trivalent low spin state. In addition, we also find the corresponding oxygen-to-metal charge transfer states. We attribute the trivalent charge
transfer state to be the active state for the oxygen evolution reaction.
The electronic structure of cobalt based catalysts used for photocatalytic water splitting in solar cells is analyzed using synchrotron radiation photoelectron spectroscopy. The catalyst films are prepared by electrochemical deposition. We employ a X-ray photoelectron spectroscopy study to analyze the Co2p and O1s core levels, absorption edges and valence bands. We discuss our resonant data in terms of the partial density of states of the valence and conduction band. We find a difference in the Co oxidation state as a function of film thickness (deposited charge). From the relative amount of Co, O, K and P we favor the molecular cobaltate cluster-like structure as the structural motif of the Co-PI catalyst. Further, at resonant PES at the Co2p edge we find the Co2p partial DOS to exhibit no sharp features next to the VBM, instead there is a broad emission at around 6eV below EFerrmi. The former are found in LiCoO2 and other Co-oxide systems with a Co3+ ground state. We attribute such sharp features to the low spin (LS) configuration of Co3+ and deduce that in the Co catalysts there is no evidence for the corresponding LS contributions. Our data prove the Co2+ ground state and demonstrate that it is exclusively in the Co3d7 high spin state in the pristine catalyst films.