44 research outputs found
Photoionization of helium dimers
Die vorliegende Arbeit bietet zunächst einen weiteren Beweis für die Existenz des neutralen Heliumdimers. Darüber hinaus konnten zwei verschiedene Prozesse identifiziert werden, über die die Absorbtion eines Photons zur Ionisation beider Atome des Dimers über sehr große Abstände führen kann. Oberhalb einer Photonenenergie von 65,4 eV konnte ein ICD Prozess beobachtet werden, der über Photoionisation mit gleichzeitiger Anregung von einem der beiden Atome realisiert wird. Bei 77,86 eV konnte ICD über elektronisch angeregte Zustände bis n=6 nachgewiesen werden. In der KER-Verteilung konnten zudem Strukturen gefunden werden, die auf Vibrationsanregungen im Zwischenzustand des Dimer-Ions schließen lassen. Eine vollständig quantenmechanische Rechnung von Sisourat et al. konnte dies schließlich hervorragend bestätigen. Es konnte also ein direkter Blick auf die Vibrationswellenfunktionen des Systems erlangt werden. In anderen Systemen ist dies in der Regel nicht möglich, da sich alle Zustände üblicherweise zu einer strukturlosen Verteilung überlagern. Weiterhin konnte gezeigt werden, dass sich die Winkelverteilungen von ICD- und Photoelektronen in verschiedenen Bereichen des KER mitunter stark voneinander unterscheiden. Dies konnte auf die unterschiedliche Besetzung von verschiedenen Potentialkurven zurückgeführt werden. Unterhalb der Photonenenergieschwelle zur Anregung und Ionisation eines Heliumatoms konnte ein weiterer, zweistufiger Ionisationsmechanismus gefunden werden. Hier wird zunächst durch Photoionisation ein Elektron aus einem der beiden Atome im Dimer freigesetzt. Dieses Photoelektron kann nun am neutralen Atom gestreut werden und dabei ausreichend viel Energie übertragen, um dieses ebenfalls zu ionisieren. Es konnte gezeigt werden, dass der Prozess einer Abhängigkeit von der Polarisation der Synchrotronstrahlung unterliegt, die man für Photoionisation erwarten würde. Die Energie- und Winkelverteilungen der Elektronen konnten daher mit vorangegangenen Elektronenstoß-Experimenten verglichen werden. Die gute Übereinstimmung mit diesen Daten rechtfertigt eine anschauliche Sichtweise des Prozesses als Analogon zum klassischen Billiard-Stoß. Der Two-Step-Prozess wurde bisher zwar schon in vielen Systemen als theoretisches Modell zur Doppelionisation beschrieben, allerdings konnten die einzelnen Unterprozesse bisher nicht gesondert gemessen werden. Die großen Abstände im Heliumdimer ermöglichen erstmals eine deutliche Trennung in Photoionisation an einem Atom und Elektronenstoß (e,2e) am Nachbaratom. Der Two-Step-Prozess konnte außerdem dazu verwendet werden, die ungewöhnliche Grundzustandswellenfunktion des Heliumdimers zu experimentell zu bestätigen. Eine Analyse des gemessenen KER konnte dabei deutliche Abweichungen zu einer klassischen Theorie aufzeigen. Erst eine vollständig quantenmechanische Rechnung des Übergangs von Sisourat et al. konnte die Messdaten beschreiben.The helium dimer is one of the most weakly bound systems in the universe. This makes it an interesting quantum mechanical object for investigation. These Van der Waals Clusters can be produced in an expansion of a cryogenic gas jet through a small nozzle into vacuum. In the present experiment we examine the interaction of He dimers with synchrotron radiation at an energy range from 64 to 78 eV. We observed different pathways leading to single ionization of both He atoms of the dimer compound. This two close standing ions begin now to dissociate in cause of their coulomb potential. All charged fragments were detected in coincidence with a COLTRIMS system. Especially Interatomic Coulombic Decay (ICD) and the two step process (TS1) were clearly identified. Furthermore a distribution of the internuclear distance was obtained from the measured Kinetic Energy Release (KER)
Photoionisation und doppelt angeregte Zustände in Wasserstoff- und Deuterium-Molekülen
In dieser Arbeit wurden ionisierende Prozesse inWasserstoff- und Deuterium-Molekülen untersucht. Das Ziel war es dabei insbesondere, doppelt angeregte Zustände näher zu betrachten, d.h. Prozesse, bei denen mit einem UV-Photon beide Elektronen des H2 angeregt werden. Das Molekül zerfällt dann schließlich in ein angeregtes Atom sowie ein Proton und ein Elektron. Diese Doppelanregung konnte in den Messdaten identifiziert werden. Durch die Art der Messung war es möglich, einen umfassenden Überblick über den Photonenenergiebereich von 29 bis 60 eV zu erhalten (siehe Abb. 4.4). Somit konnte die Dynamik verschiedener Prozesse mit sich ändernder Photonenenergie analysiert werden. Es konnte die Einfach-Ionisation vom Einsetzen bis hin zur Doppel-Ionisation beobachtet werden. Zwischen 29 und 38 eV traten dabei Anregungen auf das Q1- und Q2-Band auf. Insbesondere für einen KER=2) auftreten. Um eventuelle Strukturen in diesem Bereich zu studieren ist ein jedoch ein höher auflösendes Spektrometer notwendig. Dies könnte z.B. durch größere MCP realisiert werden
Long-range Energy Transfer and Ionization in Extended Quantum Systems Driven by Ultrashort Spatially Shaped Laser Pulses
The processes of ionization and energy transfer in a quantum system composed
of two distant H atoms with an initial internuclear separation of 100 atomic
units (5.29 nm) have been studied by the numerical solution of the
time-dependent Schr\"odinger equation beyond the Born-Oppenheimer
approximation. Thereby it has been assumed that only one of the two H atoms was
excited by temporally and spatially shaped laser pulses at various laser
carrier frequencies. The quantum dynamics of the extended H-H system, which was
taken to be initially either in an unentangled or an entangled ground state,
has been explored within a linear three-dimensional model, including two z
coordinates of the electrons and the internuclear distance R. An efficient
energy transfer from the laser-excited H atom (atom A) to the other H atom
(atom B) and the ionization of the latter have been found. It has been shown
that the physical mechanisms of the energy transfer as well as of the
ionization of atom B are the Coulomb attraction of the laser driven electron of
atom A by the proton of atom B and a short-range Coulomb repulsion of the two
electrons when their wave functions strongly overlap in the domain of atom B.Comment: 11 pages, 7 figure
Interatomic Coulombic Decay following Photoionization of the Helium Dimer: Observation of Vibrational Structure
Using synchrotron radiation we simultaneously ionize and excite one helium
atom of a helium dimer (He_2) in a shakeup process. The populated states of the
dimer ion (i.e. He^[*+](n = 2; 3)-He) are found to deexcite via interatomic
coulombic decay. This leads to the emission of a second electron from the
neutral site and a subsequent coulomb explosion. In this letter we present a
measurement of the momenta of fragments that are created during this reaction.
The electron energy distribution and the kinetic energy release of the two He^+
ions show pronounced oscillations which we attribute to the structure of the
vibrational wave function of the dimer ion.Comment: 8 pages, 5 figure
Single photon double ionization of the helium dimer
We show that a single photon can ionize the two helium atoms of the helium
dimer in a distance up to 10 {\deg}A. The energy sharing among the electrons,
the angular distributions of the ions and electrons as well as comparison with
electron impact data for helium atoms suggest a knock-off type double
ionization process. The Coulomb explosion imaging of He_2 provides a direct
view of the nuclear wave function of this by far most extended and most diffuse
of all naturally existing molecules.Comment: 10 pages, 5 figure
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Single photon induced symmetry breaking of H2 dissociation
H{sub 2}, the smallest and most abundant molecule in the universe, has a perfectly symmetric ground state. What does it take to break this symmetry? Here we show that the inversion symmetry can be broken by absorption of a linearly polarized photon, which itself has inversion symmetry. In particular, the emission of a photoelectron with subsequent dissociation of the remaining H{sub 2}{sup +} fragment shows no symmetry with respect to the ionic H+ and neutral H atomic fragments. This result is the consequence of the entanglement between symmetric and antisymmetric H{sub 2}{sup +} states resulting from autoionization. The mechanisms behind this symmetry breaking are general for all molecules
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Fragmentation pathwaysfor selected electronic states of theacetylene dication
Coincident measurement of the Auger electron and fragmention momenta emitted after carbon core-level photoionization of acetylenehas yielded new understanding of how the dication fragments. Ab initiocalculations and experimental data, including body-frame Auger angulardistributions, are used to identify the parent electronic states andtogether yield a comprehensive map of the dissociation pathways whichinclude surface crossings and barriers to direct dissociation. The Augerangular distributions show evidence of core-holelocalization
A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment
In this work we present a comprehensive and detailed study of Interatomic Coulombic Decay (ICD) occurring after irradiating argon dimers with XUV-synchrotron radiation. A manifold of different decay channels is observed and the corresponding initial and final states are assigned. Additionally, the effect of nuclear dynamics on the ICD electron spectrum is examined for one specific decay channel. The internuclear distance-dependent width Γ(R) of the decay is obtained from the measured kinetic energy release distribution of the ions employing a classical nuclear dynamics model
The multiple tasks of noun insertion: Definiteness and Gender Allocation in German-Swedish Codeswitching
Deutsch-schwedisches Codeswitching an der internationalen Universität
The study contributes to the growing field of multilingualism in university contexts. The subject is the bilingual language use of scholars working at German institutes at universities in Sweden. The study illuminates both the formal and the functional aspects of their codeswitching. It thereby goes towards filling gaps in research on codeswitching in academic communication. The analysis of the grammatical integration of switched items uses a contrastive method giving special attention to aspects where the language systems (German and Swedish) come into conflict. The findings are interpreted in relation to the sociological approach of communities of practice, which reveals that, in building such a community, the informants follow specific practices in their codeswitching.
A corpus of more than 30 hours of conversation has been compiled, comprising different com-munication situations at the workplaces.
It is exposed that the existing descriptive models do not contribute categories suitable to describing the form of codeswitching in the corpus, since they do not consider the syntactical characteristics of spoken language. Therefore, a new descriptive model is suggested. The main categorization criteria are conversational turns and morphosyntactical dependencies.
Further, categories of analysis of motivation for codeswitching were found to be a desideratum. To create a description model, the function of and motives for codeswitching mentioned in pre-vious literature were compiled and assigned to subordinated factors.
The analysis shows that the informants prefer a distinct base language, in which items from the respective other language can be inserted, mostly nouns and particles. The insertion of verbs is avoided. The investigated speakers follow strict patterns concerning the morphological and syntactical integration of inserted items. These patterns differ from those reported from other bilingual communities and predicted in theoretical models such as the MLF model: Even though the word order in bilingual utterances follows the base language, inserted words are inflected according to the embedded language, so neither Swedish nor German constitutes a classical matrix language. One grammatical item that comes into conflict as a result of this pattern is the definite article, which is an inflectional suffix in Swedish, but is a free grammatical word in German. Which system is used to mark an embedded language noun as definite, depends mainly on the motivation for the codeswitching.
Metalinguistic comments are a common motivation for codemixing in the corpus. The frequent insertion of nouns is, however, mainly motivated by linguistic domains. This is also remarkable in comparison with other bilingual communities, since linguistic domains are mostly predicted to cause a change of the base language rather than the insertion of single words