## Doctoral Thesis

In this thesis, it was the subject to build a setup to study the interaction of clusters with intense laser light. A magnetron sputter cluster ion source was built to create metal clusters for the planned investigations. Furthermore, a linear Paul trap setup was built in order to allow the investigation of the mentioned interaction at one specific cluster size. The whole apparatus was characterized and first experiments were performed.

The thesis deals with ions stored in an electrostatic ion beam trap. In the first part of the thesis the so-called self-synchronization effect is discussed. It is demonstrated that the time a bunch of injected ions is conserved by the self-synchronization effect depends on the number of injected ions. In the second part of the thesis the cooling of small anionic cobalt and copper clusters is addressed. Measurements on anionic copper clusters consisting of four to seven atoms are presented and the decay of hot clusters is observed in order to draw conclusions on the internal temperature and the cooling process itself. Afterwards measurements on Co4- are discussed and a measurement scheme based on laser induced delayed electron emission is presented enabling to monitor the internal energy distribution of the clusters over storage time in a temperature-controlled environment. The cooling of initially hot clusters as well as the heating of initially cold clusters were observed.

The laser-matter interaction is a topic of current research. In this context, the interaction of intensive laser radiation with atomic clusters is of special interest. Du to the small cluster size, the laser field can penetrate the whole cluster volume, which leads to a high absorption of energy in the cluster. As a result, plasmas with high density and high temperature are produced. In the early phase of the laser-cluster interaction, free electrons are initially created in the cluster due to tunnel ionization or photoionization. Via collisions of these electrons with the cluster atoms, the ionization is increased and thus a dense nanoplasma is produced, which is heated by the laser. If free electrons leave the cluster during the laser-cluster interaction (outer ionization), a positive charge buildup is created. The associated charge repulsion finally can lead to the fragmentation of the cluster due to Coulomb explosion. Experimentally, interesting phenomena emerging from laser-excited clusters are observed, e.g., the creation of fast electrons, the production of highly charged ions, and X-ray emission. In this dissertation, the interaction of Gaussian laser pulses in the infrared regime with argon and xenon clusters is simulated by means of a nanoplasma model. Considering laser intensities in the non-relativistic regime, the relevant processes such as ionization, heating and expansion are theoretically described in this model with a set of coupled rate equations and hydrodynamic equations. One focus of the thesis is on the heating of the nanoplasma via inverse bremsstrahlung (IB), which is due to the absorption of laser photons in electron-ion collisions. In particular, the important question is investigated whether the consideration of the ionic structure â€“ that means, the nuclear charge and the bound electrons â€“ modifies the electron-ion collisions and thus the IB heating rate. Starting from a quantum statistical description, effective electron-ion potentials are used which account for both the screening due to the dense plasma and the inner ionic structure. Within the quantum mechanical first Born approximation, the consideration of the ionic structure leads to a drastic increase of the IB heating rate, in particular for high nuclear charges and low ionic charge states. However, for the parameters relevant in experiments, the applicability of the first Born approximation is questionable. Therefore, quantum mechanical calculations going beyond the first-order perturbation theory are performed. In addition, the IB heating rate is investigated with different classical methods. These are based either on transport cross sections for elastic electron-ion scattering or on classical simulations of inelastic scattering processes. Also within the classical approaches, the consideration of the ionic structure leads to an increase of the heating rate. However, this increase is shown to be only moderate. In a further part, the thesis focuses on the question how the dynamics of the laser-cluster interaction is influenced by the consideration of excited states. This is explored exemplarily for argon clusters excited by single or double laser pulses. The consideration of excitation processes in the nanoplasma leads to a decrease of the electron temperature and to an increase of the density of free electrons. Moreover, it is shown that the consideration of excitation processes results in an essential acceleration of the ionization dynamics. As a consequence, the mean ionic charge state in the plasma as well as the number of highly charged ions is significantly increased. For the population of ground states and excited states within an ionic charge state Z, collisional deexcitation processes play an important role. By means of an analytical relation between excitation and deexcitation cross sections, the rates for the respective processes in the presence of the laser field are calculated. The role of deexcitation processes is studied in detail, showing that the inclusion of these processes is essential for the correct theoretical description of the photon emission from laser-excited clusters. Based on these results, the photon yield is calculated for selected radiative transitions resulting from highly charged argon ions in the UV and X-ray regime.

During the past decade, various physical properties of the Yukawa ball, like structure and energy states, were unraveled using experiments. However, the dynamical features served further attention. Therefore, the main aim of my thesis was to investigate and understand how a finite system-represented by Yukawa clusters-evolves from a solid, crystalline structure to a liquid-like system, how it behaves in this phase and in what manner the reordering back into the solid state can be described. As a method of choice to reach this goal, laser heating has been proven successful. Moreover, the special importance of wakefields for dust clusters confined at low neutral gas pressure was addressed. Melting of finite dust clouds can be induced in two ways, either by altering the properties of the ambient plasma or by laser heating. The latter was shown to be a generic melting scenario, allowing to estimate a critical coupling parameter at the melting point. Moreover, the melting transition of finite 3D dust systems was found to be a two-step process where angular order is lost before the radial order starts to diminish at higher energies. Next, the mode dynamics of finite 3D dust ensembles in the solid and the liquid phase was studied. Crystal and fluid modes revealed the main spectral properties of the system. The normal modes are mainly suited to describe crystalline states. Fluid modes were excited naturally and via laser heating, with excitation frequencies almost independent of the coupling parameter in the solid and the liquid-like regime. Tuning the plasma parameters can be used to vary the particle-particle interaction via the ion focus. Both methods, even though assuming equilibrium situations, allowed to hint at these wakefields. The corresponding peaks in the fluid and normal mode spectra were no eigenmodes, confirming the nonequilibrium character of the ion focusing effect. First steps to extend the normal mode theory to achieve the dynamics of wake-affected nonequilibrium dust clusters were presented. Statistical quantities were obtained evaluating long-run experiments and transport coeffcients for finite dust systems were calculated via the instantaneous normal mode technique. Diffusion was found considerably higher for 3D than for 2D dust clusters. Using the configurational entropy, we have shown that in 2D and 3D disorder increases with increasing size of the system, in agreement with simulations. The temperature dependence of the configurational entropy differs for 2D and 3D dust clouds, with a threshold behavior found for finite 2D ensembles only. Finally, using instantaneous normal modes to reveal the total fraction of unstable modes, the predictive connection of Keyes (Phys Rev E 62, p7905, 2000), between transport and disorder was tested and verified for 2D, but not for 3D clusters. The reason for this has to be left open. Finally, laser-mediated recrystallization processes of finite 3D dust clouds were investigated. First, the temporal evolution of the Coulomb coupling parameter was traced during heating and recrystallization. A cooling rate has been determined from the initial phase of recrystallization. This cooling rate is lower than damping by the neutral gas, in agreement with simulations. We have observed a large fraction of metastable states for the final cluster configurations. Further, we have revealed that the time scale for the correlation buildup in the finite 3D ensemble was on even slower scales than cooling. Thus, different time scales can be attributed to the fast emergence of the shells and to the slower individual ordering within the shells.

Multiply negatively charged aluminium clusters and fullerenes were generated in a Penning trap using the "electron-bath" technique. Aluminium monoanions were generated using a laser vaporisation source. After this, two-, three- and four-times negatively charged aluminium clusters were generated for the first time. This research marks the first observation of tetra-anionic metal clusters in the gas phase. Additionally, doubly-negatively charged fullerenes were generated. The smallest fullerene dianion observed contained 70 atoms.