ABSTRACT
The intensity-difference spectrum technique is applied to record charge-state resolved ion energy spectra from the Coulomb explosion of small Ar clusters under well-resolved laser intensity conditions. The far-reaching control of the experimental parameters permits us to identify a striking change in the expansion pattern of the nanoplasma beyond a given intensity. The simultaneous characterization of ion charge state and energy uncovers that a reduction of the laser intensity leads to a development of low energy cuts in the ion yields, not present at higher fluence. The complex interplay of outer ionization, recombination, ion screening, and the phenomenon of ionization saturation favors a surface-driven expansion at low plasma electron temperatures. With increasing laser intensity a transition into a volume-driven Coulomb explosion is observed.
ABSTRACT
The optical response of size-selected metal clusters is studied by wavelength-dependent photoemission and energy-resolved photoelectron detection. Relative photodetachment cross sections giving information on the plasmon are determined for the example of closed-shell Ag91-. Notably, the peak energy of this anion (3.74 eV) is higher than the small particle limit in Mie theory of 3.5 eV. Different methods to extract cross sections from the spectra are applied. In particular, we compare the results obtained by integrating the full electron yields to analyses based on evaluating specified binding energy windows. The approach opens up new possibilities to conduct studies on Landau fragmentation as a result of multielectron excitations.
ABSTRACT
Using the example of metal clusters, an experimental setup and procedure is presented, which allows for the generation of size and charge-state selected polyanions from monoanions in a molecular beam. As a characteristic feature of this modular setup, the further charging process via sequential electron attachment within a three-state digital trap takes place after mass-selection. In contrast to other approaches, the rf-based concept permits access to heavy particles. The procedure is highly flexible with respect to the preparation process and potentially suitable for a wide variety of anionic species. By adjusting the storage conditions, i.e., the radio frequency, to the change in the mass-to-charge ratio, we succeeded in producing clusters in highly negative charge states, i.e., Ag800 7-. The capabilities of the setup are demonstrated by experiments extracting electronic and optical properties of polyanionic metal clusters by analyzing the corresponding photoelectron spectra.
ABSTRACT
The electronic properties of silver clusters (N up to 800) charged by attachment of up to z = 7 excess electrons are investigated. As an essential preparation step, the technique of in-trap electron attachment to size-selected monoanions within a linear Paul trap is applied. By taking advantage of tunable laser pulses, the photoelectron spectra allow us to evaluate details of the electronic structure of polyanionic metal clusters, giving a multidimensional dataset. The subsequent analysis based on the liquid drop model provides information about the atomic structure and the bulk work function at a hitherto unknown quality.
ABSTRACT
Combining photoelectron spectroscopy with tunable laser pulse excitation allows us to characterize the Coulomb barrier potential of multiply negatively charged silver clusters. The spectra of mass- and charge-selected polyanionic systems, with z=2-5 excess electrons, show a characteristic dependence on the excitation energy, which emphasizes the role of electron tunneling through the barrier. By evaluating experimental data from an 800-atom system, the electron yield is parametrized with respect to tunneling near the photoemission threshold. This analysis results in the first experimentally based potential energy functions of polyanionic metal clusters.