J. Tiggesbäumker

Laser-driven nonlinear cluster dynamics

Laser excitation of nanometer-sized atomic and molecular clusters offers various opportunities to explore and control ultrafast many-particle dynamics. Whereas weak laser fields allow the analysis of photoionization, excited-state relaxation, and structural modifications on these finite quantum systems, large-amplitude collective electron motion and Coulomb explosion can be induced with intense laser pulses. This review provides an overview of key phenomena arising from laser-cluster interactions with focus on nonlinear optical excitations and discusses the underlying processes according to the current understanding. A general survey covers basic cluster properties and excitation mechanisms relevant for laser-driven cluster dynamics. Then, after an excursion in theoretical and experimental methods, results for single-photon and multiphoton excitations are reviewed with emphasis on signatures from time- and angular-resolved photoemission. A key issue of this review is the broad spectrum of phenomena arising from clusters exposed to strong fields, where the interaction with the laser pulse creates short-lived and dense nanoplasmas. The implications for technical developments such as the controlled generation of ion, electron, and radiation pulses will be addressed along with corresponding examples. Finally, future prospects of laser-cluster research as well as experimental and theoretical challenges are discussed.

Spectroscopy on rare gas–doped silver clusters in helium droplets

The optical spectrum of Ag8 in a helium droplet, first measured by Federmann et al. [Eur. Phys. J. D 9, 11 (1999)], is studied over a broad wavelength range (237–450 nm) by resonant two photon ionization. A strong resonance is found in accordance to recent ab initio calculations. Doping the droplet additionally with rare gas atoms leads to a shift of the mean resonance position, which depends on the type and the number of attached atoms. In contrast to the red-shift obtained for argon, krypton, and xenon, for neon a net shift of the resonance to shorter wavelengths is observed. The dosage-dependence of the displacements will qualitatively be explained.

Ion induced snowballs as a diagnostic tool to investigate the caging of metal clusters in large helium droplets

Metal clusters embedded in ultracold helium nanodroplets are exposed to femtosecond laser pulses with intensities of 10(13)-10(14) W/cm2. The influence of the matrix on the ionization and fragmentation dynamics is studied by pump-probe time-of-flight mass spectrometry. Special attention is paid to the generation of helium snowballs around positive metal ions (Me(z+)He(N), z=1,2). Closings of the first and second helium shells are found for silver at N(1)=10,12 and N(2)=32,44, as well as for magnesium at N1=19-20. The distinct abundance enhancement of helium snowballs in the presence of isolated atoms and small clusters in the droplets is used as a diagnostics to explore the cage effect. For silver, a reaggregation of the clusters is observed at 30 ps after femtosecond laser excitation.

Thomson scattering from near-solid density plasmas using soft x-ray free electron lasers

We propose a collective Thomson scattering experiment at the VUV free electron laser facility at DESY (FLASH) which aims to diagnose warm dense matter at near-solid density. The plasma region of interest marks the transition from an ideal plasma to a correlated and degenerate many-particle system and is of current interest, e.g. in ICF experiments or laboratory astrophysics. Plasma diagnostic of such plasmas is a longstanding issue. The collective electron plasma mode (plasmon) is revealed in a pump-probe scattering experiment using the high-brilliant radiation to probe the plasma. The distinctive scattering features allow to infer basic plasma properties. For plasmas in thermal equilibrium the electron density and temperature is determined from scattering off the plasmon mode.

Steplike intensity threshold behavior of extreme ionization in laser-driven xenon clusters.

The generation of highly charged Xe(q+) ions up to q=24 is observed in Xe clusters embedded in helium nanodroplets and exposed to intense femtosecond laser pulses (λ=800  nm). Laser intensity resolved measurements show that the high-q ion generation starts at an unexpectedly low threshold intensity of about 10(14)  W/cm2. Above threshold, the Xe ion charge spectrum saturates quickly and changes only weakly for higher laser intensities. Good agreement between these observations and a molecular dynamics analysis allows us to identify the mechanisms responsible for the highly charged ion production and the surprising intensity threshold behavior of the ionization process.

Pb 4f photoelectron spectroscopy on mass-selected anionic lead clusters at FLASH

4f core level photoelectron spectroscopy has been performed on negatively charged lead clusters, in the size range of 10?90 atoms. We deploy 4.7?nm radiation from the free-electron laser FLASH, yielding sufficiently high photon flux to investigate mass-selected systems in a beam. A new photoelectron detection system based on a hemispherical spectrometer and a time-resolving delayline detector makes it possible to assign electron signals to each micro-pulse of FLASH. The resulting 4f binding energies show good agreement with the metallic sphere model, giving evidence for a fast screening of the 4f core holes. By comparing the present work with previous 5d and valence region data, the paper presents a comprehensive overview of the energetics of lead clusters, from atoms to bulk. Special care is taken to discuss the differences of the valence- and core-level anion cluster photoionizations. Whereas in the valence case the escaping photoelectron interacts with a neutral system near its ground state, core-level ionization leads to transiently highly excited neutral clusters. Thus, the photoelectron signal might carry information on the relaxation dynamics.

Spectroscopy of silver dimers in triplet states

Silver dimers embedded in ultracold helium nanodroplets are ionized by two-photon excitation via a strong resonance which extends from 3.85 eV up to 4.1 eV. The corresponding photoelectron spectra reveal that the ionization threshold is shifted by more than 1.4 eV towards lower values when compared to the gas phase. This gives strong evidence that weakly bound dimers in the lowest lying triplet state are present, thus enabling convenient spectroscopy of the triplet Ag2. A comparison with predictions from theory allows an assignment of the structure in the spectra. The successful identification of triplet silver dimers embedded in helium droplets shows exemplarily that the formation of such weakly bound systems is not restricted to surface locations as with the alkalis, but represents a general feature of the ultracold helium droplet environment.

Time-resolved studies on the collapse of magnesium atom foam in helium nanodroplets

Magnesium atoms embedded in superfluid helium nanodroplets have been identified to arrange themselves in a metastable network, referred to as foam. In order to investigate the ionization dynamics of this unique structure with respect to a possible light-induced collapse, the femtosecond dual-pulse spectroscopy technique is applied. Around zero optical delay a strong feature is obtained which represents a direct probe of the foam response. We found that upon collapse, ionization is reduced. A particular intensity ratio of the pulses allows us to address either direct ionization or photoactivation of the neutral complexes, thus affecting reaction pathways. A simplified scheme visualizes possible excitation scenarios in accordance with the experimental observations.

Nanoplasmonic electron acceleration in silver clusters studied by angular-resolved electron spectroscopy

The nanoplasmonic field enhancement effects in the energetic electron emission from few-nm-sized silver clusters exposed to intense femtosecond dual pulses are investigated by high-resolution double differential electron spectroscopy. For moderate laser intensities of 1014?W?cm?2, the delay-dependent and angular-resolved electron spectra show laser-aligned emission of electrons up to keV kinetic energies, exceeding the ponderomotive potential by two orders of magnitude. The importance of the nanoplasmonic field enhancement due to resonant Mie-plasmon excitation observed for optimal pulse delays is investigated by a direct comparison with molecular dynamics results. The excellent agreement of the key signatures in the delay-dependent and angular-resolved spectra with simulation results allows for a quantitative analysis of the laser and plasmonic contributions to the acceleration process. The extracted field enhancement at resonance verifies the dominance of surface-plasmon-assisted re-scattering.

Collimation of metal nanoparticle beams using aerodynamic lenses

With the objective of reducing the divergence, aerodynamic lenses were applied to collimate a beam of metal nanoparticles in a size range up to 20nm. Influences of the aerodynamic devices on the particle aggregation process and the beam properties have been evaluated by time-of-flight measurements on mass filtered clusters. Additional transmission electron microscopy and atomic force microscopy studies on deposited particles complement these investigations. Perspectives for the application of aerodynamic lenses in the collimation of ultrafine particles are discussed.