Helium nanodroplets are widely used as a cold, weakly interacting matrix for spectroscopy of embedded species. In this work, we excite or ionize doped He droplets using synchrotron radiation and study the effect onto the dopant atoms depending on their location inside the droplets (rare gases) or outside at the droplet surface (alkali metals). Using photoelectron-photoion coincidence imaging spectroscopy at variable photon energies (20-25 eV), we compare the rates of charge-transfer to Penning ionization of the dopants in the two cases. The surprising finding is that alkali metals, in contrast to the rare gases, are efficiently Penning ionized upon excitation of the (n = 2)-bands of the host droplets. This indicates rapid migration of the excitation to the droplet surface, followed by relaxation, and eventually energy transfer to the alkali dopants.

Cold inelastic collisions between confined cesium (Cs) atoms and Cs2 molecules are investigated inside a CO2 laser dipole trap. Inelastic atom-molecule collisions can be observed and measured with a rate coefficient of ∼ 2.5 × 10 −11 cm 3 s −1 , mainly independent of the molecular ro-vibrational state populated. Lifetimes of purely atomic and molecular samples are essentially limited by rest gas collisions. The pure molecular trap lifetime ranges 0,3-1 s, four times smaller than the atomic one, as is also observed in a pure magnetic trap. We give an estimation of the inelastic molecule-molecule collision rate to be ∼ 10 −11 cm 3 s −1 .

We simultaneously trap ultracold lithium and cesium atoms in an optical dipole trap formed by the focus of a CO2 laser and study the exchange of thermal energy between the gases. The optically cooled cesium gas efficiently decreases the temperature of the lithium gas through sympathetic cooling. Equilibrium temperatures down to 25 microK have been reached. The measured cross section for thermalizing 133Cs-7Li collisions is 8 x 10(-12) cm(2), for both species unpolarized in their lowest hyperfine ground state. Besides thermalization, we observe evaporation of lithium purely through elastic cesium-lithium collisions (sympathetic evaporation).

Highly excited states of rubidium (Rb) atoms attached to helium (He) nanodroplets are studied by two-photon ionization spectroscopy in combination with electron and ion imaging. We find high yields of RbHe and RbHe(2) exciplexes when exciting to the 4D and 6P bands but not at the 6S band, in accord with a direct formation of exciplexes in binding RbHe pair potentials. Photoion spectra and angular distributions are in good agreement with a pseudodiatomic model for the RbHe(N) complex. Repulsive interactions in the excited states entail fast dissociation followed by ionization of free Rb atoms as well as of RbHe and RbHe(2) exciplexes.

Helium nanodroplets, commonly regarded as the "nearly ideal spectroscopic matrix", are being actively studied for more than two decades now. While they mostly serve as cold, weakly perturbing and transparent medium for high-resolution spectroscopy of embedded molecules, their intrinsic quantum properties such as microscopic superfluidity still are subject-matter of current research. This article reviews recent work on pure and doped He nanodroplets using PI spectroscopy, an approach which has greatly advanced in the past years. While the notion of the ideal spectroscopic matrix mostly no longer holds in this context, photoionization techniques provide detailed insights into the photo-physical properties of pure and doped He nanodroplets and their relaxation dynamics following electronic excitation. Exploiting nowadays available high laser fields, even highly ionized states of matter on the nanoscale can be formed. Our particular focus lies on recent experimental progress including fs time-resolved spectroscopy, photoion and electron imaging, and novel sources of highly energetic radiation.

We present the first simultaneous trapping of two different ultracold atomic species in a conservative trap. Lithium and cesium atoms are stored in an optical dipole trap formed by the focus of a CO 2 laser. Techniques for loading both species of atoms are discussed and observations of elastic and inelastic collisions between the two species are presented. A model for sympathetic cooling of two species with strongly different mass in the presence of slow evaporation is developed. From the observed Cs-induced evaporation of Li atoms we estimate a cross section for cold elastic Li-Cs collisions.

The dynamics of vibrational wave packets excited in K2 dimers attached to superfluid helium nanodroplets is investigated by means of femtosecond pump–probe spectroscopy. The employed resonant three-photon-ionization scheme is studied in a wide wavelength range and different pathways leading to K2+ formation are identified. While the wave packet dynamics of the electronic ground state is not influenced by the helium environment, perturbations of the electronically excited states are observed. The latter reveal a strong time dependence on the timescale 3–8 ps which directly reflects the dynamics of desorption of K2 off the helium droplets.

The recent development of novel extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter 1,2 . Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution 3,4 . However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within a XUV pulse sequence opens exciting new possibilities for coherent control and multidimensional spectroscopy 4 , but has