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. 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. Nonresonant excitation generates Rb atoms in low-lying electronic levels by statistical evaporation-like desorption.
We present an experimental study of the dynamics following the photo-excitation and subsequent photo-ionization of single Cs atoms on the surface of helium nanodroplets. The dynamics of excited-Cs-atom desorption and re-adsorption as well as CsHe exciplex formation are measured using femtosecond pump-probe velocity-map-imaging spectroscopy and ion-time-of-flight spectrometry. The timescales for the desorption of excited Cs atoms off helium nanodroplets as well as the timescales for CsHe exciplex formation are experimentally determined for the 6p states of Cs. For the 6p $^2Π_ {1/2}$ state, our…
Besides the use as cold matrix for spectroscopic studies, superfluid helium droplets have served as a cold environment for the synthesis of molecules and clusters. Since vibrational frequencies of molecules in helium droplets exhibit almost no shift compared to the free molecule values, one could assume the solvated particles move frictionless and undergo a reaction as soon as their paths cross. There have been a few unexplained observations that seemed to indicate cases of two species on one droplet not forming bonds but remaining isolated. In this work, we performed a systematic study of hel…
Rubidium dimers residing on the surface of He nanodroplets are doubly ionized by an intense fs laser pulse leading to fragmentation into a pair of $\mathrm{Rb^+}$ ions. We show that the kinetic energy of the $\mathrm{Rb^+}$ fragment ions can be used to identify dimers formed in either the X $^1Σ_{\mathrm{g}}^+$ ground state or in the lowest-lying triplet state, a $^3Σ_{\mathrm{u}}^+$. From the experiment, we estimate the abundance ratio of dimers in the a and X states as a function of the mean droplet size and find values between 4:1 and 5:1. Our technique applies generally to dimers and trime…
We use a novel technique to solvate silver cations in small clusters of noble gases. The technique involves formation of large, superfluid helium nanodroplets that are subsequently electron ionized, mass-selected by deflection in an electric field, and doped with silver atoms and noble gases (Ng) in pickup cells. Excess helium is then stripped from the doped nanodroplets by multiple collisions with helium gas at room temperature, producing cluster ions that contain no more than a few dozen noble gas atoms and just a few (or no) silver atoms. Under gentle stripping conditions helium atoms remai…