Alkali Atoms Attached to 3^3He Nanodroplets

We have experimentally studied the electronic $3p-> 3s$ excitation of Na atoms attached to $^3$He droplets by means of laser-induced fluorescence as well as beam depletion spectroscopy. From the similarities of the spectra (width/shift of absorption lines) with these of Na on $^4$He droplets, we conclude that sodium atoms reside in a ``dimple'' on the droplet surface and that superfluid-related effects are negligible. The experimental results are supported by Density Functional calculations at zero temperature, which confirm the surface location of Na, K and Rb atoms on $^3$He droplets. In the case of Na, the calculated shift of the excitation spectra for the two isotopes is in good agreement with the experimental data.Comment: 6 pages, 3 figures, sent to JLT

Kilohertz laser ablation for doping helium nanodroplets

A new setup for doping helium nanodroplets by means of laser ablation at kilohertz repetition rate is presented. The doping process is characterized and two distinct regimes of laser ablation are identified. The setup is shown to be efficient and stable enough to be used for spectroscopy, as demonstrated on beam-depletion spectra of lithium atoms attached to helium nanodroplets. For the first time, helium droplets are doped with high temperature refractory materials such as titanium and tantalum. Doping with the non-volatile DNA basis Guanine is found to be efficient and a number of oligomers are detected

High-resolution spectroscopy of triplet states of Rb2 by femtosecond pump-probe photoionization of doped helium nanodroplets

The dynamics of vibrational wave packets in triplet states of rubidium dimers (Rb2) formed on helium nanodroplets are studied using femtosecond pump-probe photoionization spectroscopy. Due to fast desorption of the excited Rb2 molecules off the droplets and due to their low internal temperature, wave packet oscillations can be followed up to very long pump-probe delay times >1.5ns. In the first excited triplet state (1)^3\Sigma_g^+, full and fractional revivals are observed with high contrast. Fourier analysis provides high-resolution vibrational spectra which are in excellent agreement with ab initio calculations

Spectroscopy of PTCDA attached to rare gas samples: clusters vs. bulk matrices. I. Absorption spectroscopy

The interaction between PTCDA (3,4,9,10-perylene-tetracarboxylic-dianhydride) and rare gas or para-hydrogen samples is studied by means of laser-induced fluorescence excitation spectroscopy. The comparison between spectra of PTCDA embedded in a neon matrix and spectra attached to large neon clusters shows that these large organic molecules reside on the surface of the clusters when doped by the pick-up technique. PTCDA molecules can adopt different conformations when attached to argon, neon and para-hydrogen clusters which implies that the surface of such clusters has a well-defined structure and has not liquid or fluxional properties. Moreover, a precise analysis of the doping process of these clusters reveals that the mobility of large molecules on the cluster surface is quenched, preventing agglomeration and complex formation

Stability of two-component alkali clusters formed on helium nanodroplets

The stability of two-component clusters consisting of light (Na or K) and heavy (Rb or Cs) alkali atoms formed on helium nanodroplets is studied by femtosecond laser ionization in combination with mass spectrometry. Characteristic stability patterns reflecting electron shell-closures are observed in dependence of the total number of atoms contained in the mixed clusters. Faster decay of the stability of mixed clusters compared to the pure light ones as a function of size indicates a destabilizing effect of heavy alkali atoms on light alkali clusters, presumably due to second order spin-orbit interaction