  We thoroughly investigate vibrational quantum dynamics of dimers attached to
He droplets motivated by recent measurements with K-2 [1]. For those
femtosecond pump-probe experiments, crucial observed features are not
reproduced by gas phase calculations but agreement is found using a description
based on dissipative quantum dynamics, as briefly shown in [2]. Here we present
a detailed study of the influence of possible effects induced by the droplet.
The helium droplet causes electronic decoherence, shifts of potential surfaces,
and relaxation of wave packets in attached dimers. Moreover, a realistic
description of (stochastic) desorption of dimers off the droplet needs to be
taken into account. Step by step we include and study the importance of these
effects in our full quantum calculation. This allows us to reproduce and
explain all major experimental findings. We find that desorption is fast and
occurs already within 2-10 ps after electronic excitation. A further finding is
that slow vibrational motion in the ground state can be considered
frictionless.
