  We experimentally investigate various processes present in the
photoassociative interaction of an ultracold atomic sample with shaped
femtosecond laser pulses. We demonstrate the photoassociation of pairs of
rubidium atoms into electronically excited, bound molecular states using
spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2
asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the
molecular formation rate, which are due to coherent transient dynamics in the
electronic excitation. The oscillation frequency corresponds to the detun-ing
of the spectral cut position to the asymptotic transition frequency of the
rubidium D1 or D2 lines, respectively. Measurements of the molecular
photoassociation signal as a function of the pulse energy reveal a non-linear
dependence and indicate a non-perturbative excitation process. Chirping the
association laser pulse allowed us to change the phase of the coherent
transients. Furthermore, a signature for molecules in the electronic ground
state is found, which is attributed to molecule formation by femtosecond
photoassociation followed by spontaneous decay. In a subsequent article [A.
Merli et al., submitted] quantum mechanical calculations are presented, which
compare well with the experimental data and reveal further details about the
observed coherent transient dynamics.
