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We experimentally investigate various processes present in thephotoassociative interaction of an ultracold atomic sample with shapedfemtosecond laser pulses. We demonstrate the photoassociation of pairs ofrubidium atoms into electronically excited, bound molecular states usingspectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of themolecular formation rate, which are due to coherent transient dynamics in theelectronic excitation. The oscillation frequency corresponds to the detun-ingof the spectral cut position to the asymptotic transition frequency of therubidium D1 or D2 lines, respectively. Measurements of the molecularphotoassociation signal as a function of the pulse energy reveal a non-lineardependence and indicate a non-perturbative excitation process. Chirping theassociation laser pulse allowed us to change the phase of the coherenttransients. Furthermore, a signature for molecules in the electronic groundstate is found, which is attributed to molecule formation by femtosecondphotoassociation followed by spontaneous decay. In a subsequent article [A.Merli et al., submitted] quantum mechanical calculations are presented, whichcompare well with the experimental data and reveal further details about theobserved coherent transient dynamics.

Photoassociation and coherent transient dynamics in the interaction of ultracold rubidium atoms with shaped femtosecond pulses - I. Experiment