  We present an experiment demonstrating high-resolution coherent control of a
four-level atomic system in a closed (diamond) type configuration. A
femtosecond frequency comb is used to establish phase coherence between a pair
of two-photon transitions in cold Rb atoms. By controlling the spectral phase
of the frequency comb we demonstrate the optical phase sensitive response of
the diamond system. The high-resolution state selectivity of the comb is used
to demonstrate the importance of the signs of dipole moment matrix elements in
this type of closed-loop excitation. Finally, the pulse shape is optimized
resulting in a 256% increase in the two-photon transition rate by forcing
constructive interference between the mode pairs detuned from an intermediate
resonance.
