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We present an experiment demonstrating high-resolution coherent control of afour-level atomic system in a closed (diamond) type configuration. Afemtosecond frequency comb is used to establish phase coherence between a pairof two-photon transitions in cold Rb atoms. By controlling the spectral phaseof the frequency comb we demonstrate the optical phase sensitive response ofthe diamond system. The high-resolution state selectivity of the comb is usedto demonstrate the importance of the signs of dipole moment matrix elements inthis type of closed-loop excitation. Finally, the pulse shape is optimizedresulting in a 256% increase in the two-photon transition rate by forcingconstructive interference between the mode pairs detuned from an intermediateresonance.

Control of Four-Level Quantum Coherence via Discrete Spectral Shaping of an Optical Frequency Comb