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Physical Review Letters

Kilohertz-level spectroscopy of cold atoms with a femtosecond optical frequency comb

Tara M. Fortier, Yann Le Coq, J. E. Stalnaker, D. Ortega, Scott A. Diddams, Christopher W. Oates, Leo W. Hollberg

Published Oct 19, 2006• 0 citations
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A mode-locked femtosecond laser is used to physically map the laser frequency comb into the velocity comb of the excited Rb atoms at room temperature. Upon resonant excitation by discrete optical frequencies the velocity distribution of the excited Rb atoms shows comblike structure. Simultaneously, velocity-selective population transfer occurs between ground-state hyperfine levels. Both facts are observed by modified direct frequency comb spectroscopy and verified by a detailed density matrix treatment of the multilevel system in resonant field.
We present direct observation of the velocity-selective optical pumping of the Rb ground state hyperfine levels induced by 5S(1/2) --> 5P(1/2) femtosecond pulse-train excitation. A modified direct frequency comb spectroscopy based on the fixed frequency comb and a weak cw scanning probe laser was developed. The femtosecond pulse-train excitation of a Doppler-broadened Rb four-level atomic vapor is investigated theoretically in the context of the density matrix formalism and the results are compared with the experiment.
We present experiments demonstrating high-resolution and wide-bandwidth coherent control of a four-level atomic system in a diamond configuration. A femtosecond frequency comb is used to excite a specific pair of two-photon transitions in cold 87Rb. The optical-phase-sensitive response of the closed-loop diamond system is studied by controlling the phase of the comb modes with a pulse shaper. 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.