Direct frequency-comb-driven Raman transitions in the terahertz range

We demonstrate the use of a femtosecond frequency comb to coherently drive stimulated Raman transitions between terahertz-spaced atomic energy levels. More specifically, we address the 3d ^2D_3/2 and 3d ^2D_5/2 fine structure levels of a single trapped ⁴⁰Ca^+ ion and spectroscopically resolve the transition frequency to be ν_D = 1{,}819{,}599{,}021{,}534 pm 8 Hz. The achieved accuracy is nearly a factor of five better than the previous best Raman spectroscopy, and is currently limited by the stability of our atomic clock reference. Furthermore, the population dynamics of frequency-comb-driven Raman transitions can be fully predicted from the spectral properties of the frequency comb, and Rabi oscillations with a contrast of 99.3(6)% and millisecond coherence time has been achieved. Importantly, the technique can be easily generalized to transitions in the sub-kHz to tens of THz range and should be applicable for driving, e.g., spin-resolved rovibrational transitions in molecules and hyperfine transitions in highly charged ions.