Femtosecond wavepacket interferometry using the rotational dynamics of a trapped cold molecular ion

A Ramsey-type interferometer is suggested, employing a cold trapped ion and two time-delayed off-resonant femtosecond laser pulses. The laser light couples to the molecular polarization anisotropy, inducing rotational wavepacket dynamics. An interferogram is obtained from the delay dependent populations of the final field-free rotational states. Current experimental capabilities for cooling and preparation of the initial state are found to yield an interferogram visibility of more than 80\%. The interferograms can be used to determine the polarizability anisotropy with an accuracy of about $\pm 2\%$, respectively $\pm 5\%$, provided the uncertainty in the initial populations and measurement errors are confined to within the same limits

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 $^{40}$Ca$^+$ ion and spectroscopically resolve the transition frequency to be $\nu_D = 1{,}819{,}599{,}021{,}534 \pm 8$ 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.Comment: 9 pages, 8 figure