High-Precision Spectroscopy with Counter-Propagating Femtosecond Pulses

An experimental realization of high-precision direct frequency comb spectroscopy using counter-propagating femtosecond pulses on two-photon atomic transitions is presented. Doppler broadened background signal, hampering precision spectroscopy with ultrashort pulses, is effectively eliminated with a simple pulse shaping method. As a result, all four 5S-7S two-photon transitions in a rubidium vapor are determined with both statistical and systematic uncertainties below 10$^{-11}$, which is an order of magnitude better than previous experiments on these transitions.Comment: 5 pages, 4 figures. Accepted to PR

Spatial and Spectral Coherent Control with Frequency Combs

Quantum coherent control (1-3) is a powerful tool for steering the outcome of quantum processes towards a desired final state, by accurate manipulation of quantum interference between multiple pathways. Although coherent control techniques have found applications in many fields of science (4-9), the possibilities for spatial and high-resolution frequency control have remained limited. Here, we show that the use of counter-propagating broadband pulses enables the generation of fully controlled spatial excitation patterns. This spatial control approach also provides decoherence reduction, which allows the use of the high frequency resolution of an optical frequency comb (10,11). We exploit the counter-propagating geometry to perform spatially selective excitation of individual species in a multi-component gas mixture, as well as frequency determination of hyperfine constants of atomic rubidium with unprecedented accuracy. The combination of spectral and spatial coherent control adds a new dimension to coherent control with applications in e.g nonlinear spectroscopy, microscopy and high-precision frequency metrology.Comment: 12 page

Ramsey-comb spectroscopy with intense ultrashort laser pulses

Optical frequency combs based on mode-locked lasers have revolutionized the field of metrology and precision spectroscopy by providing precisely calibrated optical frequencies and coherent pulse trains. Amplification of the pulsed output from these lasers is very desirable, as nonlinear processes can then be used to cover a much wider range of transitions and wavelengths for ultra-high precision, direct frequency comb spectroscopy. Therefore full repetition rate laser amplifiers and enhancement resonators have been employed to produce up to microjoule-level pulse energies. Here we present a spectroscopic method to obtain frequency comb accuracy and resolution by using only two frequency comb pulses amplified to the millijoule pulse energy level, orders of magnitude more energetic than what has previously been possible. The new properties of this approach, such as cancellation of optical light-shift effects, are demonstrated on weak two-photon transitions in atomic rubidium and caesium, thereby improving the frequency accuracy by up to thirty times