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Ramsey-comb spectroscopy with intense ultrashort laser pulses

Optical frequency combs based on mode-locked lasers have revolutionised 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 employed 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 show that the full frequency comb accuracy and resolution can be obtained 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 novel properties of this approach, such as cancellation of optical light-shift effects, is demonstrated on weak two-photon transitions in atomic rubidium and caesium, thereby improving the frequency accuracy up to thirty times.