Deep-ultraviolet quantum interference metrology with ultrashort laser pulses

Precision spectroscopy at ultraviolet and shorter wavelengths has been hindered by the poor access of narrow-band lasers to that spectral region. We demonstrate high-accuracy quantum interference metrology on atomic transitions with the use of an amplified train of phase-controlled pulses from a femtosecond frequency comb laser. The peak power of these pulses allows for efficient harmonic upconversion, paving the way for extension of frequency comb metrology in atoms and ions to the extreme ultraviolet and soft x-ray spectral regions. A proof-of-principle experiment was performed on a deep-ultraviolet (2 × 212.55 nanometers) two-photon transition in krypton; relative to measurement with single nanosecond laser pulses, the accuracy of the absolute transition frequency and isotope shifts was improved by more than an order of magnitude.