Observation of Rabi dynamics with a short-wavelength free-electron laser

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field 1 . They are ubiquitous in physics with applications in different areas such as photonics 2 , nano-electronics 3 , electron microscopy 4 and quantum information 5 . While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation 6 . Although intense nanometre-wavelength light sources have been available for more than a decade 7 – 9 , Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser 10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions 11 . Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond 12 and few-femtosecond 13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.