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 field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. 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 approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7-9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 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 interactions11. 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 attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

4D spatio-temporal electric field characterization of ultrashort light pulses undergoing filamentation.

We present an experimental method capable of capturing the complete spatio-temporal dynamics of filamenting ultrashort laser pulses. By employing spatially resolved Fourier transform spectrometry in combination with the capability to terminate the filament at any length, we can follow the nonlinear dynamics in four dimensions, i.e. the transverse domain, time and filament length. Our method thus not only enables the full characterization of the filamentation process throughout its evolution, but also allows to identify and select laser pulses with desired parameters.

All-optical measurement of the complete waveform of octave-spanning ultrashort light pulses.

We demonstrate the complete temporal characterization of the optical waveform of visible near-infrared octave-spanning ultrashort laser pulses, using an all-optical, all-solid-state, and fully inline dispersion-scan device based only on second-harmonic generation.

Compact single-shot d-scan setup for the characterization of few-cycle laser pulses.

We present a compact implementation of the ultrashort pulse measurement technique based on dispersion scans (d-scan), allowing single-shot measurement of few-cycle pulses. The main novelty in our design, making our setup extremely compact and simple, is the use, after a prism, of a spherical mirror in an off-axis geometry. The intentionally introduced strong astigmatism makes it possible to image the output of the crystal in one direction while focusing it in the other direction, resulting in the output face of the prism being imaged into a line in the second-harmonic crystal. The technique is validated by comparing measured dispersion scans, retrieved spectral phases and temporal profiles of this single-shot system with standard d-scan results.

Attosecond electron-spin dynamics in Xe 4d photoionization.

The photoionization of xenon atoms in the 70-100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe+ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as, and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide insight into the complex electron-spin dynamics of photo-induced phenomena.