Ultrafast processes in matter, such as the electron emission after light absorption, can now be studied using ultrashort light pulses of attosecond duration (10 seconds) in the extreme ultraviolet spectral range. The lack of spectral resolution due to the use of short light pulses has raised issues in the interpretation of the experimental results and the comparison with theoretical calculations. We determine photoionization time delays in neon atoms over a 40-electron volt energy range with an interferometric technique combining high temporal and spectral resolution. We spectrally disentangle direct ionization from ionization with shake-up, in which a second electron is left in an excited state, and obtain excellent agreement with theoretical calculations, thereby solving a puzzle raised by 7-year-old measurements.

We present a simple and robust technique to retrieve the phase of ultrashort laser pulses, based on a chirped mirror and glass wedges compressor. It uses the compression system itself as a diagnostic tool, thereby making unnecessary the use of complementary diagnostic tools. We used this technique to compress and characterize 7.1 fs laser pulses from an ultrafast laser oscillator.

We present experimental measurements and theoretical calculations of photoionization time delays from the 3s and 3p shells in Ar in the photon energy range of 32-42 eV. The experimental measurements are performed by interferometry using attosecond pulse trains and the infrared laser used for their generation. The theoretical approach includes intershell correlation effects between the 3s and 3p shells within the framework of the random phase approximation with exchange (RPAE). The connection between single-photon ionization and the two-color two-photon ionization process used in the measurement is established using the recently developed asymptotic approximation for the complex transition amplitudes of laser-assisted photoionization. We compare and discuss the theoretical and experimental results especially in the region where strong intershell correlations in the 3s → kp channel lead to an induced "Cooper" minimum in the 3s ionization cross-section.

We present an analysis and demonstration of few-cycle ultrashort laser pulse characterization using second-harmonic dispersion scans and numerical phase retrieval algorithms. The sensitivity and robustness of this technique with respect to noise, measurement bandwidth and complexity of the measured pulses is discussed through numerical examples and experimental results. Using this technique, we successfully demonstrate the characterization of few-cycle pulses with complex and structured spectra generated from a broadband ultrafast laser oscillator and a high-energy hollow fiber compressor.

Electron dynamics induced by resonant absorption of light is of fundamental importance in nature and has been the subject of countless studies in many scientific areas. Above the ionization threshold of atomic or molecular systems, the presence of discrete states leads to autoionization, which is an interference between two quantum paths: direct ionization and excitation of the discrete state coupled to the continuum. Traditionally studied with synchrotron radiation, the probability for autoionization exhibits a universal Fano intensity profile as a function of excitation energy. However, without additional phase information, the full temporal dynamics cannot be recovered. Here we use tunable attosecond pulses combined with weak infrared radiation in an interferometric setup to measure not only the intensity but also the phase variation of the photoionization amplitude across an autoionization resonance in argon. The phase variation can be used as a fingerprint of the interactions between the discrete state and the ionization continua, indicating a new route towards monitoring electron correlations in time.