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.
We determine relative photoemission time delays between valence electrons in different noble gas atoms (Ar, Ne and He) in an energy range between 31 and 37 eV. The atoms are ionized by an attosecond pulse train synchronized with an infrared laser field and the delays are measured using an interferometric technique. We compare our results with calculations using the random phase approximation with exchange and multi-configurational Hartree-Fock. We also investigate the influence of the different ionization angular channels.
We measure spectrally and spatially resolved high-order harmonics generated in argon using chirped multi-cycle laser pulses. Using a stable, high-repetition rate laser we observe detailed interference structures in the far-field. The structures are of two kinds; off-axis interference from the long trajectory only and on-axis interference including the short and long trajectories. The former is readily visible in the far-field spectrum, modulating both the spectral and spatial profile. To access the latter, we vary the chirp of the fundamental, imparting different phases on the different trajectories, thereby changing their relative phase. Using this method together with an analytical model, we are able to explain the on-axis behaviour and access the dipole phase parameters for the short (a s ) and long (a l ) trajectories. The extracted results compare very well with phase parameters calculated by solving the time-dependent Schrödinger equation. Going beyond the analytical model, we are also able to successfully reproduce the off-axis interference structure.
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