Intense, mutually coherent beams of multiharmonic extreme ultraviolet light can now be created using seeded free-electron lasers, and the phase difference between harmonics can be tuned with attosecond accuracy. However, the absolute value of the phase is generally not determined. We present a method for determining precisely the absolute phase relationship of a fundamental wavelength and its second harmonic, as well as the amplitude ratio. Only a few easily calculated theoretical parameters are required in addition to the experimental data.

Single-photon laser enabled Auger decay (spLEAD) is an electronic de-excitation process which was recently predicted and observed in Ne. We have investigated it using bichromatic phase-locked free electron laser radiation and extensive angle-resolved photoelectron measurements, supported by a detailed theoretical model. We first used separately the fundamental wavelength resonant with the Ne⁺ 2s–2p transition, 46.17 nm, and its second harmonic, 23.08 nm, then their phase-locked bichromatic combination. In the latter case the phase difference between the two wavelengths was scanned, and interference effects were observed, confirming that the spLEAD process was occurring. The detailed theoretical model we developed qualitatively predicts all observations: branching ratios between the final Auger states, their amplitudes of oscillation as a function of phase, the phase lag between the oscillations of different final states, and partial cancellation of the oscillations under certain conditions.

We present a compact experimental setup for performing attosecond-pump-infrared-probe experiments with long-time delay stability. The robustness of the setup is demonstrated over a two-day acquisition time in two-photon photoionization of argon in the photon-energy range 17−33 eV. The propagation of the input infrared pulse, as driving pulse for the high-order harmonic generation process and for the generation of the sidebands of the main photoelectron peaks, through the main optical components is simulated and discussed. Our setup allows us to perform attosecond experiments with an overall stability of ± 40 as.

Free-electron lasers (FELs) can produce radiation in the short wavelength range extending from the extreme ultraviolet (XUV) to the X-rays with a few to a few tens of femtoseconds pulse duration. These facilities have enabled significant breakthroughs in the field of atomic, molecular, and optical physics, implementing different schemes based on two-color photoionization mechanisms. In this article, we present the generation of attosecond pulse trains (APTs) at the seeded FEL FERMI using the beating of multiple phase-locked harmonics. We demonstrate the complex attosecond waveform shaping of the generated APTs, exploiting the ability to manipulate independently the amplitudes and the phases of the harmonics. The described generalized attosecond waveform synthesis technique with an arbitrary number of phase-locked harmonics will allow the generation of sub-100 as pulses with programmable electric fields.