Photoelectron interferometry with spectrally shaped polychromatic infrared pulses

Abstract

Laser-assisted photoelectron interferometry is a cornerstone of attosecond science, first used to characterize attosecond pulse trains and later to study photoionization dynamics. Extending this method to spectrally shaped polychromatic infrared probe fields enables encoding of information across multiple interferometric pathways within the photoelectron spectrum. Here, we experimentally demonstrate laser-assisted photoelectron interferometry using a spectrally shaped polychromatic infrared probe field composed of five distinct spectral components forming a Golomb ruler in the frequency domain. The measured interferograms exhibit multiple beating frequencies that agree with theoretical calculations, demonstrating the simultaneous encoding of multiple laser-assisted quantum beats in a single measurement. A quantitative analysis of the beating amplitudes shows that the strongly modulated temporal profile of the polychromatic probe introduces intensity- and delay-dependent distortions of the quantum beats that cannot be explained by second-order perturbation theory. These results establish the conditions required for the quantitative interpretation of polychromatic photoelectron interferometry and highlight the opportunities offered by spectro-temporal engineering of the probe field for future developments in attosecond science.