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Optical Measurement of Photorecombination Time Delays

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 Publication date 2021
  fields Physics
and research's language is English




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Measuring the photoionization time delay between electrons from different orbitals is one of the most important accomplishments of attosecond science. These measurements are typically done using attosecond pulses to photoionize a target inside a photoelectron spectrometer. In such experiments, the measured delay corresponds to the superposition of all possible paths to ionization and can include multiple sources of delay. These effects can be difficult to deconvolve. Here, we exploit the collision physics nature of recollision and show that, by perturbing recollision dynamics, photorecombination time delays due to electron dynamics and structure can be measured entirely optically and without obfuscation from molecular structure and propagation effects. While we concentrate on photorecombination delays in argon around the Cooper minimum our approach is general. Therefore, our work holds the potential to fundamentally change how attosecond measurement is performed and paves the way for the entirely optical measurement of ultrafast electron dynamics and photorecombination delays due to electronic structure, multielectron interaction, and strong-field driven dynamics in complex molecular systems and correlated solid-state systems.



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This tutorial presents an introduction to the interaction of light and matter on the attosecond timescale. Our aim is to detail the theoretical description of ultra-short time-delays, and to relate these to the phase of extreme ultraviolet (XUV) light pulses and to the asymptotic phase-shifts of photoelectron wave packets. Special emphasis is laid on time-delay experiments, where attosecond XUV pulses are used to photoionize target atoms at well-defined times, followed by a probing process in real time by a phase-locked, infrared laser field. In this way, the laser field serves as a clock to monitor the ionization event, but the observable delays do not correspond directly to the delay associated with single-photon ionization. Instead, a significant part of the observed delay originates from a measurement induced process, which obscures the single-photon ionization dynamics. This artifact is traced back to a phase-shift of the above-threshold ionization transition matrix element, which we call the continuum-continuum phase. It arises due to the laser-stimulated transitions between Coulomb continuum states. As we shall show here, these measurement-induced effects can be separated from the single-photon ionization process, using analytical expressions of universal character, so that eventually the attosecond time-delays in photoionization can be accessed.
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