Resetting the clock on photoemission: The ability to produce attosecond pulses of light provides access to some of the fastest electronic processes occurring within atoms. Tracking the temporal dynamics of the photoemission process in which an atom absorbs a high-energy photon and the electron escapes has exposed a discrepancy between the initial experimental findings and subsequent theoretical modeling. Isinger et al. present an ultrafast process that can account for and distinguish the different contributions to the photoemission processes in neon atoms. The findings reveal an “electron shake-up” process that may explain the discrepancy, bringing closure to a 7-year discussion. Science , this issue p. 893

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field¹. They are ubiquitous in physics with applications in different areas such as photonics², nano-electronics³, electron microscopy⁴ and quantum information⁵. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation⁶. Although intense nanometre-wavelength light sources have been available for more than a decade^7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser¹⁰ can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions¹¹. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond¹² and few-femtosecond¹³ extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

In a vibrating N ₂ molecule, a mere 2% change in bond length can delay electron emission by 100 attoseconds near a shape resonance.

To better understand the mechanisms of double ionization following the absorption of one photon, a combination of experimental techniques has been developed to probe the electron emission times in xenon on the attosecond timescale. Double ionization following the absorption of a single photon is one of the most fundamental processes requiring interaction between electrons1,2,3. Information about this interaction is usually obtained by detecting emitted particles without access to real-time dynamics. Here, attosecond light pulses4,5, electron wave packet interferometry6 and coincidence techniques7 are combined to measure electron emission times in double ionization of xenon using single ionization as a clock, providing unique insight into the two-electron ejection mechanism. Access to many-particle dynamics in real time is of fundamental importance for understanding processes induced by electron correlation in atomic, molecular and more complex systems.

Using a spectrally resolved electron interferometry technique, we measure photoionization time delays between the $3s$ and $3p$ subshells of argon over a large 34-eV energy range covering the Cooper minima in both subshells. The observed strong variations of the $3s-3p$ delay difference, including a sign change, are well reproduced by theoretical calculations using the two-photon two-color random-phase approximation with exchange. Strong shake-up channels lead to photoelectrons spectrally overlapping with those emitted from the $3s$ subshell. These channels need to be included in our analysis to reproduce the experimental data. Our measurements provide a benchmark for multielectronic theoretical models aiming at an accurate description of interchannel correlation.

The photoionization of xenon atoms in the 70–100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe⁺ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as, and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide insight into the complex electron-spin dynamics of photo-induced phenomena.