Attosecond Time-resolved Photoelectron Spectroscopy Research Articles

Attosecond science in liquid phase

Chemical Physics Many physical properties of liquid water remain unresolved due to the very fast dynamics involved in the liquid phase. Using attosecond time-resolved photoelectron spectroscopy, Jordan et al. found that photoemission of electrons from water in the liquid phase shows a time delay of about 50 to 70 attoseconds compared with photoemission from the gas phase. This difference was attributed to solvation effects and was validated by analysis of various contributions to the measured delays and by using theoretical simulations in water clusters of different sizes. Science , this issue p. [974][1] [1]: /lookup/doi/10.1126/science.abb0979

Reconstruction of attosecond pulses in the presence of interfering dressing fields using a 100 kHz laser system at ELI-ALPS

Attosecond Pulse Trains (APT) generated by high-harmonic generation (HHG) of high-intensity near-infrared (IR) laser pulses have proven valuable for studying the electronic dynamics of atomic and molecular species. However, the high intensities required for high-photon-energy, high-flux HHG usually limit the class of adequate laser systems to repetition rates below 10 kHz. Here, APT’s generated from the 100 kHz, 160 W, 40 fs laser system (HR-1) currently under commissioning at the extreme light infrastructure attosecond light pulse source (ELI-ALPS) are reconstructed using the reconstruction of attosecond beating by interference of two-photon Transitions (RABBIT) technique. These experiments constitute the first attosecond time-resolved photoelectron spectroscopy measurements with attosecond pulses performed at 100 kHz repetition rate and one of the first experiments performed at ELI-ALPS in the framework of projects commissioning its newly installed technologies. These RABBIT measurements were taken with an additional IR field temporally locked to the extreme-ultraviolet APT, resulting in an atypical ω beating. We show that the phase of the 2ω beating recorded under these conditions is strictly identical to that observed in standard RABBIT measurements within second-order perturbation theory. This work highlights an experimental simplification for future experiments based on attosecond interferometry (or RABBIT), which is particularly useful when lasers with high average powers are used.

First-principles simulations for attosecond photoelectron spectroscopy based on time-dependent density functional theory

We develop a first-principles simulation method for attosecond time-resolved photoelectron spectroscopy. This method enables us to directly simulate the whole experimental processes, including excitation, emission and detection on equal footing. To examine the performance of the method, we use it to compute the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) experiments of gas-phase Argon. The computed RABBITT photoionization delay is in very good agreement with recent experimental results from [Klünder et al., Phys. Rev. Lett. 106, 143002 (2011)] and [Guénot et al., Phys. Rev. A 85, 053424 (2012)]. This indicates the significance of a fully-consistent theoretical treatment of the whole measurement process to properly describe experimental observables in attosecond photoelectron spectroscopy. The present framework opens the path to unravel the microscopic processes underlying RABBITT spectra in more complex materials and nanostructures.

Attosecond photoelectron streaking with enhanced energy resolution for small-bandgap materials.

Attosecond photoelectron streaking spectroscopy allows time-resolved electron dynamics with a temporal resolution approaching the atomic unit of time. Studies have been performed in numerous systems, including atoms, molecules, and surfaces, and the quest for ever higher temporal resolution called for ever wider spectral extent of the attosecond pulses. For typical experiments relying on attosecond pulses with a duration of 200as, the time-bandwidth limitation for a Gaussian pulse implies a minimal spectral bandwidth larger than 9eV translating to a corresponding spread of the detected photoelectron kinetic energies. Here, by utilizing a specially tailored narrowband reflective XUV multilayer mirror, we explore experimentally the minimal spectral width compatible with attosecond time-resolved photoelectron spectroscopy while obtaining the highest possible spectral resolution. The validity of the concept is proven by recording attosecond electron streaking traces from the direct semiconductor gallium arsenide (GaAs), with a nominal bandgap of 1.42eV at room temperature, proving the potential of the approach for tracking charge dynamics also in these technologically highly relevant materials that previously have been inaccessible to attosecond science.

Photoelectron spectrometer for attosecond spectroscopy of liquids and gases.

A new apparatus for attosecond time-resolved photoelectron spectroscopy of liquids and gases is described. It combines a liquid microjet source with a magnetic-bottle photoelectron spectrometer and an actively stabilized attosecond beamline. The photoelectron spectrometer permits venting and pumping of the interaction chamber without affecting the low pressure in the flight tube. This pressure separation has been realized through a sliding skimmer plate, which effectively seals the flight tube in its closed position and functions as a differential pumping stage in its open position. A high-harmonic photon spectrometer, attached to the photoelectron spectrometer, exit port is used to acquire photon spectra for calibration purposes. Attosecond pulse trains have been used to record photoelectron spectra of noble gases, water in the gas and liquid states as well as solvated species. RABBIT scans demonstrate the attosecond resolution of this setup.