13 research outputs found
Extreme timescale core-level spectroscopy with tailored XUV pulses
A new approach for few-femtosecond time-resolved photoelectron spectroscopy
in condensed matter that balances the combined needs for both temporal and
energy resolution is demonstrated. Here, the method is designed to investigate
a prototypical Mott insulator, tantalum disulphide (1T-TaS2), which transforms
from its charge-density-wave ordered Mott insulating state to a conducting
state in a matter of femtoseconds. The signature to be observed through the
phase transition is a charge-density-wave induced splitting of the Ta 4f
core-levels, which can be resolved with sub-eV spectral resolution. Combining
this spectral resolution with few-femtosecond time resolution enables the
collapse of the charge ordered Mott state to be clocked. Precise knowledge of
the sub-20-femtosecond dynamics will provide new insight into the physical
mechanism behind the collapse and may reveal Mott physics on the timescale of
electronic hopping.Comment: 20 pages, 6 figure
Femtosecond profiling of shaped x-ray pulses
Arbitrary manipulation of the temporal and spectral properties of x-ray pulses at free-electron lasers would revolutionize many experimental applications. At the Linac Coherent Light Source at Stanford National Accelerator Laboratory, the momentum phase-space of the free-electron laser driving electron bunch can be tuned to emit a pair of x-ray pulses with independently variable photon energy and femtosecond delay. However, while accelerator parameters can easily be adjusted to tune the electron bunch phase-space, the final impact of these actuators on the x-ray pulse cannot be predicted with sufficient precision. Furthermore, shot-to-shot instabilities that distort the pulse shape unpredictably cannot be fully suppressed. Therefore, the ability to directly characterize the x-rays is essential to ensure precise and consistent control. In this work, we have generated x-ray pulse pairs via electron bunch shaping and characterized them on a single-shot basis with femtosecond resolution through time-resolved photoelectron streaking spectroscopy. This achievement completes an important step toward future x-ray pulse shaping techniques
Clocking Auger electrons
Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving it in inherently unstable states that decay on femtosecond timescales. The relaxation occurs primarily via Auger emission, so excited-state observations are constrained by Auger decay. In situ measurement of this process is therefore crucial, yet it has thus far remained elusive in XFELs owing to inherent timing and phase jitter, which can be orders of magnitude larger than the timescale of Auger decay. Here we develop an approach termed ‘self-referenced attosecond streaking’ that provides subfemtosecond resolution in spite of jitter, enabling time-domain measurement of the delay between photoemission and Auger emission in atomic neon excited by intense, femtosecond pulses from an XFEL. Using a fully quantum-mechanical description that treats the ionization, core-hole formation and Auger emission as a single process, the observed delay yields an Auger decay lifetime of 2.2_−0.3^+0.2 fs for the KLL decay channel
Clocking Auger Electrons
Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving
it in inherently unstable states that decay on femtosecond timescales. As the
relaxation occurs primarily via Auger emission, excited state observations are
constrained by Auger decay. In situ measurement of this process is therefore
crucial, yet it has thus far remained elusive at XFELs due to inherent timing
and phase jitter, which can be orders of magnitude larger than the timescale of
Auger decay. Here, we develop a new approach termed self-referenced attosecond
streaking, based upon simultaneous measurements of streaked photo- and Auger
electrons. Our technique enables sub-femtosecond resolution in spite of jitter.
We exploit this method to make the first XFEL time-domain measurement of the
Auger decay lifetime in atomic neon, and, by using a fully quantum-mechanical
description, retrieve a lifetime of fs for the KLL
decay channel. Importantly, our technique can be generalised to permit the
extension of attosecond time-resolved experiments to all current and future FEL
facilities.Comment: Main text: 20 pages, 3 figures. Supplementary information: 17 pages,
6 figure
Coherent spectral enhancement of carrier-envelope-phase stable continua with dual-gas high harmonic generation
Attosecond science is enabled by the ability to convert femtosecond near-infrared laser light into coherent harmonics in the extreme ultraviolet spectral range. While attosecond sources have been utilized in experiments that have not demanded high intensities, substantially higher photon flux would provide a natural link to the next significant experimental breakthrough. Numerical simulations of dual-gas high harmonic generation indicate that the output in the cutoff spectral region can be selectively enhanced without disturbing the single-atom gating mechanism. Here, we summarize the results of these simulations and present first experimental findings to support these predictions
Sub-Femtosecond Free-Electron Laser Pulses
Deploying the so-called ‘Streaking Spectroscopy’ technique at LCLS, we demonstrate a non-invasive scheme for temporal characterization of X-ray pulses with sub-femtosecond resolution. Analyzing the substructure indicates pulse durations on the order of hundreds of attoseconds
Angle-Resolved Electron Spectroscopy of Laser-Assisted Auger Decay Induced by a Few-Femtosecond X-Ray Pulse
Two-color (x−ray+infrared) electron spectroscopy is used for investigating laser-assisted KLL Auger decay following 1s photoionization of atomic Ne with few-femtosecond x-ray pulses from the Linac Coherent Light Source. In an angle-resolved experiment, the overall width of the laser-modified Auger-electron spectrum and its structure change significantly as a function of the emission angle. The spectra are characterized by a strong intensity variation of the sidebands revealing a gross structure. This variation is caused, as predicted by theory, by the interference of electrons emitted at different times within the duration of one optical cycle of the infrared dressing laser, which almost coincides with the lifetime of the Ne 1s vacancy