61 research outputs found
Tracking the surface atomic motion in a coherent phonon oscillation
X-ray photoelectron diffraction is a powerful tool for determining the
structure of clean and adsorbate-covered surfaces. Extending the technique into
the ultrafast time domain will open the door to studies as diverse as the
direct determination of the electron-phonon coupling strength in solids and the
mapping of atomic motion in surface chemical reactions. Here we demonstrate
time-resolved photoelectron diffraction using ultrashort soft X-ray pulses from
the free electron laser FLASH. We collect Se 3d photoelectron diffraction
patterns over a wide angular range from optically excited BiSe with a
time resolution of 140 fs. Combining these with multiple scattering simulations
allows us to track the motion of near-surface atoms within the first 3 ps after
triggering a coherent vibration of the A optical phonons. Using a
fluence of 4.2 mJ/cm from a 1.55 eV pump laser, we find the resulting
coherent vibrational amplitude in the first two interlayer spacings to be on
the order of 1 pm
Quantum Imaging with Incoherently Scattered Light from a Free-Electron Laser
The advent of accelerator-driven free-electron lasers (FEL) has opened new
avenues for high-resolution structure determination via diffraction methods
that go far beyond conventional x-ray crystallography methods. These techniques
rely on coherent scattering processes that require the maintenance of
first-order coherence of the radiation field throughout the imaging procedure.
Here we show that higher-order degrees of coherence, displayed in the intensity
correlations of incoherently scattered x-rays from an FEL, can be used to image
two-dimensional objects with a spatial resolution close to or even below the
Abbe limit. This constitutes a new approach towards structure determination
based on incoherent processes, including Compton scattering, fluorescence
emission or wavefront distortions, generally considered detrimental for imaging
applications. Our method is an extension of the landmark intensity correlation
measurements of Hanbury Brown and Twiss to higher than second-order paving the
way towards determination of structure and dynamics of matter in regimes where
coherent imaging methods have intrinsic limitations
Subpicosecond metamagnetic phase transition in FeRh driven by non-equilibrium electron dynamics
In FeRh, it is possible to optically drive a phase transition between ferromagnetic (FM) and anti-ferromagnetic (AFM) ordering. Here, using a combination of photoelectron spectroscopy and ab-initio calculations, the authors demonstrate the existence of a transient intermediate phase, explaining the delayed appearance of the FM phase. Femtosecond light-induced phase transitions between different macroscopic orders provide the possibility to tune the functional properties of condensed matter on ultrafast timescales. In first-order phase transitions, transient non-equilibrium phases and inherent phase coexistence often preclude non-ambiguous detection of transition precursors and their temporal onset. Here, we present a study combining time-resolved photoelectron spectroscopy and ab-initio electron dynamics calculations elucidating the transient subpicosecond processes governing the photoinduced generation of ferromagnetic order in antiferromagnetic FeRh. The transient photoemission spectra are accounted for by assuming that not only the occupation of electronic states is modified during the photoexcitation process. Instead, the photo-generated non-thermal distribution of electrons modifies the electronic band structure. The ferromagnetic phase of FeRh, characterized by a minority band near the Fermi energy, is established 350 +/- 30 fs after the laser excitation. Ab-initio calculations indicate that the phase transition is initiated by a photoinduced Rh-to-Fe charge transfer
The soft x-ray instrument for materials studies at the linac coherent light source x-ray free-electron laser
This content may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This material originally appeared in Review of Scientific Instruments 83, 043107 (2012) and may be found at https://doi.org/10.1063/1.3698294.The soft x-ray materials science instrument is the second operational beamline at the linac coherent light source x-ray free electron laser. The instrument operates with a photon energy range of 480–2000 eV and features a grating monochromator as well as bendable refocusing mirrors. A broad range of experimental stations may be installed to study diverse scientific topics such as: ultrafast chemistry, surface science, highly correlated electron systems, matter under extreme conditions, and laboratory astrophysics. Preliminary commissioning results are presented including the first soft x-ray single-shot energy spectrum from a free electron laser
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