Ultrafast extreme-ultraviolet reflection spectroscopy of electro-phonon dynamics in Germanium
2017
Ultrafast transient reflection spectroscopy in the extreme UV (XUV) is developed as a new technique for following bandgap
dynamics after photoexcitation. Signatures of carrier and lattice dynamics are obsd. through the measurement of
reflectivity changes in the XUV of single-cryst. germanium after exciting the sample with a sub-5 fs visible-to-IR pulse. In
the expt., a 5 fs near IR (NIR) pulse excites carriers across the band gap. The subsequent dynamics are probed by
measuring the transient reflectivity changes at the Ge M_(4,5) edge around 30 eV, corresponding to transitions from the 3d
core levels to the unoccupied conduction and valence band states. The energetically sepd. spectral signatures of
photoexcited electrons and holes in the XUV enable to measure the thermalization dynamics of the carriers. Importantly,
shifts in photon energy of the electron and hole features allow real time tracking of the energy sepn. of valence and
conduction bands change over time. The dynamics obsd. in the expts. suggest dynamics on different time scales.
Within 500fs, decays and energetic shifts of the obsd. reflectivity changes occur, which are assigned to electron-electron
and electron-optical phonon scattering thermalizing the photoexcited carrier distribution. Within 2 ps, a blue shift of the
valence band features is obsd., whereas a red shift of the conduction band features is present. This striking observation
is assigned to a renormalization of the band gap due to the lattice expansion of the crystal. This band-gap
renormalization sets in once momentum of the excited carriers has been transferred to phonons by electron-phonon and
phonon-phonon scattering. Transient reflectivity is shown to overcome the thin-film and x-ray membrane related issues
of transmission geometries. It will be shown how transient reflectivity can further be employed to ext. the time-dependent
complex dielec. function over the timescales governing carrier-carrier, carrier-phonon, and phonon-phonon interactions.
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