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Femtosecond X-ray diffraction from nanolayered oxides

2010, Von Korff Schmising, C., Harpoeth, A., Zhavoronkov, N., Woerner, M., Elsaesser, T., Bargheer, M., Schmidbauer, M., Vrejoiu, I., Hesse, D., Alexe, M.

Femtosecond X-ray scattering offers the opportunity to investigate reversible lattice dynamics with unprecedented accuracy. We show in a prototype experiment how strain propagation modifies the functionality of a ferroelectric system on its intrinsic time scale.

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Femtosecond x-ray diffraction using the rotating crystal method

2013, Freyer, B., Stingl, J., Zamponi, F., Woerner, M., Elsaesser, T.

We demonstrate the rotating-crystal method in femtosecond x-ray diffraction. Structural dynamics of a photoexcited bismuth crystal is mapped in a pump-probe scheme by measuring intensity changes of many Bragg reflections simultaneously.

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Terahertz radiative coupling and damping in multilayer graphene

2014, Bowlan, P., Martinez-Moreno, E., Reimann, K., Woerner, M., Elsaesser, T.

The nonlinear interaction between intense terahertz (THz) pulses and epitaxial multilayer graphene is studied by field-resolved THz pump-probe spectroscopy. THz excitation results in a transient induced absorption with decay times of a few picoseconds, much faster than carrier recombination in single graphene layers. The decay times increase with decreasing temperature and increasing amplitude of the excitation. This behaviour originates from the predominant coupling of electrons to the electromagnetic field via the very strong interband dipole moment while scattering processes with phonons and impurities play a minor role. The nonlinear response at field amplitudes above 1 kV cm-1 is in the carrier-wave Rabi flopping regime with a pronounced coupling of the graphene layers via the radiation field. Theoretical calculations account for the experimental results.

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Ultrafast two-dimensional terahertz spectroscopy of elementary excitations in solids

2013, Woerner, M., Kuehn, W., Bowlan, P., Reimann, K., Elsaesser, T.

Recent experimental progress has allowed for the implementation of nonlinear two-dimensional (2D) terahertz (THz) spectroscopy in the ultrafast time domain. We discuss the principles of this technique based on multiple phase-locked electric field transients interacting in a collinear geometry with a solid and the phase-resolved detection of the THz fields after interaction with the sample. To illustrate the potential of this new method, 2D correlation spectra of coupled intersubband-longitudinal optical phonon excitations in a double quantum well system and a study of ultrafast carrier dynamics in graphene are presented.

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Ultrafast two-dimensional THz spectroscopy of graphene

2013, Bowlan, P., Martinez Moreno, E., Reimann, K., Woerner, M., Elsaesser, T.

With two-dimensional THz spectroscopy the dynamics of low-energy carriers in graphene is determined. Both intra- and interband absorption contribute to the observed ultrafast pump-probe signals.

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Ultrafast inter-ionic charge transfer of transition-metal complexes mapped by femtosecond x-ray powder diffraction

2013, Zamponi, F., Freyer, B., Juvé, V., Stingl, J., Woerner, M., Chergui, M., Elsaesser, T.

Transient electron density maps are derived from x-ray diffraction patterns of photoexcited [Fe(bpy)3]2+(PF6 -)2 powder. Upon photoexcitation, the 5T 2 quintet state reveals a charge transfer from the PF 6- ions and from the Fe atoms to neighboring bpy units. The charge transfer from the Fe points to a partial and weak charge-transfer character of this state.

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Ultrafast charge relocation in an ionic crystal probed by femtosecond x-ray powder diffraction

2013, Woerner, M., Zamponi, F., Rothhardt, P., Stingl, J., Elsaesser, T.

Transient electron density maps of potassium dihydrogen phosphate(KH 2PO4, KDP) are derived from femtosecond x-ray powder diffraction patterns. Upon photoexcitation, the low-frequency TO soft mode is elongated impulsively and modulates the electronic charge distribution on the length scale of interatomic distances, much larger than the vibrational amplitude of the nuclear motion. The results demonstrate a charge transfer from the volumes around the P-atoms to those containing the O - H·· ·O units and a quadrupolar distortion of the K+ charge distribution. This behavior reflects the interplay of nuclear motions and electric polarizations in the ionic crystal lattice.