F. Zamponi

Microfocus Cu K ? source for femtosecond x-ray science

We demonstrate a subpicosecond 1 kHz femtosecond x-ray source with a well-accessible quasi-point size (10??m diameter) providing Cu K? emission with a maximum flux of 6.8×1010? photons?s for continuous operation of 10 h. A new geometry that essentially facilitates the adjustment and diminishes the temporal jitter between the x-ray probe and the laser pump pulse is implemented for time-resolved diffraction experiments.

Ultrafast large-amplitude relocation of electronic charge in ionic crystals

The interplay of vibrational motion and electronic charge relocation in an ionic hydrogen-bonded crystal is mapped by X-ray powder diffraction with a 100 fs time resolution. Photoexcitation of the prototype material KH2PO4 induces coherent low-frequency motions of the PO4 tetrahedra in the electronically excited state of the crystal while the average atomic positions remain unchanged. Time-dependent maps of electron density derived from the diffraction data demonstrate an oscillatory relocation of electronic charge with a spatial amplitude two orders of magnitude larger than the underlying vibrational lattice motions. Coherent longitudinal optical and tranverse optical phonon motions that dephase on a time scale of several picoseconds, drive the charge relocation, similar to a soft (transverse optical) mode driven phase transition between the ferro- and paraelectric phase of KH2PO4.

Persistent nonequilibrium dynamics of the thermal energies in the spin and phonon systems of an antiferromagnet

We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the Néel temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost.

Ultrafast soft-mode driven charge relocation in an ionic crystal.

Transient electron density maps of potassium dihydrogen phosphate (KH(2)PO(4), 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. The results demonstrate a charge transfer from the volumes around the P-atoms and K(+)-ions to those containing the O-HO 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.

Ultrafast x-ray diffraction thermometry measures the influence of spin excitations on the heat transport through nanolayers

We investigate the heat transport through a rare earth multilayer system composed of Yttrium (Y), Dysprosium (Dy) and Niobium (Nb) by ultrafast X-ray diffraction. This is an example of a complex heat flow problem on the nanoscale, where several different quasi-particles carry the heat. The Bragg peak positions of each layer represent layer-specific thermometers that measure the energy flow through the sample after excitation of the Y top-layer with fs-laser pulses. In an experiment-based analytic solution to the nonequilibrium heat transport problem, we derive the individual contributions of the spins and the coupled electron-lattice system to the heat conduction. The full characterization of the spatiotemporal energy flow at different starting temperatures reveals that the spin excitations of antiferromagnetic Dy speed up the heat transport into the Dy layer at low temperatures, whereas the heat transport through this layer and further into the Y and Nb layers underneath is slowed down. The experimental findings are compared to the solution of the heat equation using macroscopic temperature-dependent material parameters without separation of spin- and phonon contributions to the heat. We explain, why the simulated energy density matches our experiment-based derivation of the heat transport, although the simulated thermoelastic strain in this simulation is not even in qualitative agreement.

Characterization of an ultrafast Bragg-Switch for shortening hard x-ray pulses

We present a nanostructured device that functions as photoacoustic hard x-ray switch. The device is triggered by femtosecond laser pulses and allows for temporal gating of hard x-rays on picosecond (ps) timescales. It may be used for pulse picking or even pulse shortening in 3rd generation synchrotron sources. Previous approaches mainly suffered from insufficient switching contrasts due to excitation-induced thermal distortions. We present a new approach where thermal distortions are spatially separated from the functional switching layers in the structure. Our measurements yield a switching contrast of 14, which is sufficient for efficient hard x-ray pulse shortening. The optimized structure also allows for utilizing the switch at high repetition rates of up to 208 kHz.

Simultaneous dynamic characterization of charge and structural motion during ferroelectric switching

Monitoring structural changes in ferroelectric thin films during electric field-induced polarization switching is important for a full microscopic understanding of the coupled motion of charges, atoms and domain walls. We combine standard ferroelectric test-cycles with time-resolved x-ray diffraction to investigate the response of a nanoscale ferroelectric oxide capacitor upon charging, discharging and switching. Piezoelectric strain develops during the electronic RC time constant and additionally during structural domain-wall creep. The complex atomic motion during ferroelectric polarization reversal starts with a negative piezoelectric response to the charge flow triggered by voltage pulses. Incomplete screening limits the compressive strain. The piezoelectric modulation of the unit cell tweaks the energy barrier between the two polarization states. Domain wall motion is evidenced by a broadening of the in-plane components of Bragg reflections. Such simultaneous measurements on a working device elucidate and visualize the complex interplay of charge flow and structural motion and challenges theoretical modelling.

Grueneisen-approach for the experimental determination of transient spin and phonon energies from ultrafast x-ray diffraction data: gadolinium

We study gadolinium thin films as a model system for ferromagnets with negative thermal expansion. Ultrashort laser pulses heat up the electronic subsystem and we follow the transient strain via ultrafast x-ray diffraction. In terms of a simple Grueneisen approach, the strain is decomposed into two contributions proportional to the thermal energy of spin and phonon subsystems. Our analysis reveals that upon femtosecond laser excitation, phonons and spins can be driven out of thermal equilibrium for several nanoseconds.