Optical control of 4f orbital state in rare-earth metals.

A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved x-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4f-electronic excitations out of the ground-state multiplet occur after optical pumping. These excitations are driven by inelastic 5d-4f-electron scattering, altering the 4f-orbital state and consequently the MCA with important implications for magnetization dynamics in 4f-metals and more general for the excitation of localized electronic states in correlated materials.

Using the photoinduced L 3 resonance shift in Fe and Ni as time reference for ultrafast experiments at low flux soft x-ray sources.

We study the optical-pump induced ultrafast transient change of x-ray absorption at L 3 absorption resonances of the transition metals Ni and Fe in the Fe0.5Ni0.5 alloy. We find the effect for both elements to occur simultaneously on a femtosecond timescale. This effect may hence be used as a handy cross correlation scheme, providing a time-zero reference for ultrafast optical-pump soft x-ray-probe measurement. The method benefits from a relatively simple experimental setup as the sample itself acts as time-reference tool. In particular, this technique works with low flux ultrafast soft x-ray sources. The measurements are compared to the cross correlation method introduced in an earlier publication.

Ultrafast and Energy-Efficient Quenching of Spin Order: Antiferromagnetism Beats Ferromagnetism.

By comparing femtosecond laser pulse induced ferro- and antiferromagnetic dynamics in one and the same material-metallic dysprosium-we show both to behave fundamentally different. Antiferromagnetic order is considerably faster and much more efficiently reduced by optical excitation than its ferromagnetic counterpart. We assign the fast and extremely efficient process in the antiferromagnet to an interatomic transfer of angular momentum within the spin system. Our findings imply that this angular momentum transfer channel is effective in other magnetic metals with nonparallel spin alignment. They also point out a possible route towards energy-efficient spin manipulation for magnetic devices.

Influence of the pump pulse wavelength on the ultrafast demagnetization of Gd(0 0 0 1) thin films.

We studied the magnetization dynamics of gadolinium metal after femtosecond laser excitation recording the x-ray magnetic circular dichroism in reflection (XMCD-R) at the Gd M 5 absorption edge. Varying the photon energy of the pump pulse allows us to change the initial energy distribution of photoexcited carriers. The overall similar response for excitation with 0.95, 1.55 and 3.10 eV photons at comparable pump fluences indicates that ultrafast ballistic carrier transport leads to a homogeneous energy distribution on the femtosecond timescale in the probed sample volume. Differences are observed in the initial ultrafast demagnetization magnitude. They are attributed to an enhanced spin-flip probability at higher electron energies characterizing the non-thermal electron distribution.

Versatile soft X-ray-optical cross-correlator for ultrafast applications.

We present an X-ray-optical cross-correlator for the soft ([Formula: see text]) up to the hard X-ray regime based on a molybdenum-silicon superlattice. The cross-correlation is done by probing intensity and position changes of superlattice Bragg peaks caused by photoexcitation of coherent phonons. This approach is applicable for a wide range of X-ray photon energies as well as for a broad range of excitation wavelengths and requires no external fields or changes of temperature. Moreover, the cross-correlator can be employed on a 10 ps or 100 fs time scale featuring up to 50% total X-ray reflectivity and transient signal changes of more than 20%.

Analysis of the halo background in femtosecond slicing experiments.

The slicing facility FemtoSpeX at BESSY II offers unique opportunities to study photo-induced dynamics on femtosecond time scales by means of X-ray magnetic circular dichroism, resonant and non-resonant X-ray diffraction, and X-ray absorption spectroscopy experiments in the soft X-ray regime. Besides femtosecond X-ray pulses, slicing sources inherently also produce a so-called `halo' background with a different time structure, polarization and pointing. Here a detailed experimental characterization of the halo radiation is presented, and a method is demonstrated for its correct and unambiguous removal from femtosecond time-resolved data using a special laser triggering scheme as well as analytical models. Examples are given for time-resolved measurements with corresponding halo correction, and errors of the relevant physical quantities caused by either neglecting or by applying a simplified model to describe this background are estimated.

FemtoSpeX: a versatile optical pump-soft X-ray probe facility with 100†fs X-ray pulses of variable polarization.

Here the major upgrades of the femtoslicing facility at BESSY II (Khan et al., 2006) are reviewed, giving a tutorial on how elliptical-polarized ultrashort soft X-ray pulses from electron storage rings are generated at high repetition rates. Employing a 6 kHz femtosecond-laser system consisting of two amplifiers that are seeded by one Ti:Sa oscillator, the total average flux of photons of 100 fs duration (FWHM) has been increased by a factor of 120 to up to 10(6) photons s(-1) (0.1% bandwidth)(-1) on the sample in the range from 250 to 1400 eV. Thanks to a new beamline design, a factor of 20 enhanced flux and improvements of the stability together with the top-up mode of the accelerator have been achieved. The previously unavoidable problem of increased picosecond-background at higher repetition rates, caused by `halo' photons, has also been solved by hopping between different `camshaft' bunches in a dedicated fill pattern (`3+1 camshaft fill') of the storage ring. In addition to an increased X-ray performance at variable (linear and elliptical) polarization, the sample excitation in pump-probe experiments has been considerably extended using an optical parametric amplifier that supports the range from the near-UV to the far-IR regime. Dedicated endstations covering ultrafast magnetism experiments based on time-resolved X-ray circular dichroism have been either upgraded or, in the case of time-resolved resonant soft X-ray diffraction and reflection, newly constructed and adapted to femtoslicing requirements. Experiments at low temperatures down to 6 K and magnetic fields up to 0.5 T are supported. The FemtoSpeX facility is now operated as a 24 h user facility enabling a new class of experiments in ultrafast magnetism and in the field of transient phenomena and phase transitions in solids.

A novel monochromator for experiments with ultrashort X-ray pulses.

Aiming at advancing storage-ring-based ultrafast X-ray science, over the past few years many upgrades have been undertaken to continue improving beamline performance and photon flux at the Femtoslicing facility at BESSY II. In this article the particular design upgrade of one of the key optical components, the zone-plate monochromator (ZPM) beamline, is reported. The beamline is devoted to optical pump/soft X-ray probe applications with 100 fs (FWHM) X-ray pulses in the soft X-ray range at variable polarization. A novel approach consisting of an array of nine off-axis reflection zone plates is used for a gapless coverage of the spectral range between 410 and 1333 eV at a designed resolution of E/ΔE = 500 and a pulse elongation of only 30 fs. With the upgrade of the ZPM the following was achieved: a smaller focus, an improved spectral resolution and bandwidth as well as excellent long-term stability. The beamline will enable a new class of ultrafast applications with variable optical excitation wavelength and variable polarization.

Hot-electron-driven enhancement of spin-lattice coupling in Gd and Tb 4f ferromagnets observed by femtosecond x-ray magnetic circular dichroism.

Femtosecond x-ray magnetic circular dichroism was used to study the time-dependent magnetic moment of 4f electrons in the ferromagnets Gd and Tb, which are known for their different spin-lattice coupling. We observe a two-step demagnetization with an ultrafast demagnetization time of 750 fs identical for both systems and slower times which differ sizeably with 40 ps for Gd and 8 ps for Tb. We conclude that spin-lattice coupling in the electronically excited state is enhanced up to 50 times compared to equilibrium.

Metal-to-ligand and ligand-to-metal charge transfer in thin films of Prussian blue analogues investigated by X-ray absorption spectroscopy.

A series of thin films of Prussian blue analogues is investigated by X-ray absorption spectroscopy (XAS) at the Fe, Co and Mn L(2,3)-edges. The ligand field multiplet theory enables us to examine accurately the electronic structure of these materials. Experimental XAS spectra of CoFe Prussian blue analogues are successfully reproduced using a ground state configuration including metal-to-ligand (MLCT) and ligand-to-metal charge transfer (LMCT) at the Co and Fe L(2,3)-edges. In particular, a huge improvement is achieved for satellite peaks at the Co(iii) L(2,3)-edges compared to previous calculations in the literature based on LMCT effects only. On the other hand, XAS spectra of MnFe analogues synthesized for the first time, can be reproduced conveniently by taking into account either MLCT or LMCT depending on the conditions of the sample preparation. For each thin film, the proportion of the different oxidation states of Co, Fe and Mn is evaluated. Unexpectedly, this analysis reveals the presence of a significant amount of a reduced phase, which turns out to be strongly dependent on the sample synthesis and storage conditions.

Femtosecond microscopy of surface plasmon polariton wave packet evolution at the silver/vacuum interface.

A movie of the dispersive and dissipative propagation of surface plasmon polariton (SPP) wave packets at a silver/vacuum interface is recorded by the interferometric time-resolved photoemission electron microscopy with 60 nm spatial resolution and 330 as frame interval. The evolution of SPP wave packets is imaged through a two-path interference created by a pair of 10 fs phase correlated pump-probe light pulses at 400 nm. The wave packet evolution is simulated using the complex dielectric function of silver.