Two-color synchrotron X-ray spectroscopy based on transverse resonance island buckets.

We report on a novel multi-color method of X-ray spectroscopy at a Synchrotron radiation source that uses two simultaneously filled electron orbits in an electron storage ring to generate multiple soft or tender X-ray beams of different wavelength. To establish the second orbit, we use nonlinear beam dynamics in the so called TRIBs-transverse resonance island buckets-mode of the BESSY II storage ring, where a second electron orbit winds around the regular one leading to transversely separated source points. X-ray beams of multiple colors are generated by imaging the individual source points via different pathways through a monochromator. The particular colors can be varied by changing the traversal electron beam positions through storage-ring parameters and/or via the monochromator dispersion. As a proof of principle, X-ray absorption spectroscopy is performed on thin Fe films in transmission as well as a scanning transmission measurement on a Fe3GeTe2 sample of inhomogeneous thickness normalizing resonant signals with the pre-edge intensity. Using the extraordinary pointing fidelity of successive X-ray macro-pulses arriving at MHz repetition rates, a detection of tiny contrasts in diluted systems, contrast enhancement in X-ray microscopy as well as fast dynamics studies come into reach.

Field-induced single-ion magnet based on a quasi-octahedral Co(II) complex with mixed sulfur-oxygen coordination environment.

Synthesis and characterization of structure and magnetic properties of the quasi-octahedral complex (pipH2)[Co(TDA)2] 2H2O (I), (pipH22+ = piperazine dication, TDA2- = thiodiacetic anion) are described. X-ray diffraction studies reveal the first coordination sphere of the Co(II) ion, consisting of two chelating tridentate TDA ligands with a mixed sulfur-oxygen strongly elongated octahedral coordination environment. SQUID magnetometry, frequency-domain Fourier-transform (FD-FT) THz-EPR spectroscopy, and high-level ab initio SA-CASSCF/NEVPT2 quantum chemical calculations reveal a strong "easy-plane" type magnetic anisotropy (D ≈ +54 cm-1) of complex I. The complex shows field-induced slow relaxation of magnetization at an applied DC field of 1000 Oe.

Phonon anharmonicities and ultrafast dynamics in epitaxial Sb2Te3.

In this study we report on the investigation of epitaxially grown Sb2Te3 by employing Fourier-Transform transmission Spectroscopy (FTS) with laser-induced Coherent Synchrotron Radiation (CSR) in the Terahertz (THz) spectral range. Static spectra in the range between 20 and 120 cm-1 highlight a peculiar softening of an in-plane IR-active phonon mode upon temperature decrease, as opposed to all Raman active modes which instead show a hardening upon temperature decrease in the same energy range. The phonon mode softening is found to be accompanied by an increase of free carrier concentration. A strong coupling of the two systems (free carriers and phonons) is observed and further evidenced by exciting the same phonon mode at 62 cm-1 within an ultrafast pump-probe scheme employing a femtosecond laser as pump and a CSR single cycle THz pulse as probe. Separation of the free carrier contribution and the phonon resonance in the investigated THz range reveals that, both damping of the phonon mode and relaxation of hot carriers in the time domain happen on the same time scale of 5 ps. This relaxation is about a factor of 10 slower than expected from the Lorentz time-bandwidth limit. The results are discussed in the framework of phonon scattering at thermal and laser induced transient free carriers.

Laser-pump/X-ray-probe experiments with electrons ejected from a Cu(111) target: space-charge acceleration.

A comprehensive investigation of the emission characteristics for electrons induced by X-rays of a few hundred eV at grazing-incidence angles on an atomically clean Cu(111) sample during laser excitation is presented. Electron energy spectra due to intense infrared laser irradiation are investigated at the BESSY II slicing facility. Furthermore, the influence of the corresponding high degree of target excitation (high peak current of photoemission) on the properties of Auger and photoelectrons liberated by a probe X-ray beam is investigated in time-resolved pump and probe measurements. Strong electron energy shifts have been found and assigned to space-charge acceleration. The variation of the shift with laser power and electron energy is investigated and discussed on the basis of experimental as well as new theoretical results.

Far-Infrared and Raman Spectroscopy Investigation of Phonon Modes in Amorphous and Crystalline Epitaxial GeTe-Sb2Te3 Alloys.

A combination of far-infrared and Raman spectroscopy is employed to investigate vibrational modes and the carrier behavior in amorphous and crystalline ordered GeTe-Sb2Te3 alloys (GST) epitaxially grown on Si(111). The infrared active GST mode is not observed in the Raman spectra and vice versa, indication of the fact that inversion symmetry is preserved in the metastable cubic phase in accordance with the Fm3 space group. For the trigonal phase, instead, a partial symmetry break due to Ge/Sb mixed anion layers is observed. By studying the crystallization process upon annealing with both the techniques, we identify temperature regions corresponding to the occurrence of different phases as well as the transition from one phase to the next. Activation energies of 0.43 eV and 0.08 eV for the electron conduction are obtained for both cubic and trigonal phases, respectively. In addition a metal-insulator transition is clearly identified to occur at the onset of the transition between the disordered and the ordered cubic phase.

Single bunch X-ray pulses on demand from a multi-bunch synchrotron radiation source.

Synchrotron radiation facilities routinely operate in a multi-bunch regime, but applications relying on time-of-flight schemes require single bunch operation. Here we show that pulse picking by resonant excitation in a storage ring creates in addition to the multi-bunch operation a distinct and separable single bunch soft X-ray source. It has variable polarization, a photon flux of up to 10(7)-10(9) ph s(-1)/0.1%BW at purity values of 10(4)-10(2) and a repetition rate of 1.25 MHz. The quasi-resonant excitation of incoherent betatron oscillations of electrons allows horizontal pulse separation at variable (also circular) polarization accessible for both, regular 30 ps pulses and ultrashort pulses of 2-3 ps duration. Combined with a new generation of angularly resolving electron spectrometers this creates unique opportunities for time-resolved photoemission studies as confirmed by time-of-flight spectra. Our pulse picking scheme is particularly suited for surface physics at diffraction-limited light sources promising ultimate spectral resolution.

First observation of photons carrying orbital angular momentum in undulator radiation.

Photon beams of 99 eV energy carrying orbital angular momentum (OAM) have been observed in the 2nd harmonic off-axis radiation of a helical undulator at the 3rd generation synchrotron radiation light source BESSY II. For detection, the OAM carrying photon beam was superimposed with a reference beam without OAM. The interference pattern, a spiral intensity distribution, was recorded in a plane perpendicular to the propagation direction. The orientation of the observed spiral structure is related to the helicity of the undulator radiation. Excellent agreement between measurements and simulations has been found.

Ultrafast spin transport as key to femtosecond demagnetization.

Irradiating a ferromagnet with a femtosecond laser pulse is known to induce an ultrafast demagnetization within a few hundred femtoseconds. Here we demonstrate that direct laser irradiation is in fact not essential for ultrafast demagnetization, and that electron cascades caused by hot electron currents accomplish it very efficiently. We optically excite a Au/Ni layered structure in which the 30 nm Au capping layer absorbs the incident laser pump pulse and subsequently use the X-ray magnetic circular dichroism technique to probe the femtosecond demagnetization of the adjacent 15 nm Ni layer. A demagnetization effect corresponding to the scenario in which the laser directly excites the Ni film is observed, but with a slight temporal delay. We explain this unexpected observation by means of the demagnetizing effect of a superdiffusive current of non-equilibrium, non-spin-polarized electrons generated in the Au layer.

Femtosecond modification of electron localization and transfer of angular momentum in nickel.

The rapidly increasing information density required of modern magnetic data storage devices raises the question of the fundamental limits in bit size and writing speed. At present, the magnetization reversal of a bit can occur as quickly as 200 ps (ref. 1). A fundamental limit has been explored by using intense magnetic-field pulses of 2 ps duration leading to a non-deterministic magnetization reversal. For this process, dissipation of spin angular momentum to other degrees of freedom on an ultrafast timescale is crucial. An even faster regime down to 100 fs or below might be reached by non-thermal control of magnetization with femtosecond laser radiation. Here, we show that an efficient novel channel for angular momentum dissipation to the lattice can be opened by femtosecond laser excitation of a ferromagnet. For the first time, the quenching of spin angular momentum and its transfer to the lattice with a time constant of 120+/-70 fs is determined unambiguously with X-ray magnetic circular dichroism. We report the first femtosecond time-resolved X-ray absorption spectroscopy data over an entire absorption edge, which are consistent with an unexpected increase in valence-electron localization during the first 120+/-50 fs, possibly providing the driving force behind femtosecond spin-lattice relaxation.

Femtosecond undulator radiation from sliced electron bunches.

At the 1.7-GeV electron storage ring BESSY II, a first source of synchrotron radiation with 100 fs pulse duration, variable (linear and circular) polarization, tunable photon energy (300 to 1400 eV), and excellent signal-to-background ratio was constructed and is now in routine operation.

Femtosecond terahertz radiation from femtoslicing at BESSY.

Femtosecond far-infrared radiation pulses in the THz spectral range were observed as a consequence of the energy modulation of 1.7 GeV electrons by femtosecond laser pulses in the BESSY storage ring in order to generate femtosecond x-ray pulses ("femtoslicing"). In addition to being crucial for diagnostics of the laser-electron interaction, the THz radiation itself is useful for experiments where intense ultrashort THz pulses of well-defined temporal and spectral characteristics are required.

A model describing stable coherent synchrotron radiation in storage rings.

We present a model describing high power stable broadband coherent synchrotron radiation (CSR) in the terahertz frequency region in an electron storage ring. The model includes distortion of bunch shape from the synchrotron radiation (SR), which enhances higher frequency coherent emission, and limits to stable emission due to an instability excited by the SR wakefield. It gives a quantitative explanation of several features of the recent observations of CSR at the BESSY II storage ring. We also use this model to optimize the performance of a source for stable CSR emission.

Brilliant, coherent far-infrared (THz) synchrotron radiation.

A new technology for generating steady state, brilliant, broadband, coherent, far-infrared (FIR) radiation in electron storage rings is presented, suitable for FIR spectroscopy. An FIR power increase of up to 100 000 compared to the normal, incoherent synchrotron radiation in the range of approximately 5 to approximately 40 cm(-1) could be achieved. The source is up to 1000 times more brillant compared to a standard Hg arc lamp. The coherent synchrotron radiation is produced in a "low alpha" optics mode of the synchrotron light source BESSY, by bunch shortening and non-Gaussian bunch deformation.

Steady-state far-infrared coherent synchrotron radiation detected at BESSY II.

At BESSY II it is demonstrated that far-infrared coherent synchrotron radiation (CSR) can be generated by a controlled, steady-state process at storage rings. As an indication for coherent emission, the radiated power grows with the square of the beam current. The spectrum was analyzed by an interferometer in the 1-mm to 0.3-mm wavelength range. The CSR was enhanced more than 3000 times above background; the incoherent radiation remained below the background level. Steady-state and bursting CSR were discriminated by time resolved analysis from micro seconds to seconds.

Diagnostic front end for BESSY II.

For BESSY II, synchrotron radiation beam diagnostics will be incorporated in both the insertion-device front ends and the dipole-beamline front ends. In order to gain a complete picture of the source characteristics, a diagnostic front end has been designed and tested for dipole radiation. This consists of (i) a pinhole array imaging system, (ii) a double-blade system for the determination of the vertical center of gravity of the synchrotron radiation fan, and (iii) a Bragg-Fresnel multilayer system for the most precise image information about the source size and shape.

[The atrial sound over the carotid artery]. / Der Vorhofton über der Arteria carotis.

The appearance of carotid atrial sounds has been observed in 6 out of 19 patients with stroke. It is assumed that these patients have obstructions in the carotid-subclavian area. Further studies to prove this working hypothesis are in progress.