I. Uschmann

Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit

The study of phase-transition dynamics in solids beyond a time-averaged kinetic description requires direct measurement of the changes in the atomic configuration along the physical pathways leading to the new phase. The timescale of interest is in the range 10-14 to 10-12 s. Until recently, only optical techniques were capable of providing adequate time resolution, albeit with indirect sensitivity to structural arrangement. Ultrafast laser-induced changes of long-range order have recently been directly established for some materials using time-resolved X-ray diffraction. However, the measurement of the atomic displacements within the unit cell, as well as their relationship with the stability limit of a structural phase, has to date remained obscure. Here we report time-resolved X-ray diffraction measurements of the coherent atomic displacement of the lattice atoms in photoexcited bismuth close to a phase transition. Excitation of large-amplitude coherent optical phonons gives rise to a periodic modulation of the X-ray diffraction efficiency. Stronger excitation corresponding to atomic displacements exceeding 10 per cent of the nearest-neighbour distance—near the Lindemann limit—leads to a subsequent loss of long-range order, which is most probably due to melting of the material.

Femtosecond time-resolved X-ray diffraction from laser-heated organic films

The extension of time-resolved X-ray diffraction to the subpicosecond domain is an important challenge, as the nature of chemical reactions and phase transitions is determined by atomic motions on these timescales. An ultimate goal is to study the structure of transient states with a time resolution shorter than the typical period of vibration along a reaction coordinate (around 100 fs). Biological processes that can be initiated optically have been studied extensively by ultrafast infrared, visible and ultraviolet spectroscopy. But these techniques probe only electronic states, whereas time-resolved crystallography should be able to directly monitor atomic positions. Here we show that changes in the X-ray diffraction pattern from an organic film heated by a laser pulse can be monitored on a timescale of less than a picosecond. We have studied the response of a Langmuir–Blodgett multilayer film of cadmium arachidate to laser heating by observing changes in the intensity of one Bragg peak for different delays between the perturbing optical pulse and the X-ray probe pulse. A strong decrease in intensity is seen within a picosecond of heating, resulting from disorder introduced to the layers of cadmium atoms before thermal expansion of the film (which ultimately leads to its destruction) has time to occur.

Monochromatic focusing of subpicosecond x-ray pulses in the keV range

An effective x-ray optical method to focus keV x-ray pulses shorter than one picosecond by using spherically or toroidally bent crystals is presented. The spectral, spatial, and time-dependent properties of focusing by two-dimensional bent crystals are calculated by considering geometrical effects, physical limitation in high performance crystal optics, and reflectivities obtained by x-ray diffraction theory. These properties are compared with first experimental results of focusing x rays from a plasma created by a laser pulse with 4.5 mJ energy and 100 fs pulse length. The x-ray signals, simultaneously obtained from a von Hamos spectrometer and two-dimensional bent crystals are compared and found in good agreement with theoretical data. The possibilities and aspects of laser pump x-ray probe experiments using this type of x-ray optics system and currently available laser systems are discussed.

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.

X-ray microscopy of laser-produced plasmas with the use of bent crystals

X-ray spectroscopical and microscopical methods are used for the determination of the spectral and spatial distribution of X-ray intensity of laser-produced plasmas. The use of Bragg reflections of two-dimensionally bent crystals enables the X-ray microscopical imaging in narrow spectral ranges (Δλ/λ=10 −4 to 10 −2 ) with wavelengths 0.1 nm

Novel method for characterizing relativistic electron beams in a harsh laser-plasma environment.

Particle pulses generated by laser-plasma interaction are characterized by ultrashort duration, high particle density, and sometimes a very strong accompanying electromagnetic pulse (EMP). Therefore, beam diagnostics different from those known from classical particle accelerators such as synchrotrons or linacs are required. Easy to use single-shot techniques are favored, which must be insensitive towards the EMP and associated stray light of all frequencies, taking into account the comparably low repetition rates and which, at the same time, allow for usage in very space-limited environments. Various measurement techniques are discussed here, and a space-saving method to determine several important properties of laser-generated electron bunches simultaneously is presented. The method is based on experimental results of electron-sensitive imaging plate stacks and combines these with Monte Carlo-type ray-tracing calculations, yielding a comprehensive picture of the properties of particle beams. The total charge, the energy spectrum, and the divergence can be derived simultaneously for a single bunch.

X-ray reflection properties of elastically bent perfect crystals in Bragg geometry

Reflection curves of bent crystals were calculated using the Takagi–Taupin theory of dependence on bending radius, wavelength, crystal thickness and Bragg angle. The reflection properties of bent crystals were measured for bending radii down to 90 mm. Usually, for the measurement of rocking curves of crystals with large bending radii, the double-crystal diffractometer was used in parallel position (n, −n). A special achromatic diffractometer consisting of a plane and a bent crystal is proposed. It is used to measure rocking curves of bent crystals with small bending radii (R < 1 m). Experimental values show close agreement with the theory. The reflection properties are important for X-ray microscopy with two-dimensionally bent crystals and for X-ray spectroscopy with bent crystals.

Analyzer-based phase contrast imaging and phase retrieval using a rotating anode x-ray source

We have performed an analyzer crystal based phase contrast imaging (ABI) experiment using a rotating anode x-ray source. The use of such an incoherent source demonstrates the potential of ABI as a quantitative characterization tool for the laboratory environment. A phase contrast image of a plastic phantom was recorded on high resolution x-ray film and the projected thickness was retrieved from a single image. The projected thickness recovered from the phase contrast image was shown to quantitatively agree with a reference optical microscope measurement.

Vacuum-assisted generation and control of atomic coherences at x-ray energies.

The control of light-matter interaction at the quantum level usually requires coherent laser fields. But already an exchange of virtual photons with the electromagnetic vacuum field alone can lead to quantum coherences, which subsequently suppress spontaneous emission. We demonstrate such spontaneously generated coherences (SGC) in a large ensemble of nuclei operating in the x-ray regime, resonantly coupled to a common cavity environment. The observed SGC originates from two fundamentally different mechanisms related to cooperative emission and magnetically controlled anisotropy of the cavity vacuum. This approach opens new perspectives for quantum control, quantum state engineering and simulation of quantum many-body physics in an essentially decoherence-free setting.

Kinetic to thermal energy transfer and interpenetration in the collision of laser-produced plasmas

An experimental and numerical analysis of the collision of two plasmas produced from laser-exploded Al/Al and Al/Mg pairs of foils is presented. Various imaging and spectroscopic x-ray techniques have been used to diagnose the collision over a broad range of intertarget distances and laser intensities. Ion temperatures in the 10 keV range have been measured from Doppler broadening. Electron temperatures and densities have been deduced from line ratios and interpenetration distances have been determined by the spatial extent of Mg and Al x-ray lines. Eulerian multifluid simulations have been developed and coupled to atomic physics postprocessing. The comparison of the measurements with these simulations shows that interpenetration prevails at large intertarget distances and high laser intensities; kinetic to thermal energy transfer then takes place on a ∼200-μm wide region and during ∼150 ps.