Klaus Sokolowski-Tinten

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 melting and ablation of semiconductors studied with time of flight mass spectroscopy

Using time-of-flight mass spectroscopy, we have investigated melting and ablation of gallium arsenide and silicon irradiated by femtosecond pulses. Below the ablation threshold the maximum surface temperature is obtained from the collisionless time-of-flight distributions of evaporated or sublimated particles. At the melting threshold, we estimate a temperature for the silicon surface which is approximately 500 K higher than the equilibrium melting temperature. In the fluence regime where melting is known to be a nonthermal process, we measure maximum surface temperatures in excess of 2500 K for both silicon and gallium arsenide, indicating rapid thermalization after nonthermal melting. At the ablation threshold, we estimated for both materials surface temperatures between 3000 and 4000 K. We observed a clear threshold-like effect in the number of detected particles, indicating the occurrence of a bulk effect. The flow parameters above the ablation threshold are discussed and compared to the different mod...

Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.

Characteristics of focused soft X-ray free-electron laser beam determined by ablation of organic molecular solids

A linear accelerator based source of coherent radiation, FLASH (Free-electron LASer in Hamburg) provides ultra-intense femtosecond radiation pulses at wavelengths from the extreme ultraviolet (XUV; lambda<100nm) to the soft X-ray (SXR; lambda<30nm) spectral regions. 25-fs pulses of 32-nm FLASH radiation were used to determine the ablation parameters of PMMA - poly (methyl methacrylate). Under these irradiation conditions the attenuation length and ablation threshold were found to be (56.9+/-7.5) nm and approximately 2 mJ*cm(-2), respectively. For a second wavelength of 21.7 nm, the PMMA ablation was utilized to image the transverse intensity distribution within the focused beam at mum resolution by a method developed here.

Damage threshold of inorganic solids under free-electron-laser irradiation at 32.5 nm wavelength

We exposed samples of B4C, amorphous C, chemical-vapor-deposition (CVD)-diamond C, Si, and SiC to single 25 fs-long pulses of 32.5 nm free-electron-laser radiation at fluences of up to 2.2 J/cm{sup 2}. The samples were chosen as candidate materials for x-ray free electron laser (XFEL) optics. We found that the threshold for surface-damage is on the order of the fluence required for thermal melting. For larger fluences, the crater depths correspond to temperatures on the order of the critical temperature, suggesting that the craters are formed by two-phase vaporization [1]. XFELs have the promise of producing extremely high-intensity ultrashort pulses of coherent, monochromatic radiation in the 1 to 10 keV regime. The expected high output fluence and short pulse duration pose significant challenges to the optical components, including radiation damage. It has not been possible to obtain direct experimental verification of the expected damage thresholds since appropriate x-ray sources are not yet available. FLASH has allowed us to study the interaction of high-fluence short-duration photon pulses with materials at the shortest wavelength possible to date. With these experiments, we have come closer to the extreme conditions expected in XFEL-matter interaction scenarios than previously possible.

Ultrafast imaging interferometry at femtosecond- laser-excited surfaces

�2 rad and amplitude changes 1% with micrometer spatial resolution 1 m. Interferograms are processed using a 2D-Fourier transform algorithm. We discuss the image formation and the physical interpretation of the measured interferograms. The technique is applied to measure transient changes of a GaAs surface irradiated with intense femtosecond laser pulses with fluences near the ablation threshold.

Single-shot pulse duration monitor for extreme ultraviolet and X-ray free-electron lasers

The resolution of ultrafast studies performed at extreme ultraviolet and X-ray free-electron lasers is still limited by shot-to-shot variations of the temporal pulse characteristics. Here we show a versatile single-shot temporal diagnostic tool that allows the determination of the extreme ultraviolet pulse duration and the relative arrival time with respect to an external pump-probe laser pulse. This method is based on time-resolved optical probing of the transient reflectivity change due to linear absorption of the extreme ultraviolet pulse within a solid material. In this work, we present measurements performed at the FLASH free-electron laser. We determine the pulse duration at two distinct wavelengths, yielding (184±14) fs at 41.5 nm and (21±19) fs at 5.5 nm. Furthermore, we demonstrate the feasibility to operate the tool as an online diagnostic by using a 20-nm-thin Si3N4 membrane as target. Our results are supported by detailed numerical and analytical investigations.

Picosecond acoustic response of a laser-heated gold-film studied with time-resolved x-ray diffraction

We apply time-resolved x-ray diffraction using ultrashort x-ray pulses from a laser-produced plasma to probe the picosecond acoustic response of a thin laser-heated gold film. Measurements of the temporal changes in the angular distribution of diffracted x-rays provide direct quantitative information on the transient evolution of lattice strain. This allows to disentangle electronic and thermal pressure contributions driving lattice expansion after impulsive laser excitation. The electron-lattice energy equilibration time τE=(5±0.3) ps as well as the electronic Gruneisen parameter γe=(1.48±0.3) have been determined.

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained. (Less)

Visualization of nanocrystal breathing modes at extreme strains.

Nanoscale dimensions in materials lead to unique electronic and structural properties with applications ranging from site-specific drug delivery to anodes for lithium-ion batteries. These functional properties often involve large-amplitude strains and structural modifications, and thus require an understanding of the dynamics of these processes. Here we use femtosecond X-ray scattering techniques to visualize, in real time and with atomic-scale resolution, light-induced anisotropic strains in nanocrystal spheres and rods. Strains at the percent level are observed in CdS and CdSe samples, associated with a rapid expansion followed by contraction along the nanosphere or nanorod radial direction driven by a transient carrier-induced stress. These morphological changes occur simultaneously with the first steps in the melting transition on hundreds of femtosecond timescales. This work represents the first direct real-time probe of the dynamics of these large-amplitude strains and shape changes in few-nanometre-scale particles.