Ultrafast Formation of a Charge Density Wave State in 1T-TaS_{2}: Observation at Nanometer Scales Using Time-Resolved X-Ray Diffraction.

Femtosecond time-resolved x-ray diffraction is used to study a photoinduced phase transition between two charge density wave (CDW) states in 1T-TaS_{2}, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photoinduced I-CDW phase then develops through a nucleation and growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a nonconservative order parameter.

Femtosecond X-ray absorption study of electron localization in photoexcited anatase TiO2.

Transition metal oxides are among the most promising solar materials, whose properties rely on the generation, transport and trapping of charge carriers (electrons and holes). Identifying the latter's dynamics at room temperature requires tools that combine elemental and structural sensitivity, with the atomic scale resolution of time (femtoseconds, fs). Here, we use fs Ti K-edge X-ray absorption spectroscopy (XAS) upon 3.49 eV (355 nm) excitation of aqueous colloidal anatase titanium dioxide nanoparticles to probe the trapping dynamics of photogenerated electrons. We find that their localization at Titanium atoms occurs in <300 fs, forming Ti(3+) centres, in or near the unit cell where the electron is created. We conclude that electron localization is due to its trapping at pentacoordinated sites, mostly present in the surface shell region. The present demonstration of fs hard X-ray absorption capabilities opens the way to a detailed description of the charge carrier dynamics in transition metal oxides.

Coherent structural dynamics of a prototypical charge-density-wave-to-metal transition.

Using femtosecond time-resolved x-ray diffraction, we directly monitor the coherent lattice dynamics through an ultrafast charge-density-wave-to-metal transition in the prototypical Peierls system K(0.3)MoO(3) over a wide range of relevant excitation fluences. While in the low fluence regime we directly follow the structural dynamics associated with the collective amplitude mode; for fluences above the melting threshold of the electronic density modulation we observe a transient recovery of the periodic lattice distortion. We can describe these structural dynamics as a motion along the coordinate of the Peierls distortion triggered by the prompt collapse of electronic order after photoexcitation. The results indicate that the dynamics of a structural symmetry-breaking transition are determined by a high-symmetry excited state potential energy surface distinct from that of the initial low-temperature state.

Directional bremsstrahlung from a Ti laser-produced x-ray source at relativistic intensities in the 3-12 keV range.

Front and rear side x-ray emission from thin titanium foils irradiated by ultraintense laser pulses at intensities up to ≈5 × 10(19) W/cm2 was measured using a high-resolution imaging system. Significant differences in intensity, dimension, and spectrum between front and rear side emission intensity in the 3-12 keV photon energy range was found even for 5 µm thin Ti foils. Simulations and analysis of space-resolved spectra explain this behavior in terms of directional bremsstrahlung emission from fast electrons generated during the interaction process.

Novel x-ray multispectral imaging of ultraintense laser plasmas by a single-photon charge coupled device based pinhole camera.

Spectrally resolved two-dimensional imaging of ultrashort laser-produced plasmas is described, obtained by means of an advanced technique. The technique has been tested with microplasmas produced by ultrashort relativistic laser pulses. The technique is based on the use of a pinhole camera equipped with a charge coupled device detector operating in the single-photon regime. The spectral resolution is about 150 eV in the 4-10 keV range, and images in any selected photon energy range have a spatial resolution of 5 microm. The potential of the technique to study fast electron propagation in ultraintense laser interaction with multilayer targets is discussed and some preliminary results are shown.

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.

Spatial characteristics of Kalpha x-ray emission from relativistic femtosecond laser plasmas.

The spatial structure of the Kalpha emission from Ti targets irradiated with a high intensity femtosecond laser has been studied using a two-dimensional monochromatic imaging technique. For laser intensities I<5 x 10(17) W/cm(2), the observed spatial structure of the Kalpha emission can be explained by the scattering of the hot electrons inside the solid with the help of a hybrid particle-in-cell/Monte Carlo model. By contrast, at the maximum laser intensity I=7 x 10(18) W/cm(2) the half-width of the Kalpha emission was 70 microm compared to a laser-focus half-width of 3 microm. Moreover, the main Kalpha peak was surrounded by a halo of weak Kalpha emission with a diameter of 400 microm and the Kalpha intensity at the source center did not increase with increasing laser intensity. These three features point to the existence of strong self-induced fields, which redirect the hot electrons over the target surface.