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.
Single-shot time-of-flight spectra for Coulomb explosion of N2 and I2 molecules have been recorded at the Free Electron LASer in Hamburg (FLASH) and have been analysed using a partial covariance ...mapping technique. The partial covariance analysis unravels a detailed picture of all significant Coulomb explosion pathways, extending up to the N4+-N5+ channel for nitrogen and up to the I8+-I9+ channel for iodine. The observation of the latter channel is unexpected if only sequential ionization processes from the ground state ions are considered. The maximum kinetic energy release extracted from the covariance maps for each dissociation channel shows that Coulomb explosion of nitrogen molecules proceeds much faster than that of the iodine. The N2 ionization dynamics is modelled using classical trajectory simulations in good agreement with the outcome of the experiments. The results suggest that covariance mapping of the Coulomb explosion can be used to measure the intensity and pulse duration of free-electron lasers.
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.
High-frequency modulations appearing in the kinetic energy distribution of laser-accelerated ions are proposed for retrieving the acceleration field dynamics at the femtosecond timescale. Such an ...approach becomes possible if the laser-cycling field modulates the particle density in the ion spectra and produces quasitime stamps for analysis. We investigate target and laser parameters determining this effect and discuss the dependencies of the observed modulation. Our findings refine a basic mechanism, the target normal sheath acceleration, where an intense and ultrafast laser pulse produces a very strong electrical field at a plasma-vacuum interface. The field decays rapidly due to energy dissipation and forms a characteristic spectrum of fast ions streaming away from the interface. We show that the derived decay function of the field is in accordance with model predictions of the accelerating field structure. Our findings are supported by two-dimensional particle-in-cell simulations. The knowledge of the femtosecond field dynamics helps to rerate optimization strategies for laser ion acceleration.
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.
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.
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.
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