Ultrafast time-resolved optical spectroscopy has revealed new classes of physical, chemical and biological reactions, in which directed, deterministic motions of atoms have a key role. This contrasts with the random, diffusive motion of atoms across activation barriers that typically determines kinetic rates on slower timescales. An example of these new processes is the ultrafast melting of semiconductors, which is believed to arise from a strong modification of the inter-atomic forces owing to laser-induced promotion of a large fraction (10% or more) of the valence electrons to the conduction band. The atoms immediately begin to move and rapidly gain sufficient kinetic energy to induce melting--much faster than the several picoseconds required to convert the electronic energy into thermal motions. Here we present measurements of the characteristic melting time of InSb with a recently developed technique of ultrafast time-resolved X-ray diffraction that, in contrast to optical spectroscopy, provides a direct probe of the changing atomic structure. The data establish unambiguously a loss of long-range order up to 900 A inside the crystal, with time constants as short as 350 femtoseconds. This ability to obtain the quantitative structural characterization of non-thermal processes should find widespread application in the study of ultrafast dynamics in other physical, chemical and biological systems.

Single-phase vanadium dioxide (VO2) thin films have been grown on Si3N4∕Si substrates by means of a well-controlled magnetron sputtering process. The deposited VO2 films were found to exhibit a semiconductor-to-metal transition (SMT) at ∼69°C with a resistivity change as high as 3.2 decades. A direct and clear-cut correlation is established between the SMT characteristics (both amplitude and abruptness of the transition) of the VO2 films and their crystallite size.

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We report on the first demonstration of femtosecond x-ray absorption spectroscopy, made uniquely possible by the use of broadly tunable bending-magnet radiation from "laser-sliced" electron bunches within a synchrotron storage ring. We measure the femtosecond electronic rearrangements that occur during the photoinduced insulator-metal phase transition in VO2. Symmetry- and element-specific x-ray absorption from V2p and O1s core levels (near 500 eV) separately measures the filling dynamics of differently hybridized V3d-O2p electronic bands near the Fermi level.

We use optical-pump terahertz-probe spectroscopy to investigate the near-threshold behavior of the photoinduced insulator-to-metal (IM) transition in vanadium dioxide thin films. Upon approaching Tc a reduction in the fluence required to drive the IM transition is observed, consistent with a softening of the insulating state due to an increasing metallic volume fraction (below the percolation limit). This phase coexistence facilitates the growth of a homogeneous metallic conducting phase following superheating via photoexcitation. A simple dynamic model using Bruggeman effective medium theory describes the observed initial condition sensitivity.

Terahertz time-domain spectroscopy is used to measure the complex terahertz conductivity of a nanogranular vanadium dioxide (VO2) thin film as a function of temperature through the metal-insulator transition. The Drude–Smith model provides a good fit to the observed terahertz conductivity, revealing a metallic state that forms via switching of individual nanograins and strong carrier confinement within the nanograins due to scattering off grain boundaries. Furthermore, the directly applied Drude–Smith model provides a more accurate description of the measured terahertz conductivity in this material than either Bruggeman or Maxwell–Garnett effective medium theories.

Development of x-ray phase contrast imaging applications with a laboratory scale source have been limited by the long exposure time needed to obtain one image. We demonstrate, using the Betatron x-ray radiation produced when electrons are accelerated and wiggled in the laser-wakefield cavity, that a high quality phase contrast image of a complex object (here, a bee), located in air, can be obtained with a single laser shot. The Betatron x-ray source used in this proof of principle experiment has a source diameter of 1.7 µm and produces a synchrotron spectrum with critical energy Ec = 12.3 ± 2.5 keV and 10 9 photons per shot in the whole spectrum.

We have analyzed the coupling of ultraintense lasers (at ∼2×10{19}  W/cm{2}) with solid foils of limited transverse extent (∼10  s of μm) by monitoring the electrons and ions emitted from the target. We observe that reducing the target surface area allows electrons at the target surface to be reflected from the target edges during or shortly after the laser pulse. This transverse refluxing can maintain a hotter, denser and more homogeneous electron sheath around the target for a longer time. Consequently, when transverse refluxing takes places within the acceleration time of associated ions, we observe increased maximum proton energies (up to threefold), increased laser-to-ion conversion efficiency (up to a factor 30), and reduced divergence which bodes well for a number of applications.