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We photoexcite SrTiO3 and EuTiO3 in their purely soft-mode-driven structurally distorted phase and trace the structural order parameter via ultra-short x-rays. We observe a rapid decay for SrTiO3 and an intriguing transient enhancement for EuTiO3.

Time resolved optical reflectivity and x-ray diffraction techniques are employed to study the laser-induced structural response in two charge and orbitally ordered manganites. Optical data indicate a non-thermal nature of the laser-triggered phase transition via the disappearance of an optical phonon related to the charge and orbitally ordered phase. The x-ray diffraction measurements on superlattice reflections confirm the non-thermal time scale of the initial step of this phase transition but also show that the complete change of structural symmetry is not instantaneous.

We present a non-comprehensive review of some representative experimental studies in crystalline condensed matter systems where the effects of intense ultrashort light pulses are probed using x-ray diffraction and photoelectron spectroscopy. On an ultrafast (sub-picosecond) time scale, conventional concepts derived from the assumption of thermodynamic equilibrium must often be modified in order to adequately describe the time-dependent changes in material properties. There are several commonly adopted approaches to this modification, appropriate in different experimental circumstances. One approach is to treat the material as a collection of quasi-thermal subsystems in thermal contact with each other in the so-called "N-temperature" models. On the other extreme, one can also treat the time-dependent changes as fully coherent dynamics of a sometimes complex network of excitations. Here, we present examples of experiments that fall into each of these categories, as well as experiments that partake of both models. We conclude with a discussion of the limitations and future potential of these concepts.

Using femtosecond time-resolved hard x-ray diffraction, we investigate the structural dynamics of the orthorhombic distortion in the Fe-pnictide parent compound BaFe2As2. The orthorhombic distortion analyzed by the transient splitting of the (1 0 3) Bragg reflection is suppressed on an initial timescale of 35 ps, which is much slower than the suppression of magnetic and nematic order. This observation demonstrates a transient state with persistent structural distortion and suppressed magnetic/nematic order which are strongly linked in thermal equilibrium. We suggest a way of quantifying the coupling between structural and nematic degrees of freedom based on the dynamics of the respective order parameters. [ABSTRACT FROM AUTHOR]

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 Ti3+ 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. [ABSTRACT FROM AUTHOR]

The Swiss Light Source (SLS) at the Paul Scherrer Institut (PSI) started user operation in 2001. It has been the first medium energy light source to rely on undulators for the production of X-rays up to 20 keV. For soft X-rays, APPLE II-type undulators, providing full polarization control and quasiperiodic electromagnetic undulators, have been installed. The hard X-ray range has been accessed by the newly developed small-gap, short-period, in-vacuum undulators operated on high harmonics. Based on this, FEMTO, the first hard X-ray undulator source for femtosecond (fs) experiments, started operation in 2006. [ABSTRACT FROM PUBLISHER]

We have studied the ultrafast changes of electronic states in bulk ZnO upon intense hard x-ray excitation from a free electron laser. By monitoring the transient anisotropy induced in an optical probe beam, we observe a delayed breaking of the initial c-plane symmetry of the crystal that lasts for several picoseconds. Interaction with the intense x-ray pulses modifies the electronic state filling in a manner inconsistent with a simple increase in electronic temperature. These results may indicate a way to use intense ultrashort x-ray pulses to investigate high-energy carrier dynamics and to control certain properties of solid-state materials. [ABSTRACT FROM AUTHOR]

Strongly correlated electron systems often exhibit very strong interactions between structural and electronic degrees of freedom that lead to complex and interesting phase diagrams. For technological applications of these materials it is important to learn how to drive transitions from one phase to another. A key question here is the ultimate speed of such phase transitions, and to understand how a phase transition evolves in the time domain. Here we apply time-resolved X-ray diffraction to directly measure the changes in long-range order during ultrafast melting of the charge and orbitally ordered phase in a perovskite manganite. We find that although the actual change in crystal symmetry associated with this transition occurs over different timescales characteristic of the many electronic and vibrational coordinates of the system, the dynamics of the phase transformation can be well described using a single time-dependent 'order parameter' that depends exclusively on the electronic excitation. [ABSTRACT FROM AUTHOR]

The Swiss Light Source (SLS) is a synchrotron radiation user facility (2000 users/year, 18 beamlines, 5000 hrs/year) in operation at Paul Scherrer Institut (PSI) since 2001. Figure 1 presents a schematic view. [ABSTRACT FROM AUTHOR]

We use time-resolved optical reflectivity to study the laser stimulated dynamics in the magnetic shape memory alloy Ni2MnGa. We observe two coherent optical phonons, at 1.2 THz in the martensite phase and at 0.7 THz in the pre-martensite phase, which we interpret as a zone-folded acoustic phonon and a heavily damped amplitudon, respectively. In the martensite phase the martensitic phase transition can be induced by a fs laser pulse on a timescale of a few ps. [ABSTRACT FROM AUTHOR]

The timescales for structural changes in a single crystal of bismuth after excitation with an intense near-infrared laser pulse are studied with femtosecond pump-probe X-ray diffraction. Changes in the intensity and reciprocal-lattice vector of several reflections give quantitative information on the structure factor and lattice strain as a function of time, with a resolution of 200 fs. The results indicate that the majority of excess carrier energy that remains near the surface is transferred to vibrational modes on a timescale of about 10 ps, and that the resultant increase in the variance of the atomic positions at these times is consistent with the overall magnitude of lattice strain that develops. [ABSTRACT FROM AUTHOR]

FEMTO, a femtosecond (fs) X-ray source based on laser interaction with a relativistic electron beam, began operation in the fall of 2006. It is installed at the μXAS beamline of the Swiss Light Source (SLS) at the Paul Scherrer Institut, Villigen. “Laser slicing” of an electron beam has first been proposed and demonstrated at the ALS [1] and has recently been implemented at BESSY [2] to generate fs soft X-rays (1-2 keV) with variable polarization. FEMTO is the first undulator source providing tunable, fs hard X-rays in the range 4.5-12 keV for laser/X-ray pump-probe absorption and diffraction experiments. [ABSTRACT FROM AUTHOR]

The elastic and inelastic scattering ofC onC has been measured in the angular range between 2.8° and 70.4° in the c.m. system at E=300 MeV. Optical model calculations have been performed with Woods-Saxon and folded potentials, the ground state and the first 2-state were coupled in the calculations. The large cross sections of the elastic scattering at large angles is related to the nuclear rainbow scattering, which is centered at about 56°. This requires a potential depth of 100 MeV at a distance of 3 fm, the fit to the data is sensitive down to this region. The calculations with the folded potential show a better agreement with the data than those with the Woods-Saxon shape. The total reaction cross section of 1,420 mb, obtained from the optical model analysis, corresponds to the geometrical value; no transparency is observed. [ABSTRACT FROM AUTHOR]

Understanding the initial steps during ultrafast molecular reactions involving large spin state changes is a vital goal in structural dynamics research. These involve knowledge of the geometric structure of the system. Ultrafast X-ray absorption spectroscopy with 50-100 picosecond time resolution establishes the geometric structure of the short-lived (τ = 0:6 ns) high spin state. Here we focus on time-resolved X-ray absorption studies with 160-200 fs temporal resolution to monitor the structural evolution in this spin-conversion process. [ABSTRACT FROM AUTHOR]