Does femtosecond time-resolved second-harmonic generation probe electron temperatures at surfaces?

Femtosecond pump-probe second-harmonic generation (SHG) and transient linear reflectivity measurements were carried out on polycrystalline Cu, Ag and Au in air to analyze whether the electron temperature affects Fresnel factors or nonlinear susceptibilities, or both. Sensitivity to electron temperatures was attained by using photon energies near the interband transition threshold. We find that the nonlinear susceptibility carries the electron temperature dependence in case of Ag and Au, while for Cu the dependence is in the Fresnel factors. This contrasting behavior emphasizes that SHG is not a priori sensitive to electron dynamics at surfaces or interfaces, notwithstanding its cause.Comment: 11 pages, 4 figure

Probing reaction dynamics of transition-metal complexes in solution via time-resolved soft x-ray spectroscopy

We report the first time-resolved soft x-ray measurements of solvated transition-metal complexes. L-edge spectroscopy directly probes dynamic changes in ligand-field splitting of 3d orbitals associated with the spin transition, and mediated by changes in ligand-bonding. We report the first time-resolved soft x-ray spectroscopy of solution-phase molecular dynamics. Changes in ligand-field splitting and spin-state populations in 3d orbitals of the Fe{sup II} complex are directly probed via transient absorption changes of the Fe L{sub 2} and L{sub 3} edges following photo-induced metal-to-ligand charge transfer. With the emergence of high-flux ultrafast soft x-ray sources, details on interplay between atomic structure, electronic states, and spin contributions will be revealed. Our experimental approach opens the door to femtosecond soft x-ray investigations of liquid phase chemistry that have previously been inaccessible

Lattice motions from THz phonon polaritons measured with femtosecond X-ray diffraction

We use femtosecond x-ray diffraction to measure the coherent lattice displacements associated with the excitation and propagation of THz phonon polaritons in LiTaO3

Femtosecond X-ray Pulses from a Synchrotron

An important frontier in ultrafast science is the application of femtosecond x-ray pulses to the study of structural dynamics in condensed matter. We show that femtosecond laser pulses can be used to generate high-brightness, tunable, femtosecond x-ray pulses from a synchrotron. Performance of existing and proposed femtosecond x-ray beamlines at the Advanced Light Source synchrotron are discussed

Giant, ultrafast optical switching based on an Insulator-to-Metal Transition in VO2 Nano-particles: Photo-activation of shape-controlled plasmons at 1.55 mu-m

A new generation of devices where the electronic, optical or magnetic state of a system can be controlled optically on the ultrafast timescale is one of the most compelling technological ramifications of the rapidly advancing field of strongly correlated electrons. However, for real-world applications it is also necessary to incorporate these compounds in appropriate environments (e.g. optical fibers or silicon-based electronics), to ensure compatibility with existing technologies (e.g. telecom wavelengths), room temperature operation and limited power densities. Here, we report on the study of the photo-activated optical switching in nanorods of strongly correlated VO{sub 2}. The particles are grown by ion-implantation and self-assembly within a Silica matrix or an optical fiber, operate at room temperature and can be switched between the insulating and metallic phase within less than 100 fs. The energy threshold to achieve switching corresponds to approximately 500 pJ within the core of a single mode fiber and is compatible with current diode technologies. Tailoring of the spherical/cylindrical geometry results in control of the spectral response of the system, which is dominated by the impulsive formation of a surface plasmon upon the insulator-to-metal transition. The response at the technologically important 1.55 {micro}m wavelength is in this way maximized

Ultrafast x-ray science at the Advanced Light Source

Our scientific understanding of the static or time-averaged structure of condensed matter on the atomic scale has been dramatically advanced by direct structural measurements using x-ray techniques and modern synchrotron sources. Of course the structure of condensed matter is not static, and to understanding the behavior of condensed matter at the most fundamental level requires structural measurements on the time scale on which atoms move. The evolution of condensed-matter structure, via the making and breaking of chemical bonds and the rearrangement of atoms, occurs on the fundamental time scale of a vibrational period, ~;100 fs. Atomic motion and structural dynamics on this time scale ultimately determine the course of phase transitions in solids, the kinetic pathways of chemical reactions, and even the efficiency and function of biological processes. The integration of x-ray measurement techniques, a high-brightness femtosecond x-ray source, femtosecond lasers, and stroboscopic pump-probe techniques will provide the unique capability to address fundamental scientific questions in solid-state physics, chemistry, AMO physics, and biology involving structural dynamics. In this paper, we review recent work in ultrafast x-ray science at the ALS including time-resolved diffraction measurements and efforts to develop dedicated beamlines for femtosecond x-ray experiments