Eric M. Dufresne

Probing Impulsive Strain Propagation with X-Ray Pulses

Pump-probe time-resolved x-ray diffraction of allowed and nearly forbidden reflections in InSb is used to follow the propagation of a coherent acoustic pulse generated by ultrafast laser excitation. The surface and bulk components of the strain could be simultaneously measured due to the large x-ray penetration depth. Comparison of the experimental data with dynamical diffraction simulations suggests that the conventional model for impulsively generated strain underestimates the partitioning of energy into coherent modes.

Coherent control of pulsed X-ray beams

Synchrotrons produce continuous trains of closely spaced X-ray pulses. Application of such sources to the study of atomic-scale motion requires efficient modulation of these beams on timescales ranging from nanoseconds to femtoseconds. However, ultrafast X-ray modulators are not generally available. Here we report efficient subnanosecond coherent switching of synchrotron beams by using acoustic pulses in a crystal to modulate the anomalous low-loss transmission of X-ray pulses. The acoustic excitation transfers energy between two X-ray beams in a time shorter than the synchrotron pulse width of about 100 ps. Gigahertz modulation of the diffracted X-rays is also observed. We report different geometric arrangements, such as a switch based on the collision of two counter-propagating acoustic pulses: this doubles the X-ray modulation frequency, and also provides a means of observing a localized transient strain inside an opaque material. We expect that these techniques could be scaled to produce subpicosecond pulses, through laser-generated coherent optical phonon modulation of X-ray diffraction in crystals. Such ultrafast capabilities have been demonstrated thus far only in laser-generated X-ray sources, or through the use of X-ray streak cameras.

The 7BM beamline at the APS: a facility for time-resolved fluid dynamics measurements

The 7BM beamline, a facility for time-resolved fluid dynamics measurements at the Advanced Photon Source, is described.

Picosecond time-resolved laser pump/X-ray probe experiments using a gated single-photon-counting area detector.

The recent developments in X-ray detectors have opened new possibilities in the area of time-resolved pump/probe X-ray experiments; this article presents the novel use of a PILATUS detector to achieve X-ray pulse duration limited time-resolution at the Advanced Photon Source (APS), USA. The capability of the gated PILATUS detector to selectively detect the signal from a given X-ray pulse in 24 bunch mode at the APS storage ring is demonstrated. A test experiment performed on polycrystalline organic thin films of alpha-perylene illustrates the possibility of reaching an X-ray pulse duration limited time-resolution of 60 ps using the gated PILATUS detector. This is the first demonstration of X-ray pulse duration limited data recorded using an area detector without the use of a mechanical chopper array at the beamline.

Lithium metal for x-ray refractive optics

Lithium metal is the best material for refractive lenses that must focus x-rays with energies below 15 keV, but to date no lens from Li has been reported. This letter demonstrates focusing of 10 keV x-rays with a one-dimensional sawtooth lens made from Li. The lens’ theoretical gain is 4.5, with manufacturing imperfections likely responsible for the threefold gain that is observed. Despite the Li reactivity the lens is stable over months of operation if kept under vacuum.

Transient Strain Driven by a Dense Electron-Hole Plasma

We measure transient strain in ultrafast laser-excited Ge by time-resolved x-ray anomalous transmission. The development of the coherent strain pulse is dominated by rapid ambipolar diffusion. This pulse extends considerably longer than the laser penetration depth because the plasma initially propagates faster than the acoustic modes. X-ray diffraction simulations are in agreement with the observed dynamics.

X‐ray synchrotron studies of ultrafast crystalline dynamics

Ultrafast X-ray experiments at synchrotron sources hold tremendous promise for measuring the atomistic dynamics of materials under a wide variety of transient conditions. In particular, the marriage of synchrotron radiation and ultrafast laser technology is opening up a new frontier of materials research. Structural changes initiated by femtosecond laser pulses can be tracked in real time using time-resolved X-ray diffraction on picosecond time scales or shorter. Here, research at the Advanced Photon Source is described, illustrating the opportunities for ultrafast diffraction with some recent work on the generation of impulsive strain, coherent phonon generation and supersonic diffusion of electron-hole plasmas. The flexibility of time-resolved Bragg and Laue diffraction geometries are both utilized to illuminate the strain generation and evolution process. Time-resolved X-ray science will become increasingly important with the construction of linac-based ultrafast X-ray sources.

Subnanosecond piezoelectric x-ray switch

We report an ultrafast piezoelectric switch for synchrotron x rays. A thin epitaxial film of piezoelectric Pb(Zr,Ti)O3 works as a diffractive optical switch at frequencies from dc to >1GHz. The broad frequency range allows single bunches of synchrotron x rays to be selected in an arbitrary sequence. The piezoelectric effect introduces mechanical strains of a fraction of 1% in the Pb(Zr,Ti)O3 film, which can be used for blocking or passing diffracted x rays.

Structural and electronic recovery pathways of a photoexcited ultrathin VO 2 film

The structural and electronic recovery pathways of a photoexcited ultrathin VO2 film at nanosecond time scales have been studied using time-resolved x-ray diffraction and transient optical absorption techniques. The recovery pathways from the tetragonal metallic phase to the monoclinic insulating phase are highly dependent on the optical pump fluence. At pump fluences higher than the saturation fluence of 14.7 mJ/cm2, we observed a transient structural state with lattice parameter larger than that of the tetragonal phase, which is decoupled from the metal-to-insulator phase transition. Subsequently, the photoexcited VO2 film recovered to the ground state at characteristic times dependent upon the pump fluence, as a result of heat transport from the film to the substrate. We present a procedure to measure the time-resolved film temperature by correlating photoexcited and temperature-dependent x-ray diffraction measurements. A thermal transport model that incorporates changes of the thermal parameters across the phase transition reproduces the observed recovery dynamics. The optical excitation and fast recovery of ultrathin VO2 films provides a practical method to reversibly switch between the monoclinic insulating and tetragonal metallic state at nanosecond time scales.

Time-Resolved Research at the Advanced Photon Source Beamline 7-ID

The Sector 7 undulator beamline (7‐ID) of the Advanced Photon Source (APS) is dedicated to time‐resolved x‐ray research and is capable of ultrafast measurements on the order of 100 ps. Beamline 7‐ID has a laser laboratory featuring a Ti:Sapphire system (average power of 2.5 W, pulse duration <50 fs, repetition rate 1–5 kHz) that can be synchronized to the bunch pattern of the storage ring. The laser is deliverable to x‐ray enclosures, which contain diffractometers, as well as motorized optical tables for table‐top experiments. Beamline 7‐ID has a single APS Undulator A and uses a diamond (111) double‐crystal monochromator, providing good energy resolution over a range of 6–24 keV. Available optics include Kirkpatrick‐Baez (KB) mirrors to microfocus the x‐ray beam. A variety of time‐resolved diffraction and spectroscopy research is available at 7‐ID, with experiments being done in the atomic, molecular, optical, chemistry, and solid state (bulk and surface) fields.