D. A. Arms

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.

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.

Transient x-ray absorption spectroscopy of hydrated halogen atom

Time-resolved x-ray absorption spectroscopy has been used to observe the transient species generated by one-photon detachment of an electron from aqueous bromide. The K-edge spectrum of the short-lived Br(0) atom exhibits a resonant 1s-4p transition that is absent for the Br(-) precursor. The strong 1s-4p resonance suggests that there is very little charge transfer from the solvent to the open-shell atom, whereas weak oscillations above the absorption edge indicate that the solvent shell around a neutral Br(0) atom is defined primarily by hydrophobic interactions. These conclusions are in agreement with Monte Carlo and quantum chemical simulations of the solvent structure.

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.

Empirical dead-time corrections for synchrotron sources.

An experimental comparison of models for performing dead-time corrections of photon-counting detectors at synchrotron sources is presented. The performance of several detectors in the three operating modes of the Advanced Photon Source is systematically compared, with particular emphasis on asymmetric fill patterns. Several simple and well known correction formulas are evaluated. The results demonstrate the critical importance of detector speed and synchrotron fill pattern in selecting the proper dead-time correction.

An x-ray probe of laser-aligned molecules

We demonstrate a hard x-ray probe of laser-aligned small molecules. To align small molecules with optical lasers, high intensities at nonresonant wavelengths are necessary. We use 95ps pulses focused to 40μm from an 800nm Ti:sapphire laser at a peak intensity of 1012W∕cm2 to create an ensemble of aligned bromotrifluoromethane (CF3Br) molecules. Linearly polarized, 120ps x-ray pulses, focused to 10μm, tuned to the Br 1s→σ* preedge resonance at 13.476keV, probe the ensemble of laser-aligned molecules. The demonstrated methodology has a variety of applications and can enable ultrafast imaging of laser-controlled molecular motions with Angstrom-level resolution.

K-edge x-ray-absorption spectroscopy of laser-generated Kr{sup +} and Kr{sup 2+}

Tunable, polarized, microfocused x-ray pulses were used to record x-ray absorption spectra across the K edges of Kr{sup +} and Kr{sup 2+} produced by laser ionization of Kr. Prominent 1s {yields} 4p and 5p excitations are observed below the 1s ionization thresholds in accord with calculated transition energies and probabilities. Due to alignment of 4p hole states in the laser-ionization process, the Kr{sup +} 1s {yields} 4p cross section varies with respect to the angle between the laser and x-ray polarization vectors. This effect is used to determine the Kr{sup +} 4p{sub 3/2} and 4p{sub 1/2} quantum state populations, and these are compared with results of an adiabatic strong-field ionization theory that includes spin-orbit coupling.

Parabolic lithium refractive optics for x rays

Excellent x-ray optics for photons at around 10 keV can be expected with lithium metal. One of the best compound refractive lens designs [Lengeler et al., J. Appl. Phys. 84, 5855 (1998)] is now produced routinely in aluminum, and more recently has been demonstrated using beryllium [M. Kuhlmann et al. (unpublished)]. Here, we report a similar refractive lens made from lithium. At 10.87 keV, this lens has a ≃2 m focal length, more than 90% peak transmission, and an average transmission of 49%. The lens shows a very useful gain of up to 40. The full widths at half maximum (FWHM) of the focus are blurred by roughly 20 μm, resulting in a horizontal and vertical FWHM of 33 and 17 μm for an image distance of 2.13 m. The lens produces speckle on the x-ray beam, which is likely due to the inhomogeneities of the lens surface: Coherent x-ray scattering is useful in understanding imperfections in x-ray optics, such as mirrors and lenses. Better molding techniques should result in improved performance and enable microbeam techniques with this type of Li lens.

Characterization of the spatiotemporal evolution of laser-generated plasmas

We characterize the time evolution of ion spatial distributions in a laser-produced plasma. Krypton ions are produced in strong, linearly and circularly polarized optical laser fields (1014–1015 W/cm2). The Kr+ ions are preferentially detected by resonant x-ray absorption. Using microfocused, tunable x rays from Argonne’s Advanced Photon Source, we measure ion densities as a function of time with 10 μm spatial resolution for times ≤50 ns. For plasma densities of the order of 1014 cm−3, we observe a systematic expansion of the ions outward from the laser focus. We find the expansion timescale to be independent of the plasma density though strongly dependent on the plasma shape and electron temperature. The former is defined by the laser focus, while the latter is controlled by the laser polarization state. We have developed a fluid description assuming a collisionless quasineutral plasma, which is modeled using a particle-in-cell approach. This simulation provides a quantitative description of the observed...