Philip A. Heimann

Performance of the vacuum ultraviolet high-resolution and high-flux beamline for chemical dynamics studies at the Advanced Light Source

At the Advanced Light Source an undulator beamline, with an energy range from 6 to 30 eV, has been constructed for chemical dynamics experiments. The higher harmonics of the undulator are suppressed by a novel, windowless gas filter. In one branchline high-flux, 2% bandwidth radiation is directed toward an end station for photodissociation and crossed molecular-beam experiments. A photon flux of 1016 photon/s has been measured at this end station. In a second branchline a 6.65 m off-plane Eagle monochromator delivers narrow bandwidth radiation to an end station for photoionoization studies. At this second end station a peak flux of 3×1011 was observed for 25 000 resolving power. This monochromator has achieved a resolving power of 70 000 using a 4800 grooves/mm grating, one of the highest resolving powers obtained by a vacuum ultraviolet monochromator.

A differentially pumped harmonic filter on the Chemical Dynamics Beamline at the Advanced Light Source

A differentially pumped rare gas cell has been developed to suppress undulator harmonics on the Chemical Dynamics Beamline at the Advanced Light Source. Greater than 104 suppression of the harmonics has been demonstrated with no measurable (<5%) attenuation of the fundamental. The overall design is presented, and vacuum and optical performance are reported.

A setup for ultrafast time-resolved x-ray absorption spectroscopy

We present a setup which allows the measurement of time-resolved x-ray absorption spectra with picosecond temporal resolution on liquid samples at the Advanced Light Source at Lawrence Berkeley National Laboratories. The temporal resolution is limited by the pulse width of the synchrotron source. We characterize the different sources of noise that limit the experiment and present a single-pulse detection scheme.

A high resolution photoionization study of Ne and Ar: Observation of mass analyzed threshold ions using synchrotron radiation and direct current electric fields

Using the high resolution vacuum ultraviolet (vuv) photon source provided by the monochromatized undulator synchrotron radiation of the Chemical Dynamics Beamline at the Advanced Light Source, we have measured the photoionization efficiency (PIE) spectrum for Ne in the energy range of 21.56–21.67 eV at a wavelength resolution of 0.3 meV [full width at half‐maximum (FWHM)]. The PIE spectra for Ne obtained using 0.76 and 2.4 V/cm electric fields reveal autoionizing features attributable to the Rydberg states Ne[2p5ns′(1/2)1; n=14–29] and Ne[2p5nd′(3/2)1; n=12–35] converging to the spin–orbit excited Ne+(2P1/2) state. The positions of these Rydberg states are compared to previous experimental results and those calculated using the quantum defects and IE for Ne+(2P1/2) given in Moore [Natl. Stand Ref. Data Ser. Natl. Bur. Stand. 35 (1971)]. We have also observed mass analyzed threshold ions (MATI) for Ne formed in the Ne+(2P3/2,1/2) states. For Ar, only the MATI peak for Ar+(2P3/2) is observed. The failure to...

High resolution threshold and pulsed field ionization photoelectron spectroscopy using multi-bunch synchrotron radiation

We have demonstrated a resolution of 0.8 meV [full width at half-maximum (FWHM)] for threshold photoelectron measurements using a steradiancy-type zero kinetic energy photoelectron (ZEKE-PE) analyzer and the high resolution monochromatized vacuum ultraviolet (VUV) undulator synchrotron radiation of the chemical dynamics beamline at the advanced light source (ALS). Using this high resolution ZEKE-PE energy analyzer to filter prompt electrons and by employing a proper voltage pulsing scheme adapted to the timing structure of the ALS, we have achieved a resolution of 0.5 meV (FWHM) for pulsed field ionization photoelectron (PFI-PE) measurements with little contamination from prompt photoelectrons produced from direct photoionization and autoionizing processes. The experiment scheme presented here is generally applicable to PFI-PE studies using multi-bunch VUV synchrotron radiation at other synchrotron radiation facilities.

Linac Coherent Light Source soft x-ray materials science instrument optical design and monochromator commissioning

We present the x-ray optical design of the soft x-ray materials science instrument at the Linac Coherent Light Source, consisting of a varied line-spaced grating monochromator and Kirkpatrick-Baez refocusing optics. Results from the commissioning of the monochromator are shown. A resolving power of 3000 was achieved, which is within a factor of two of the design goal.

High resolution soft X-ray bending magnet beamline 9.3.2 with circularly polarized radiation capability at the Advanced Light Source

Abstract Bending magnet beamline 9.3.2 at the Advanced Light Source (ALS) was designed for high resolution spectroscopy in the soft x-ray energy region, covering a range from 30 eV to 1500 eV with three gratings. The monochromator itself is a standard fixed included angle 55 m spherical grating monochromator and was originally used at the Stanford Synchrotron Radiation Laboratory (SSRL) as a prototype for later insertion device based monochromators for the ALS. For operations at the ALS, the toroidal pre-mirror used at SSRL to vertically focus onto the entrance slit and horizontally focus onto the exit slit was replaced by two separate crossed mirrors (Kirkpatrick-Baez configuration). Circularly polarized radiation is obtained by inserting a water-cooled movable aperture in front of the vertically focusing mirror to allow selecting the beam either above or below the horizontal plane. To maintain a stable beam intensity through the entrance slit, the photocurrent signals from the upper and lower jaws of the entrance slit are utilized to set a feedback loop with the vertically deflecting mirror Piezoelectric drive. The beamline end station has a rotatable platform (through 60°) that accommodates two experimental chambers, enabling the synchrotron radiation to be directed to either one without breaking vacuum.

Shape‐resonant and many‐electron effects in the S 2p photoionization of SF6

The core‐level photoexcitation and photoionization of SF6 were studied in the vicinity of the resonances below and above the S 2p threshold. The decay channels of the S 2p→6a1g discrete excitation were characterized, with decay leading mostly to valence‐shell satellites. The S 2p continuum data show an oscillatory asymmetry parameter β(S 2p) near threshold that is virtually identical to β(Si 2p) in SiF4. It also resembles—but differs from—theoretical curves for β(S 2p) in atomic sulfur and in SF6. Data at the feature assigned as an eg shape resonance indicate strong multielectron properties for this state, because a resonance in the S 2p satellite is observed at the same photon energy as the main‐line resonance. We propose a unified model which generally includes configuration interaction both in the continuum‐state manifold and between discrete doubly excited states and the continua, to explain this unexpected satellite behavior. Finally, the S(L2,3VV) Auger electron asymmetry parameter shows no signific...

A high resolution energy-selected kinetic energy release study of the process SF6+hν→SF5++F+e−: Heat of formation of SF5+

Using the newly constructed photoelectron-photoion coincidence apparatus associated with the chemical dynamics beamline at the advanced light source, we have performed a high resolution energy-selected kinetic energy release measurement for the dissociative photoionization process SF6+hν→SF5++F+e−. After taking into account the center-of-mass kinetic energy release, the thermochemical threshold for this process is determined to be 14.11±0.08 eV. This value yields 18.5±1.9 and −202.9±2.2 kcal/mol for the heats of formation at 0 K for SF5+ and SF5, respectively.

The Matter in Extreme Conditions instrument at the Linac Coherent Light Source

A description of the Matter in Extreme Conditions instrument at the Linac Coherent Light Source is given. Recent scientific highlights illustrate phase-contrast imaging of shock waves, X-ray Thomson scattering and X-ray diffraction of shocked materials.