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Belkacem, Ali

Publications and source records attributed to Belkacem, Ali.

Sizes of pure and doped helium droplets from single shot x-ray imaging

Advancements in x-ray free-electron lasers on producing ultrashort, ultrabright, and coherent x-ray pulses enable single-shot imaging of fragile nanostructures, such as superfluid helium droplets. Furthermore, this imaging technique gives unique access to the sizes and shapes of individual droplets. In the past, such droplet characteristics have only been indirectly inferred by ensemble averaging techniques. Here, we report on the size distributions of both pure and doped droplets collected from single-shot x-ray imaging and produced from the free-jet expansion of helium through a 5 μm diameter nozzle at 20 bars and nozzle temperatures ranging from 4.2 to 9 K. This work extends the measurement of large helium nanodroplets containing 10 9 –10 11 atoms, which are shown to follow an exponential size distribution. Additionally, we demonstrate that the size distributions of the doped droplets follow those of the pure droplets at the same stagnation condition but with smaller average sizes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Selective bond scission in formic acid by low-energy electrons

We report recent results of mass-resolved anion fragment momentum imaging experiments to investigate dissociative electron attachment to formic acid, for incident energies between 5 eV and 9 eV. A remarkable site-selectivity is found for a resonance at 8.5 eV by comparing anion fragment yields for two deuterated isotopologues of formic acid. This results in an H – fragment from the O-H bond of the transient anion, with negligible contribution from C-H break. In contrast, a lower-energy resonance at 7.1 eV dissociates by C–H or O–H break to produce H – and the neutral radicals HOCO or HCOO.

74 ATOMIC AND MOLECULAR PHYSICS↗

Time-Resolved Ultrafast Transient Polarization Spectroscopy to Investigate Nonlinear Processes and Dynamics in Electronically Excited Molecules on the Femtosecond Time Scale

Here, we report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of excited electronic states using the optical Kerr effect by time-resolved polarization spectroscopy. Optical heterodyne and optical homodyne detection are demonstrated to measure the third-order nonlinear optical response for the S 1 excited state of liquid nitrobenzene, which is populated by 2-photon absorption of a 780 nm 35 fs excitation pulse.

47 OTHER INSTRUMENTATION↗

Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using ultrafast transient polarization spectroscopy, extending the well-known technique of optical Kerr effect spectroscopy to excited electronic states. The third-order nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S 1 excited state. By measuring this response, which is highly sensitive to details of the excited state character and structure, as a function of time delays between the three pulses involved, we extract the dephasing time of the wave packet on the excited state. The dephasing time, measured as a function of time delay after pump excitation, shows oscillations indicating oscillatory wave packet dynamics on the excited state. Finally, from the experimental measurements and supporting theoretical calculations, we deduce that the wave packet completely leaves the S 1 state potential energy surface after three traversals of the intersystem crossing between the singlet S 1 and triplet T 2 states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗