Initial-site characterization of hydrogen migration following strong-field double-ionization of ethanol.

An essential problem in photochemistry is understanding the coupling of electronic and nuclear dynamics in molecules, which manifests in processes such as hydrogen migration. Measurements of hydrogen migration in molecules that have more than two equivalent hydrogen sites, however, produce data that is difficult to compare with calculations because the initial hydrogen site is unknown. We demonstrate that coincidence ion-imaging measurements of a few deuterium-tagged isotopologues of ethanol can determine the contribution of each initial-site composition to hydrogen-rich fragments following strong-field double ionization.

Single- and multi-photon-induced ultraviolet excitation and photodissociation of CHI probed by coincident ion momentum imaging.

The UV-induced photodissociation dynamics of iodomethane (CHI) in its A-band are investigated by time-resolved coincident ion momentum imaging using strong-field ionization as a probe. The delay-dependent kinetic energy distribution of the photofragments resulting from double ionization of the molecule maps the cleavage of the carbon-iodine bond and shows how the existence of a potential well in the di-cationic potential energy surfaces shapes the observed distribution at small pump-probe delays. Furthermore, the competition between single- and multi-photon excitation and ionization of the molecule is studied as a function of the intensity of the UV-pump laser pulse.

Two- and three-body fragmentation of multiply charged tribromomethane by ultrafast laser pulses.

We investigate the two- and three-body fragmentation of tribromomethane (bromoform, CHBr) resulting from multiple ionization by 28-femtosecond near-infrared laser pulses with a peak intensity of 6 × 10 W cm. The analysis focuses on channels consisting exclusively of ionic fragments, which are measured by coincidence momentum imaging. The dominant two-body fragmentation channel is found to be Br + CHBr.

Strong-Field-Induced Coulomb Explosion Imaging of Tribromomethane.

The Coulomb explosion of tribromomethane (bromoform, CHBr) induced by 28 fs near-infrared laser pulses is investigated by three-dimensional coincidence ion momentum imaging. We focus on the fragmentation into three, four, and five ionic fragments measured in coincidence and present different ways of visualizing the three-dimensional momentum correlations. We show that the experimentally observed momentum correlations for 4- and 5-fold coincidences are well reproduced by classical Coulomb explosion simulations and contain information about the structure of the parent molecule that could be used to differentiate structural isomers formed, for example, in a pump-probe experiment.

Multi-channel photodissociation and XUV-induced charge transfer dynamics in strong-field-ionized methyl iodide studied with time-resolved recoil-frame covariance imaging.

The photodissociation dynamics of strong-field ionized methyl iodide (CH3I) were probed using intense extreme ultraviolet (XUV) radiation produced by the SPring-8 Angstrom Compact free electron LAser (SACLA). Strong-field ionization and subsequent fragmentation of CH3I was initiated by an intense femtosecond infrared (IR) pulse. The ensuing fragmentation and charge transfer processes following multiple ionization by the XUV pulse at a range of pump-probe delays were followed in a multi-mass ion velocity-map imaging (VMI) experiment.

Synthesis and application of a green surfactant for the treatment of water containing PFAS/ hazardous metal ions.

In this work, the effectiveness of a biodegradable and natural surfactant synthesized through a novel method has been studied through the ion flotation process to treat waters containing Per/Poly Fluoroalkyl Substances (PFAS) and heavy-metal ions. This cysteine-based surfactant, which is environmentally acceptable, showed considerable solubility and foaming ability over a wide range of pH. It also could remove 97-99(%) of 5 mg/L of cadmium, chromium, copper, nickel, zinc, and manganese ions in a single batch physicochemical process.

H roaming chemistry and the formation of H from organic molecules in strong laser fields.

Roaming mechanisms, involving the brief generation of a neutral atom or molecule that stays in the vicinity before reacting with the remaining atoms of the precursor, are providing valuable insights into previously unexplained chemical reactions. Here, the mechanistic details and femtosecond time-resolved dynamics of H formation from a series of alcohols with varying primary carbon chain lengths are obtained through a combination of strong-field laser excitation studies and ab initio molecular dynamics calculations. For small alcohols, four distinct pathways involving hydrogen migration and H roaming prior to H formation are uncovered.

Coulomb explosion imaging of CHI and CHClI photodissociation dynamics.

The photodissociation dynamics of CHI and CHClI at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815 nm probe pulse. Fragment ion momenta over a wide / range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion.

Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation.

A key question concerning the three-body fragmentation of polyatomic molecules is the distinction of sequential and concerted mechanisms, i.e., the stepwise or simultaneous cleavage of bonds.

Time-resolved ion imaging at free-electron lasers using TimepixCam.

The application of a novel fast optical-imaging camera, TimepixCam, to molecular photoionization experiments using the velocity-map imaging technique at a free-electron laser is described. TimepixCam is a 256 × 256 pixel CMOS camera that is able to detect and time-stamp ion hits with 20 ns timing resolution, thus making it possible to record ion momentum images for all fragment ions simultaneously and avoiding the need to gate the detector on a single fragment. This allows the recording of significantly more data within a given amount of beam time and is particularly useful for pump-probe experiments, where drifts, for example, in the timing and pulse energy of the free-electron laser, severely limit the comparability of pump-probe scans for different fragments taken consecutively.