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Mason, R.

Publications and source records attributed to Mason, R..

5 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Characterizing the multi-dimensional reaction dynamics of dihalomethanes using XUV-induced Coulomb explosion imaging

Site-selective probing of iodine 4d orbitals at 13.1 nm was used to characterize the photolysis of CH 2 I 2 and CH 2 BrI initiated at 202.5 nm. Time-dependent fragment ion momenta were recorded using Coulomb explosion imaging mass spectrometry and used to determine the structural dynamics of the dissociating molecules. Correlations between these fragment momenta, as well as the onset times of electron transfer reactions between them, indicate that each molecule can undergo neutral three-body photolysis. For CH 2 I 2 , the structural evolution of the neutral molecule was simultaneously characterized along the C–I and I–C–I coordinates, demonstrating the sensitivity of these measurements to nuclear motion along multiple degrees of freedom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Fragmentation Dynamics of Fluorene Explored Using Ultrafast XUV-Vis Pump-Probe Spectroscopy

We report on the use of extreme ultraviolet (XUV, 30.3 nm) radiation from the Free-electron LASer in Hamburg (FLASH) and visible (Vis, 405 nm) photons from an optical laser to investigate the relaxation and fragmentation dynamics of fluorene ions. The ultrashort laser pulses allow to resolve the molecular processes occurring on the femtosecond timescales. Fluorene is a prototypical small polycyclic aromatic hydrocarbon (PAH). Through their infrared emission signature, PAHs have been shown to be ubiquitous in the universe, and they are assumed to play an important role in the chemistry of the interstellar medium. Our experiments track the ionization and dissociative ionization products of fluorene through time-of-flight mass spectrometry and velocity-map imaging. Multiple processes involved in the formation of each of the fragment ions are disentangled through analysis of the ion images. The relaxation lifetimes of the excited fluorene monocation and dication obtained through the fragment formation channels are reported to be in the range of a few tens of femtoseconds to a few picoseconds.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast $\mathrm{XUV}$-$\mathrm{IR}$ regime

Polycyclic aromatic hydrocarbons (PAHs) play an important role in interstellar chemistry and are subject to high energy photons that can induce excitation, ionization, and fragmentation. Previous studies have demonstrated electronic relaxation of parent PAH monocations over 10–100 femtoseconds as a result of beyond-Born-Oppenheimer coupling between the electronic and nuclear dynamics. Here, we investigate three PAH molecules: fluorene, phenanthrene, and pyrene, using ultrafast XUV and IR laser pulses. Simultaneous measurements of the ion yields, ion momenta, and electron momenta as a function of laser pulse delay allow a detailed insight into the various molecular processes. We report relaxation times for the electronically excited PAH * , PAH +* and PAH 2+* states, and show the time-dependent conversion between fragmentation pathways. Additionally, using recoil-frame covariance analysis between ion images, we demonstrate that the dissociation of the PAH 2+ ions favors reaction pathways involving two-body breakup and/or loss of neutral fragments totaling an even number of carbon atoms.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2006

Ice Chemistry Through Quiescent Dust In IC5146

IC 5146 is a nearby (200pc) dark cloud complex in Cygnus. The lack of star formation activity makes it an excellent laboratory for the study of the chemical complexity in the earliest stages of dense molecular cloud evolution. We have used the Spitzer Infrared Spectrometer (IRS) to probe dust along 10 sight-lines toward K-Giant background stars, sampling a range of visual extinction from 2-20mag. Here we present 5-20micron spectra and correlation studies of the 6.0micron water-ice band and 9.7micron silicate absorption band with Av for a sample of our Spitzer program sources. Our IC5146 Spitzer data indicate grain growth and ice formation occurs early in the history of dense cloud formation. Each sight-line observed reveals the 9.7micron amorphous silicate absorption band. The highest Av sightlines show clear detections of ices at 6.0micron (water-ice mixture), 6.85micron (processed ice) and 15.2micron (CO2). However, sight-lines in the low-to-mid Av range provide intriguing variations. We may have the first example of two objects, one with ice features and one without, seen through the same cloud sightline with similar Av approx. 6 and similar silicate band optical depths. Also, the nominally expected linear correlation of Av with silicate band depth does not appear to hold for this cloud (turnover at Av approx.10-12). Both trends imply complexities in the grain growth at one of the earliest stages of dust and ice interaction ever observed. The highest extinction source in our sample, Av=20, reveals the 6.0micron (water), 6.85micron (processed ice), 9.7micron silicate and 15.2micron CO2 ice bands. Until recently, the 6.85micron band had only been detected towards embedded protostellar objects. Two additional quiescent dust sightlines from the C2D results now also indicate the 6.85micron band (Taurus and Serpens) by Knez et al. 2005, demonstrating the role of energetic processing within pristine ices prior to the onset of star formation.

Ennico, Kimberly↗