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Howard, A. J.

Publications and source records attributed to Howard, A. J..

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↗

Strong-field ionization of water: Nuclear dynamics revealed by varying the pulse duration

Polyatomic molecules in strong laser fields can undergo substantial nuclear motion within tens of femtoseconds. Ion imaging methods based on dissociation or Coulomb explosion therefore have difficulty faithfully recording the geometry dependence of the field ionization that initiates the dissociation process. Here we compare the strong-field double ionization and subsequent dissociation of water (both H 2 O and D 2 O) in 10-fs and 40-fs 800-nm laser pulses. We find that 10-fs pulses turn off before substantial internuclear motion occurs, whereas rapid internuclear motion can take place during the double ionization process for 40-fs pulses. The short-pulse measurements are consistent with a simple tunnel ionization picture whose predictions help interpret the motion observed in the long-pulse measurements.

74 ATOMIC AND MOLECULAR PHYSICS↗

Photon Acceleration in a Flying Focus

A high-intensity laser pulse propagating through a medium triggers an ionization front that can accelerate and frequency-upshift the photons of a second pulse. Here, the maximum upshift is ultimately limited by the accelerated photons outpacing the ionization front or the ionizing pulse refracting from the plasma. Here we apply the flying focus—a moving focal point resulting from a chirped laser pulse focused by a chromatic lens—to overcome these limitations. Theory and simulations demonstrate that the ionization front produced by a flying focus can frequency-upshift an ultrashort optical pulse to the extreme ultraviolet over a centimeter of propagation. An analytic model of the upshift predicts that this scheme could be scaled to a novel table-top source of spatially coherent x-rays.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗