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Time-resolved site-selective imaging of predissociation and charge transfer dynamics: The CH3I B-band
2020, Forbes, Ruaridh, Allum, Felix, Bari, Sadia, Boll, Rebecca, Borne, Kurtis, Brouard, Mark, Bucksbaum, Philip H., Ekanayake, Nagitha, Erk, Benjamin, Howard, Andrew J., Johnsson, Per, Lee, Jason W.L., Manschwetus, Bastian, Mason, Robert, Passow, Christopher, Peschel, Jasper, Rivas, Daniel E., Rörig, Aljoscha, Rouzée, Arnaud, Vallance, Claire, Ziaee, Farzaneh, Rolles, Daniel, Burt, Michael
The predissociation dynamics of the 6s (B2E) Rydberg state of gas-phase CH3I were investigated by time-resolved Coulomb-explosion imaging using extreme ultraviolet (XUV) free-electron laser pulses. Inner-shell ionization at the iodine 4d edge was utilized to provide a site-specific probe of the ensuing dynamics. The combination of a velocity-map imaging (VMI) spectrometer coupled with the pixel imaging mass spectrometry (PImMS) camera permitted three-dimensional ionic fragment momenta to be recorded simultaneously for a wide range of iodine charge states. In accord with previous studies, initial excitation at 201.2 nm results in internal conversion and subsequent dissociation on the lower-lying A-state surface on a picosecond time scale. Examination of the time-dependent yield of low kinetic energy iodine fragments yields mechanistic insights into the predissociation and subsequent charge transfer following multiple ionization of the iodine products. The effect of charge transfer was observed through differing delay-dependencies of the various iodine charge states, from which critical internuclear distances for charge transfer could be inferred and compared to a classical over-the-barrier model. Time-dependent photofragment angular anisotropy parameters were extracted from the central slice of the Newton sphere, without Abel inversion, and highlight the effect of rotation of the parent molecule before dissociation, as observed in previous © 2020 The Author(s). Published by IOP Publishing Ltd Printed in the UK
Singleshot polychromatic coherent diffractive imaging with a high-order harmonic source
2020, Malm, Erik, Wikmark, Hampus, Pfau, Bastian, Villanueva-Perez, Pablo, Rudawski, Piotr, Peschel, Jasper, Maclot, Sylvain, Schneider, Michael, Eisebitt, Stefan, Mikkelsen, Anders, L’Huillier, Anne, Johnsson, Per
Singleshot polychromatic coherent diffractive imaging is performed with a high-intensity high-order harmonic generation source. The coherence properties are analyzed and several reconstructions show the shot-to-shot fluctuations of the incident beam wavefront. The method is based on a multi-step approach. First, the spectrum is extracted from double-slit diffraction data. The spectrum is used as input to extract the monochromatic sample diffraction pattern, then phase retrieval is performed on the quasi-monochromatic data to obtain the sample’s exit surface wave. Reconstructions based on guided error reduction (ER) and alternating direction method of multipliers (ADMM) are compared. ADMM allows additional penalty terms to be included in the cost functional to promote sparsity within the reconstruction. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement.