Probing ultrafast dynamics with time-resolved multi-dimensional coincidence imaging: butadiene

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Journal titleJournal of Modern Optics
Pages14091425; # of pages: 17
Subjectultrafast dynamics, coincidence imaging, butadiene, photoionization, time-resolved photoelectron spectroscopy (TRPES), time-resolved photoelectron angular distributions (TRPADs)
AbstractTime-resolved coincidence imaging of photoelectrons and photoions represents the most complete experimental measurement of ultrafast excited state dynamics, a multi-dimensional measurement for a multi-dimensional problem. Here we present the experimental data from recent coincidence imaging experiments, undertaken with the aim of gaining insight into the complex ultrafast excited-state dynamics of 1,3-butadiene initiated by absorption of 200 nm light. We discuss photoion and photoelectron mappings of increasing dimensionality, and focus particularly on the time-resolved photoelectron angular distributions (TRPADs), expected to be a sensitive probe of the electronic evolution of the excited state and to provide significant information beyond the time-resolved photoelectron spectrum (TRPES). Complex temporal behaviour is observed in the TRPADs, revealing their sensitivity to the dynamics while also emphasising the difficulty of interpretation of these complex observables. From the experimental data some details of the wavepacket dynamics are discerned relatively directly, and we make some tentative comparisons with existing ab initio calculations in order to gain deeper insight into the experimental measurements; finally, we sketch out some considerations for taking this comparison further in order to bridge the gap between experiment and theory. © 2013 Copyright Crown Copyright 2013. Reproduced with the permission of the National Research Council of Canada.
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AffiliationSecurity and Disruptive Technologies; National Research Council Canada
Peer reviewedYes
NPARC number21270491
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Record identifier3a504ec3-2d6d-46d8-a318-3244d986e5c1
Record created2014-02-13
Record modified2016-05-09
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