Improved insights in time-resolved photoelectron imaging

Kotsina, Nikoleta; Townsend, David

doi:10.1039/d1cp00933h

Cited by 17 publications

(16 citation statements)

References 126 publications

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“…This is a parallel model (i.e., all fitted functions originate from Δ t = 0) that assumes no details a priori about the nature (sequential or otherwise) of the participating mechanistic processes. Illustrative examples and additional details may be found elsewhere. − …”

Section: Methodsmentioning

confidence: 99%

Ultraviolet Excitation Dynamics of Nitrobenzenes

et al. 2021

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Time-resolved photoelectron imaging was used to investigate nonadiabatic processes operating in the excited electronic states of nitrobenzene and three methyl-substituted derivatives: 3,5-, 2,6-, and 2,4-dimethylnitrobenzene. The primary goal was evaluating the dynamical impact of the torsional angle between the NO2 group and the benzene ring planesomething previously implicated in mediating the propensity for branching into different photodissociation pathways (NO vs NO2 elimination). Targeted, photoinitiated release of NO radicals is of interest for clinical medicine applications, and there is a need to establish basic structure–dynamics–function principles in systematically varied model systems following photoexcitation. Within our 200 ps experimental detection window, we observed no significant differences in the excited-state lifetimes exhibited by all species under study using a 267 nm pump and ionization with an intense 400 nm probe. In agreement with previous theoretical predictions, this suggests that the initial energy redistribution dynamics within the singlet and triplet manifolds are driven by motions localized predominantly on the NO2 group. Our findings also imply that both NO and NO2 elimination occur from a vibrationally hot ground state on extended (nanosecond) timescales, and any variations in NO vs NO2 branching upon site-selective methylation are due to steric effects influencing isomerization prior to dissociation.

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Section: Methodsmentioning

confidence: 99%

Ultraviolet Excitation Dynamics of Nitrobenzenes

et al. 2021

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“…This methodological corpus builds up a strong potential for future studies of molecular structure and dynamics in real time. 1,444…”

Section: Perspectivementioning

confidence: 99%

“…This methodological corpus builds up a strong potential for future studies of molecular structure and dynamics in real time. 1,444 From the experimental side, new challenges are driven by the impressive achievements of light sources, both at largescale XFEL facilities and based on advanced table-top laser sources, pushing to higher intensity and higher energy photons, ever shorter pulse duration, with increasing repetition rates in the range of several hundreds of kHz up to MHz, but also ever more complex pulses and nonclassical light, characterized by fields structured in the four-dimensional space-time, with strong inhomogeneity of all light parameters. 234,236 Angular distributions from ionization with specially tailored fields are mostly untouched.…”

Section: Perspectivementioning

confidence: 99%