Ultrafast dynamics of formation and autodetachment of a dipole-bound state in an open-shell π-stacked dimer anion

Chemical Science
James N BullJan R R Verlet

Abstract

Isolated π-stacked dimer radical anions present the simplest model of an excess electron in a π-stacked environment. Here, frequency-, angle-, and time-resolved photoelectron imaging together with electronic structure calculations have been used to characterise the π-stacked coenzyme Q0 dimer radical anion and its exited state dynamics. In the ground electronic state, the excess electron is localised on one monomer with a planar para-quinone ring, which is solvated by the second monomer in which carbonyl groups are bent out of the para-quinone ring plane. Through the π-stacking interaction, the dimer anion exhibits a number of charge-transfer (intermolecular) valence-localised resonances situated in the detachment continuum that undergo efficient internal conversion to a cluster dipole-bound state (DBS) on a ∼60 fs timescale. In turn, the DBS undergoes vibration-mediated autodetachment on a 2.0 ± 0.2 ps timescale. Experimental vibrational structure and supporting calculations assign the intermolecular dynamics to be facilitated by vibrational wagging modes of the carbonyl groups on the non-planar monomer. At photon energies ∼0.6-1.0 eV above the detachment threshold, a competition between photoexcitation of an intermolecular re...Continue Reading

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Citations

Sep 18, 2018·Physical Chemistry Chemical Physics : PCCP·Cate S AnstöterJan R R Verlet
May 11, 2019·Physical Chemistry Chemical Physics : PCCP·James N BullJan R R Verlet
Oct 31, 2019·Physical Chemistry Chemical Physics : PCCP·Maria Elena CastellaniJan R R Verlet
Nov 30, 2019·The Journal of Chemical Physics·Golda Mensa-BonsuJan R R Verlet
May 10, 2020·The Journal of Chemical Physics·Golda Mensa-BonsuJan R R Verlet
Dec 22, 2019·Nature Communications·James N BullJan R R Verlet
Jun 1, 2017·Science Advances·James N Bull, Jan R R Verlet
Sep 28, 2017·Physical Chemistry Chemical Physics : PCCP·James N Bull, Jan R R Verlet
Sep 12, 2020·Physical Review Letters·Do Hyung KangSang Kyu Kim
Feb 17, 2021·The Journal of Physical Chemistry Letters·Do Hyung KangSang Kyu Kim
Mar 10, 2021·Physical Chemistry Chemical Physics : PCCP·Eleanor K AshworthJames N Bull
Sep 19, 2019·The Journal of Physical Chemistry. a·Christopher L AdamsJ Mathias Weber
Nov 5, 2016·The Journal of Physical Chemistry Letters·Christopher W WestJan R R Verlet
Apr 26, 2018·The Journal of Physical Chemistry Letters·Joshua P RogersJan R R Verlet
Jan 30, 2019·The Journal of Physical Chemistry. a·Joshua P RogersJan R R Verlet
Feb 16, 2019·The Journal of Physical Chemistry. B·Alexandra L Tyson, Jan R R Verlet
Feb 28, 2020·The Journal of Physical Chemistry. a·James N BullJan R R Verlet
Apr 3, 2020·The Journal of Physical Chemistry. a·Jan R R VerletJoshua P Rogers

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