Fluorescence depolarization in poly[2-methoxy-5-((2-ethylhexyl)oxy)-1,4-phenylenevinylene]: sites versus eigenstates hopping

The Journal of Chemical Physics
Jaykrishna SinghGregory D Scholes

Abstract

We report upon a theoretical study of singlet exciton migration and relaxation within a model conjugated polymer chain. Starting from poly[2-methoxy-5-((2-ethylhexyl)oxy)-1,4-phenylenevinylene] polymer chains, we assume that the pi-conjugation is disrupted by conformational disorder of the chain itself, giving rise to a localized Frenkel exciton basis. Electronic coupling between segments as determined by the coupling between the transition densities of the localized excitons gives rise to delocalized exciton states. Using a kinetic Monte Carlo approach to compute the exciton transfer kinetics within the manifold of either the dressed chromophore site basis or dressed eigenstate basis, we find that the decay of the polarization anisotropy of the exciton is profoundly affected by the delocalization of the exciton over multiple basis segments. Two time scales emerge from the exciton migration simulations: a short, roughly 10 ps, time scale corresponding to rapid hopping about the initial excitation site followed by a slower, 180 ps, component corresponding to long range hopping. We also find that excitations can become trapped at long times when the hopping rate to lower-energy states is longer than the radiative lifetime of the ...Continue Reading

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Citations

Oct 4, 2012·The Journal of Physical Chemistry. a·William BarfordAlec Ward
Feb 23, 2013·The Journal of Physical Chemistry. a·William Barford
Jun 15, 2010·Physical Chemistry Chemical Physics : PCCP·Jaykrishna Singh, Eric R Bittner
Jul 23, 2011·Physical Chemistry Chemical Physics : PCCP·Subhash S Pingale
Nov 5, 2014·The Journal of Chemical Physics·William Barford, Oliver Robert Tozer
Jan 2, 2016·The Journal of Physical Chemistry Letters·Marina CorbellaCarles Curutchet
Jul 3, 2015·The Journal of Chemical Physics·Xunmo Yang, Eric R Bittner
Sep 7, 2016·Chemistry : a European Journal·Roza Al-AqarAnthony Harriman
Feb 13, 2016·Physical Review. E·Jan J J Roden, K Birgitta Whaley
Jun 25, 2015·The Journal of Physical Chemistry. B·Elizabeth M Y LeeAdam P Willard
Jan 12, 2011·The Journal of Physical Chemistry. B·Tammie NelsonSergei Tretiak

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