Manipulating Triplet Yield through Control of Symmetry-Breaking Charge Transfer

The Journal of Physical Chemistry Letters
Saptaparna DasStephen E Bradforth

Abstract

The efficiency of an organic solar cell depends on the efficacy of exciton diffusion and dissociation processes, and this can be enhanced by reducing the exciton binding energy and increasing the exciton lifetime. Zinc chlorodipyrrin (ZCl) complexes exhibit reduced exciton binding energy due to ultrafast generation of intramolecular charge transfer (ICT) states via symmetry-breaking charge transfer in polar media. This Letter explores the fate of the ICT states using nanosecond transient absorption. In cyclohexane, ZCl undergoes intersystem crossing to produce triplets with ∼8 ns time constant (∼30% yield), and no ICT states are generated. However, in more polar solvents, triplets are generated within 1 ns via ICT state recombination with ∼3 times higher yield than produced via ISC. This high triplet yield in toluene (89%) and acetonitrile (76%) via ICT state recombination is a beneficial pathway to spin-protect the excited-state decay for additional charge generation from triplet excited states.

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Citations

Nov 30, 2018·Physical Chemistry Chemical Physics : PCCP·Romain LetrunEric Vauthey
Apr 26, 2019·Faraday Discussions·Michael KelloggMark E Thompson
Dec 18, 2019·Chemistry : a European Journal·Josué JiménezSantiago de la Moya
May 18, 2020·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Zoltan SzakacsEric Vauthey
Jul 7, 2020·Physical Chemistry Chemical Physics : PCCP·Xinmiao NiuAndong Xia
Sep 22, 2018·Proceedings of the National Academy of Sciences of the United States of America·Doran I G BennettKapil Amarnath
Jul 17, 2021·The Journal of Physical Chemistry. B·Stanislav L BondarevAnatoly I Ivanov
Nov 25, 2020·The Journal of Physical Chemistry Letters·Jie KongAndong Xia
Oct 7, 2020·Journal of the American Chemical Society·Carolyn E RamirezMichael R Wasielewski
Nov 18, 2020·The Journal of Physical Chemistry. B·Alexey E Nazarov, Anatoly I Ivanov

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