Enhancing Singlet Fission Dynamics by Suppressing Destructive Interference between Charge-Transfer Pathways

The Journal of Physical Chemistry Letters
Maria A Castellanos, Pengfei Huo

Abstract

We apply a real-time path-integral approach to investigate the charge-transfer (CT)-mediated singlet fission quantum dynamics in a model pentacene dimer. Our path-integral method gives reliable fission dynamics across various reaction regimes as well as a broad range of reorganization energies and temperatures. With this method, we investigated the destructive interference between the two CT-mediated fission pathways and discovered two mechanisms that can suppress this deleterious effect. First, increasing the energy gap between the two CT states effectively shuts down the high-lying CT pathway, leaving a better functioning low-lying CT pathway with a minimum amount of destructive interference. Second, intermolecular vibrations induce electronic coupling fluctuations, such that the destructive cancellations due to the different signs in static electronic couplings are suppressed. Our numerical results suggest that these two effects can enhance the fission rate up to three times. These findings reveal promising design principles for more efficient singlet fission materials.

References

Oct 13, 2006·The Journal of Physical Chemistry. B·Randall H GoldsmithMark A Ratner
Oct 26, 2007·Journal of the American Chemical Society·Astrid M MüllerChristopher J Bardeen
Aug 4, 2009·Accounts of Chemical Research·David N BeratanDequan Xiao
Jul 24, 2010·Nature Chemistry·Paul M ZimmermanCharles B Musgrave
Oct 19, 2010·The Journal of Chemical Physics·Jonathan J BurdettChristopher J Bardeen
Nov 9, 2010·Chemical Reviews·Millicent B Smith, Josef Michl
Jul 16, 2011·Journal of the American Chemical Society·Mark W B WilsonRichard H Friend
Sep 8, 2011·The Journal of Chemical Physics·Alberto GirlandoElisabetta Venuti
Nov 17, 2011·Journal of the American Chemical Society·Paul M ZimmermanMartin Head-Gordon
Dec 2, 2011·The Journal of Chemical Physics·Pengfei Huo, David F Coker
May 17, 2012·The Journal of Physical Chemistry. B·Paul E Teichen, Joel D Eaves
Nov 9, 2012·The Journal of Physical Chemistry. a·Nicolas RenaudMark A Ratner
Dec 1, 2012·The Journal of Physical Chemistry. B·Hajime YamagataFrank C Spano
Jan 5, 2013·The Journal of Physical Chemistry. B·Mahdi ZareaMark A Ratner
Jan 10, 2013·Annual Review of Physical Chemistry·Millicent B Smith, Josef Michl
Mar 29, 2013·The Journal of Chemical Physics·Timothy C BerkelbachDavid R Reichman
Mar 29, 2013·The Journal of Chemical Physics·Timothy C BerkelbachDavid R Reichman
Apr 16, 2013·Accounts of Chemical Research·Wai-Lun ChanX-Y Zhu
Apr 25, 2013·Accounts of Chemical Research·Jiye LeeMarc A Baldo
Sep 10, 2013·Journal of the American Chemical Society·Samuel W EatonMichael R Wasielewski
Nov 22, 2013·Nature Chemistry·Brian J WalkerRichard H Friend
Jan 9, 2014·Journal of the American Chemical Society·Alexey V Akimov, Oleg V Prezhdo
Apr 5, 2014·Journal of the American Chemical Society·Tao ZengNandini Ananth
May 23, 2014·Nature Chemistry·Shane R YostTroy Van Voorhis
Jul 2, 2014·Journal of the American Chemical Society·Erik BusbyOmer Yaffe
Aug 26, 2014·The Journal of Chemical Physics·Timothy C BerkelbachDavid R Reichman
Jan 31, 2015·Physical Review Letters·Juan Aragó, Alessandro Troisi
Feb 5, 2015·Annual Review of Physical Chemistry·N Monahan, X-Y Zhu
Apr 11, 2015·Proceedings of the National Academy of Sciences of the United States of America·Johannes ZirzlmeierDirk M Guldi
Jun 16, 2015·Physical Chemistry Chemical Physics : PCCP·Pengfei Huo, Thomas F Miller
Aug 4, 2015·The Journal of Chemical Physics·Paul E Teichen, Joel D Eaves
Aug 12, 2015·The Journal of Physical Chemistry Letters·Nicolas Renaud, Ferdinand C Grozema
Aug 12, 2015·The Journal of Physical Chemistry Letters·Oleg VarnavskiTheodore Goodson
Aug 12, 2015·The Journal of Physical Chemistry Letters·Geoffrey B Piland, Christopher J Bardeen
May 1, 2014·The Journal of Physical Chemistry Letters·Roel TempelaarThomas L C Jansen
Aug 19, 2015·The Journal of Physical Chemistry Letters·ShuGuang ChenMark A Ratner
Aug 19, 2015·The Journal of Physical Chemistry Letters·Linjun WangDavid Beljonne
Aug 19, 2015·The Journal of Physical Chemistry Letters·Geoffrey B PilandChristopher J Bardeen
Apr 4, 2013·The Journal of Physical Chemistry Letters·Nicolas RenaudMark A Ratner
Sep 24, 2015·Nature Chemistry·Sean T Roberts
Nov 18, 2015·Journal of Chemical Theory and Computation·Guohua Tao

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Citations

Sep 19, 2019·Nature Communications·Christoph SchnedermannAndrew J Musser
Aug 3, 2019·The Journal of Chemical Physics·S Rajagopala ReddyMichael Thoss
Jan 31, 2021·The Journal of Chemical Physics·Sutirtha N ChowdhuryPengfei Huo
Nov 22, 2020·The Journal of Chemical Physics·Jonathan R Mannouch, Jeremy O Richardson
Nov 22, 2020·The Journal of Chemical Physics·Jonathan R Mannouch, Jeremy O Richardson
Jun 27, 2020·The Journal of Physical Chemistry. B·Arkajit MandalPengfei Huo
Apr 10, 2021·The Journal of Physical Chemistry. a·Takanori NagamiMasayoshi Nakano
Sep 3, 2019·The Journal of Physical Chemistry Letters·Arkajit Mandal, Pengfei Huo
Sep 30, 2017·The Journal of Physical Chemistry Letters·Hang ZangWanZhen Liang
Nov 6, 2020·The Journal of Physical Chemistry Letters·Maria Fumanal, Clémence Corminboeuf
Mar 1, 2018·Journal of Chemical Theory and Computation·Arkajit MandalPengfei Huo
Sep 28, 2018·The Journal of Physical Chemistry Letters·S Rajagopala ReddyMichael Thoss

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