A microscopic model of singlet fission

The Journal of Physical Chemistry. B
Paul E Teichen, Joel D Eaves

Abstract

Singlet fission, where an electronically excited singlet on one chromophore converts into a doubly excited state on two, has gone from a curiosity in organic photophysics to a potential pathway for increasing solar energy conversion efficiencies. Focusing on the role of solvent-induced energy level fluctuations that would be present in a dye-sensitized solar cell, we present a microscopic model for singlet fission. Starting from an electronic model Hamiltonian, we construct diabatic states in a manifold of single and double excitations with total singlet multiplicity and then develop a multilevel non-Markovian theory of dynamics for electronic populations in the presence of energy level fluctuations. Depending on the energy scales, energy gap fluctuations can either facilitate or hinder interconversion steps that lead to singlet fission. We critically assess the Markovian approximation that leads to golden rule rates and study the role of intramolecular solvation dynamics and electron transfer.

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Citations

Apr 16, 2013·Accounts of Chemical Research·Wai-Lun ChanX-Y Zhu
Sep 10, 2013·Journal of the American Chemical Society·Samuel W EatonMichael R Wasielewski
Apr 5, 2014·Journal of the American Chemical Society·Tao ZengNandini Ananth
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
Dec 10, 2013·Annual Review of Physical Chemistry·Christopher J Bardeen
Aug 26, 2014·The Journal of Chemical Physics·Timothy C BerkelbachDavid R Reichman
Jan 10, 2013·Annual Review of Physical Chemistry·Millicent B Smith, Josef Michl
Jan 7, 2016·The Journal of Physical Chemistry Letters·Yuta Fujihashi, Akihito Ishizaki
Oct 28, 2015·The Journal of Physical Chemistry Letters·Niels H Damrauer, Jamie L Snyder
Aug 4, 2015·The Journal of Chemical Physics·Paul E Teichen, Joel D Eaves
Nov 18, 2015·Journal of Chemical Theory and Computation·David Casanova
Jul 9, 2016·The Journal of Chemical Physics·Hsing-Ta ChenDavid R Reichman
Apr 11, 2015·Proceedings of the National Academy of Sciences of the United States of America·Johannes ZirzlmeierDirk M Guldi
Aug 12, 2015·The Journal of Physical Chemistry Letters·Steven E Strong, Joel D Eaves
Feb 5, 2015·Annual Review of Physical Chemistry·N Monahan, X-Y Zhu
Aug 12, 2015·The Journal of Physical Chemistry Letters·Nicolas Renaud, Ferdinand C Grozema
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