alexa A microscopic model of singlet fission.


Journal of Lasers, Optics & Photonics

Author(s): Teichen PE, Eaves JD

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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. This article was published in J Phys Chem B and referenced in Journal of Lasers, Optics & Photonics

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