Issue 26, 2021

Influence of the crystal packing in singlet fission: one step beyond the gas phase approximation

Abstract

Singlet fission (SF), a multiexciton generation process, has been proposed as an alternative to enhance the performance of solar cells. The gas phase dimer model has shown its utility to study this process, but it does not always cover all the physics and the effect of the surrounding atoms has to be included in such cases. In this contribution, we explore the influence of crystal packing on the electronic couplings, and on the so-called exciton descriptors and electron–hole correlation plots. We have studied three tetracene dimers extracted from the crystal structure, as well as several dimers and trimers of the α and β polymorphs of 1,3-diphenylisobenzofuran (DPBF). These polymorphs show different SF yields. Our results highlight that the character of the excited states of tetracene depends on both the mutual disposition of molecules and inclusion of the environment. The latter does however not change significantly the interpretation of the SF mechanism in the studied systems. For DPBF, we establish how the excited state analysis is able to pinpoint differences between the polymorphs. We observe strongly bound correlated excitons in the β polymorph which might hinder the formation of the 1TT state and, consequently, explain its low SF yield.

Graphical abstract: Influence of the crystal packing in singlet fission: one step beyond the gas phase approximation

Supplementary files

Article information

Article type
Paper
Submitted
21 Jan 2021
Accepted
09 May 2021
First published
10 May 2021
This article is Open Access
Creative Commons BY-NC license

Phys. Chem. Chem. Phys., 2021,23, 14164-14177

Influence of the crystal packing in singlet fission: one step beyond the gas phase approximation

L. E. Aguilar Suarez, C. de Graaf and S. Faraji, Phys. Chem. Chem. Phys., 2021, 23, 14164 DOI: 10.1039/D1CP00298H

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