Maria Fumanal^1*, Clemence Corminboeuf^1*

1 Laboratory for Computational Molecular Design, Institute of Chemical Sciences and Engineering, EPFL, CH-1015 Lausanne, Switzerland

* Corresponding authors emails: maria.fumanal@epfl.ch, clemence.corminboeuf@epfl.ch

DOI10.24435/materialscloud:gg-1s [version v1]

Publication date: Mar 23, 2022

How to cite this record

Maria Fumanal, Clemence Corminboeuf, Optimizing the thermodynamics and kinetics of the triplet-pair dissociation in donor-acceptor copolymers for intramolecular singlet fission, Materials Cloud Archive 2022.43 (2022), https://doi.org/10.24435/materialscloud:gg-1s

Description

Singlet fission (SF) is a two-step process in which a singlet splits into two triplets throughout the so-called correlated triplet-pair (1TT) state. Intramolecular SF (iSF) materials in particular, have attracted growing interest as they can be easily implemented in single junction solar cells and boost their power conversion efficiency. Still, the potential of iSF materials such as polymers and oligomers for photovoltaic applications has been partially hindered by their ability to go beyond the 1TT intermediate and generate free triplets, which mechanism remains poorly understood. In this work, the main aspects governing the 1TT dissociation in donor-acceptor copolymers and the key features that optimize this process are exposed. First, we show that both thermodynamics and kinetics play a crucial role in the intramolecular triplet-pair separation and second, we uncover the inherent flexibility of the donor unit as the fundamental ingredient to optimize them simultaneously. Overall, these results provide a better understanding of the intramolecular 1TT dissociation process and establish a new paradigm for the development of novel iSF active materials.

Materials Cloud sections using this data

Files

File name	Size	Description
Database3.tar.gz MD5md5:cecc141d9e9269d7bc26aca0a7b9c9ae	2.8 GiB	The compressed folder contains all the computations reported in the paper
readme3.txt MD5md5:938f98fd59ec925208d7cc307a0819a6	2.3 KiB	Readme file with the information of the database folder

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External references

Keywords

singlet fission donor-acceptor copolymers electronic structure EPFL Marie Curie Fellowship H2020