J. Terence Blaskovits^1*, Maria Fumanal^1*, Sergi Vela^1*, Raimon Fabregat^1*, Clemence Corminboeuf^1*

1 Laboratory for Computational Molecular Design (LCMD), Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

* Corresponding authors emails: jacob.blaskovits@epfl.ch, maria.fumanal@epfl.ch, sergi.vela@epfl.ch, raimon.fabregat@epfl.ch, clemence.corminboeuf@epfl.ch

DOI10.24435/materialscloud:xj-9d [version v1]

Publication date: Dec 22, 2020

How to cite this record

J. Terence Blaskovits, Maria Fumanal, Sergi Vela, Raimon Fabregat, Clemence Corminboeuf, Identifying the trade-off between intramolecular singlet fission requirements in donor-acceptor copolymers, Materials Cloud Archive 2020.168 (2020), https://doi.org/10.24435/materialscloud:xj-9d

Description

Intramolecular singlet fission (iSF) has shown potential to improve the power conversion efficiency in photovoltaic devices by promoting the splitting of a photon-absorbing singlet exciton into two triplet excitons within a single molecule. Among different possibilities, the donor-acceptor modular strategy of copolymers has shown great promise in its ability to undergo iSF under certain conditions. However, the number of iSF donor-acceptor copolymers reported in the literature remains remarkably narrow and clear trends for the molecular design of better candidates have not yet been established. In this work, we identify the trade-off between the main iSF requirements of the donor-acceptor strategy and formulate design rules that allow them to be tuned simultaneously in a fragment-based approach. Based on a library of 2944 donor-acceptor copolymers, we establish simple guidelines to build promising novel materials for iSF. These consist in (1st) selecting an acceptor core with high intrinsic singlet-triplet splitting, (2nd) locating a donor with a larger monomer frontier molecular orbital (FMO) gap than that of the acceptor, and (3rd) tuning the relative energy of donor and/or acceptor FMOs through functionalization to promote photoinduced charge transfer in the resulting polymer. Remarkably, systems containing benzothiadiazole and thiophene-1,1-dioxide acceptors, which have been shown to undergo iSF, fulfill all criteria simultaneously when paired with appropriate donors. This is due to their particular electronic features, which make them highly promising candidates in the quest for iSF materials.

Materials Cloud sections using this data

Files

File name	Size	Description
relevant_data.csv MD5md5:e1430b211534d3a25ce5d9a033284c1f	1014.8 KiB	Summary of relevant output data used to generate figures and interactive database.
README.txt MD5md5:0e8a3b5e3a138f4bbe59337f93c8530c	1.8 KiB	Readme file with information on the database folder
ALL_DATA_SF_paper_2.tar.bz2 MD5md5:6e82129f6404d296fd1587f8ebdc0053	2.7 GiB	Compressed folder containing all computations reported in the paper

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External references

Keywords

EPFL singlet fission excited states conjugated polymers