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  4. Identifying the Trade-off between Intramolecular Singlet Fission Requirements in Donor-Acceptor Copolymers
 
research article

Identifying the Trade-off between Intramolecular Singlet Fission Requirements in Donor-Acceptor Copolymers

Blaskovits, J. Terence
•
Fumanal, Maria  
•
Vela, Sergi
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April 13, 2021
Chemistry Of Materials

Intramolecular singlet fission (iSF) has shown Or potential to improve the power conversion efficiency in photo-voltaic 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 of (first) selecting an acceptor core with high intrinsic singlet-triplet splitting, (second) locating a donor with a larger monomer frontier molecular orbital (FMO) gap than that of the acceptor, and (third) 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.

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Type
research article
DOI
10.1021/acs.chemmater.1c00057
Web of Science ID

WOS:000640650800031

Author(s)
Blaskovits, J. Terence
Fumanal, Maria  
Vela, Sergi
Fabregat, Raimon  
Corminboeuf, Clemence  
Date Issued

2021-04-13

Publisher

AMER CHEMICAL SOC

Published in
Chemistry Of Materials
Volume

33

Issue

7

Start page

2567

End page

2575

Subjects

Chemistry, Physical

•

Materials Science, Multidisciplinary

•

Chemistry

•

Materials Science

•

pi-conjugated polymers

•

molecular design

•

solar-cells

•

fluorescence

•

fluorination

•

strategy

•

impact

•

states

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCMD  
Available on Infoscience
May 22, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/178167
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