Mukhopadhyay, T., Musser, A.J. orcid.org/0000-0002-4600-6606, Puttaraju, B. et al. (3 more authors) (2017) Is the Chemical Strategy for imbuing ‘Polyene’ Character in Diketopyrrolopyrrole Based Chromophores sufficient for Singlet Fission? Journal of Physical Chemistry Letters. ISSN 1948-7185
Abstract
In this work, we have rationally designed and synthesized a novel thiophene-diketopyrrolopyrrole (TDPP)-vinyl based dimer. We have investigated the optical and electronic properties and have probed the photophysical dynamics using transient absorption to investigate the possibility of singlet exciton fission. These revealed extremely rapid decay to the ground state (< 50 ps), which we confirm is due to intramolecular excitonic processes rather than large-scale conformational change enabled by the vinyl linker. In all cases the main excited state appears to be ‘dark’, suggesting rapid internal conversion into a dark 2Ag-type singlet state. We found no evidence of triplet formation in TDPP-V-TDPP under direct photo excitation. This may be a consequence of significant singlet stabilization in the dimer, bringing it below the energy needed to form two triplets. Our studies on this model compound set valuable lessons for design of novel triplet-forming materials, and highlight the need for more broadly applicable design principles.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2017 American Chemical Society. This is an author produced version of a paper subsequently published in Journal of Physical Chemistry Letters . Uploaded in accordance with the publisher's self-archiving policy. |
Keywords: | singlet fission; donor-acceptor; viny; DPP; polyene; internal conversion; transient absorption |
Dates: |
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Institution: | The University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Science (Sheffield) > Department of Physics and Astronomy (Sheffield) |
Depositing User: | Symplectic Sheffield |
Date Deposited: | 09 Feb 2017 14:54 |
Last Modified: | 23 Jan 2018 01:38 |
Published Version: | https://doi.org/10.1021/acs.jpclett.6b02919 |
Status: | Published |
Publisher: | American Chemical Society |
Refereed: | Yes |
Identification Number: | 10.1021/acs.jpclett.6b02919 |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:112152 |