Reversible gating of singlet fission by tuning the role of a charge-transfer state
Abstract Stimulus-responsive triplet excited states and multiexcitonic logic gates have garnered increasing interest. Singlet fission is an efficient multiple exciton generation process, in which one singlet converts into two triplets. Singlet fission is, however, rarely reported to be switchable by...
Saved in:
| Main Authors: | , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-03-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-58168-9 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1850208486388924416 |
|---|---|
| author | Yifan Bo Yuxuan Hou Dominic A. X. Lavergne Timothy Clark Michael J. Ferguson Rik R. Tykwinski Dirk M. Guldi |
| author_facet | Yifan Bo Yuxuan Hou Dominic A. X. Lavergne Timothy Clark Michael J. Ferguson Rik R. Tykwinski Dirk M. Guldi |
| author_sort | Yifan Bo |
| collection | DOAJ |
| description | Abstract Stimulus-responsive triplet excited states and multiexcitonic logic gates have garnered increasing interest. Singlet fission is an efficient multiple exciton generation process, in which one singlet converts into two triplets. Singlet fission is, however, rarely reported to be switchable by external stimuli. Here we design a meta-diethynylphenylene-linked tetracene dimer featuring pyridyl endgroups that function as an acid/base-responsive switch, enabling the reversible modulation of singlet fission. In its neutral form, the interchromophore charge-transfer state facilitates singlet fission and promotes the formation of a correlated triplet-pair state. Upon treatment with acid, protonation of the pyridyl nitrogens generates a more strongly electron-accepting pyridinium, leading to an intra-chromophore charge-transfer state, which inhibits singlet fission. Finally, an IMPLICATION logic gate is constructed by using acid and base as inputs and monitoring the formation of triplet excited states based on singlet fission. |
| format | Article |
| id | doaj-art-9e0e380e309b450bb57f6c55ae30dc2c |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-03-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-9e0e380e309b450bb57f6c55ae30dc2c2025-08-20T02:10:14ZengNature PortfolioNature Communications2041-17232025-03-0116111210.1038/s41467-025-58168-9Reversible gating of singlet fission by tuning the role of a charge-transfer stateYifan Bo0Yuxuan Hou1Dominic A. X. Lavergne2Timothy Clark3Michael J. Ferguson4Rik R. Tykwinski5Dirk M. Guldi6Department of Chemistry and Pharmacy & Interdisciplinary Center for Molecular Materials (ICMM), FAU Profile Center Solar, Friedrich-Alexander-Universität Erlangen-NürnbergDepartment of Chemistry, University of AlbertaDepartment of Chemistry, University of AlbertaDepartment of Chemistry and Pharmacy & Computer-Chemie-Center (CCC), Friedrich-Alexander-Universität Erlangen-NürnbergDepartment of Chemistry, University of AlbertaDepartment of Chemistry, University of AlbertaDepartment of Chemistry and Pharmacy & Interdisciplinary Center for Molecular Materials (ICMM), FAU Profile Center Solar, Friedrich-Alexander-Universität Erlangen-NürnbergAbstract Stimulus-responsive triplet excited states and multiexcitonic logic gates have garnered increasing interest. Singlet fission is an efficient multiple exciton generation process, in which one singlet converts into two triplets. Singlet fission is, however, rarely reported to be switchable by external stimuli. Here we design a meta-diethynylphenylene-linked tetracene dimer featuring pyridyl endgroups that function as an acid/base-responsive switch, enabling the reversible modulation of singlet fission. In its neutral form, the interchromophore charge-transfer state facilitates singlet fission and promotes the formation of a correlated triplet-pair state. Upon treatment with acid, protonation of the pyridyl nitrogens generates a more strongly electron-accepting pyridinium, leading to an intra-chromophore charge-transfer state, which inhibits singlet fission. Finally, an IMPLICATION logic gate is constructed by using acid and base as inputs and monitoring the formation of triplet excited states based on singlet fission.https://doi.org/10.1038/s41467-025-58168-9 |
| spellingShingle | Yifan Bo Yuxuan Hou Dominic A. X. Lavergne Timothy Clark Michael J. Ferguson Rik R. Tykwinski Dirk M. Guldi Reversible gating of singlet fission by tuning the role of a charge-transfer state Nature Communications |
| title | Reversible gating of singlet fission by tuning the role of a charge-transfer state |
| title_full | Reversible gating of singlet fission by tuning the role of a charge-transfer state |
| title_fullStr | Reversible gating of singlet fission by tuning the role of a charge-transfer state |
| title_full_unstemmed | Reversible gating of singlet fission by tuning the role of a charge-transfer state |
| title_short | Reversible gating of singlet fission by tuning the role of a charge-transfer state |
| title_sort | reversible gating of singlet fission by tuning the role of a charge transfer state |
| url | https://doi.org/10.1038/s41467-025-58168-9 |
| work_keys_str_mv | AT yifanbo reversiblegatingofsingletfissionbytuningtheroleofachargetransferstate AT yuxuanhou reversiblegatingofsingletfissionbytuningtheroleofachargetransferstate AT dominicaxlavergne reversiblegatingofsingletfissionbytuningtheroleofachargetransferstate AT timothyclark reversiblegatingofsingletfissionbytuningtheroleofachargetransferstate AT michaeljferguson reversiblegatingofsingletfissionbytuningtheroleofachargetransferstate AT rikrtykwinski reversiblegatingofsingletfissionbytuningtheroleofachargetransferstate AT dirkmguldi reversiblegatingofsingletfissionbytuningtheroleofachargetransferstate |