Bo Yifan, Hou Yuxuan, Lavergne Dominic A X, Clark Timothy, Ferguson Michael J, Tykwinski Rik R, Guldi Dirk M
Department of Chemistry and Pharmacy & Interdisciplinary Center for Molecular Materials (ICMM), FAU Profile Center Solar, Friedrich-Alexander-Universität Erlangen-Nürnberg, Erlangen, Germany.
Department of Chemistry, University of Alberta, Edmonton, AB, Canada.
Nat Commun. 2025 Mar 26;16(1):2968. doi: 10.1038/s41467-025-58168-9.
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.
对刺激有响应的三重态激发态和多激子逻辑门已引起越来越多的关注。单线态裂变是一种高效的多激子产生过程，其中一个单线态转化为两个三线态。然而，很少有报道称单线态裂变可通过外部刺激进行切换。在这里，我们设计了一种以吡啶基端基为特征的间二乙炔基苯连接的并四苯二聚体，其作为酸/碱响应开关，能够对单线态裂变进行可逆调制。在其中性形式下，发色团间电荷转移态促进单线态裂变并促进相关三线态对态的形成。用酸处理后，吡啶氮的质子化产生更强的电子接受体吡啶鎓，导致发色团内电荷转移态，从而抑制单线态裂变。最后，通过使用酸和碱作为输入并基于单线态裂变监测三线态激发态的形成，构建了一个蕴含逻辑门。
