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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 <i>meta</i>-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.

刺激响应三重激发态（stimulus-responsive triplet excited states）与多激子逻辑门（multiexcitonic logic gates）日益受到学界关注。单重态裂变（Singlet Fission）是一类高效的多激子生成过程，即一个单重态可转化为两个三重态。然而，目前鲜有报道表明单重态裂变可通过外部刺激实现开关调控。本研究设计了一种以间位（meta）二乙炔基亚苯基（diethynylphenylene）连接、带有吡啶基端基（pyridyl endgroups）的并四苯二聚体（tetracene dimer），其端基可作为酸碱响应开关（acid/base-responsive switch），实现对单重态裂变的可逆调控。在中性状态下，发色团间电荷转移态（interchromophore charge-transfer state）可促进单重态裂变，并推动关联三重态对态（correlated triplet-pair state）的形成。经酸处理后，吡啶氮原子发生质子化（protonation），生成电子接受能力更强的吡啶鎓（pyridinium）基团，进而形成发色团内电荷转移态（intra-chromophore charge-transfer state），抑制单重态裂变。最后，本研究以酸与碱作为输入信号，基于单重态裂变介导的三重激发态生成情况进行监测，构建了蕴含逻辑门（IMPLICATION logic gate）。