Development of organic molecules that can harvest triplet excitons under ambient conditions by a relatively simple strategy holds great promise in the paradigm of photophysics. Deploying through-space charge transfer (CT) interactions via noncovalently stacked donor–acceptor molecular design that can be tuned in accordance with simple structural modifications can be considered an attractive strategy toward this direction. Herein, we accomplish a precise control in tuning the triplet harvesting pathways in donor–acceptor cocrystals by engineering CT complexation between them. We use pyromellitic diimide (PmDI) phosphor to cocrystallize with different donors such as dibenzofuran (DBF), dibenzothiophene (DBT), and dibenzoselenophene (DBS) that augment CT complexation between the two counterparts and carefully toggle the emission into singlet CT (¹CT) fluorescence, thermally activated delayed fluorescence (TADF), and triplet CT (³CT) phosphorescence, in their respective cocrystals. On moving from PmDI-DBF to PmDI-DBT, emission was biased from ¹CT fluorescence to TADF. The synergistic involvement of the strong heavy-atom effect with CT complexation diverts the excited emission from TADF to exclusively ³CT phosphorescence in PmDI-DBS. Most crucially, we not only put forward a methodology for biasing the excited state to various ambient triplet harvesting pathways but also glorify a modular noncovalent donor–acceptor strategy without complicated synthetic efforts unlike conventional covalent donor–acceptor molecular designs.

中文翻译：

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通过模块化非共价电荷转移相互作用释放亚芳基二酰亚胺中的环境三重态收获途径

通过相对简单的策略开发能够在环境条件下收获三重态激子的有机分子在光物理学范式中具有巨大的前景。通过非共价堆叠的供体-受体分子设计来部署空间电荷转移（CT）相互作用，可以根据简单的结构修饰进行调整，可以被认为是朝着这个方向发展的一个有吸引力的策略。在此，我们通过设计供体-受体共晶之间的 CT 络合来实现对供体-受体共晶中三重态收获途径的精确控制。我们使用均苯四甲酸二酰亚胺 ( PmDI ) 荧光粉与不同的供体共结晶，例如二苯并呋喃 ( DBF )、二苯并噻吩 ( DBT ) 和二苯并硒吩 ( DBS)），增强两个对应物之间的 CT 络合，并在各自的共晶中小心地将发射切换为单线态 CT ( ¹ CT) 荧光、热激活延迟荧光 (TADF) 和三线态 CT ( ^{3 CT) 磷光。}从PmDI-DBF转移到PmDI-DBT时，发射从¹ CT 荧光偏向 TADF。强重原子效应与 CT 络合的协同作用将 TADF 的激发发射转移到PmDI-DBS中的³ CT 磷光。最重要的是，我们不仅提出了一种将激发态偏向于各种环境三重态收获途径的方法，而且还美化了模块化非共价供体-受体策略，而无需与传统共价供体-受体分子设计不同的复杂合成工作。