ArticleAngewandte Chemie (International ed. in English)2026
Intramolecular Charge-Transfer Dopants Enable Isolated Triplet Excitons as Spin Qutrits in a Single Crystal.
Article in Angewandte Chemie (International ed. in English), 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Organic molecular crystals enable spin alignment of triplet excitons over macroscopic distances, offering a molecular route to solid-state quantum technologies. In typical crystals, however, dense packing promotes spin decoherence through dipolar coupling and exciton hopping. Although dilution doping can mitigate these effects, reported examples remain scarce because dopants must satisfy stringent structural and energetic constraints. Here, we broaden the design space for doped organic crystals by introducing a strategy that employs a host-derived dopant with intramolecular charge-transfer (ICT) character that maintains structural compatibility with the host lattice, while its ICT character lowers the triplet energy to localize triplet excitons. Ultrafast transient absorption spectroscopy confirms triplet formation, while time-resolved electron paramagnetic resonance (TREPR) spectroscopy reveals that these oriented triplets possess selectively addressable spin sublevel transitions. Additionally, pulse-EPR measurements yield a phase memory time (T
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