Very recently, considerable attention has been given to pure organic circularly polarized room-temperature phosphorescent (CP-RTP) materials due to their unique photophysical properties. However, the directed construction of optically active phosphorescent signals within achiral systems remains a formidable challenge. In this study, two achiral crystals, 2CN4S and 2F4S, belonging to the achiral point groups 2/m and 1¯1, exhibit strong CP-RTP emission with high photoluminescence dissymmetry factors (glum) up to 5. 5 × 10-2 (543 nm) and 4. 3 × 10-2 (550 nm), respectively. This phenomenon is attributed to the intrinsic mirror-antiparallel molecular conformations induced by the targeted substitution of cyano/fluoro groups, which spontaneously assemble into symmetry-breaking helical superstructures through synergistic C─H···N hydrogen bonding and π-π interactions. This work not only establishes a novel approach for CP-RTP material design but also overcomes structural constraints in optically active materials within achiral point group systems.
Li et al. (Mon,) studied this question.
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