AbstractIt is noteworthy that cholesteric liquid crystal (CLC) platforms have been witnessed in high‐performance circularly polarized luminescence (CPL) behaviors through the highly organized chiral co‐assembled arrangement of achiral dyes. However, most CPL‐active design strategies are closely relative to the helix co‐assembly structure of CLC rather than achiral dyes. Herein, we developed an intriguing regulation strategy for CPL‐active CLC materials. They were regulated using the orientational order parameter (SF) of achiral dichroic dyes as an incisive probe for the order arrangement degree of achiral dyes in CLC media. The I‐shaped phenothiazine derivative PHECN dye (SF=0.30) emitted a strong CPL signal (|glum|=0.47). In contrast, the T‐shaped derivative (PHEBen) dye (SF=0.09) showed a weak circular polarization level (|glum|=0.07) at similar CLC textures. Most interestingly, this kind of dichroic PHECN dye with a higher SF could greatly improve the contrast ratio of CPL (Δglum=0.47) and emission intensity (ΔFL=46.0 %) at direct‐current electric field compared with the T‐shaped PHEBen (Δglum=0.07 and ΔFL=1.0 %) in CLC. This work demonstrates that an induced CPL emission can be mediated using achiral dichroic dye, which will open a new avenue for developing excellent CPL‐active display materials.
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