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Considerable luminescence dissymmetry factor (g lum) is vital for application implementation of circularly polarized luminescence (CPL) materials. Moreover, a dual CPL switch has promising prospects in high-security encryption and sensor devices. Herein, we designed and synthesized an emissive chiral nematic liquid crystal (N*-LC) by doping a luminescent chiral additive (NO2-CS-C6-Chol) into a nematic liquid crystal (5CB). The helical assembly structure produced by inducing the formation of N*-LC endows the prepared emissive N*-LC with a larger g lum value. With the increase of the doping concentration from 1 to 10 wt %, the helical pitch (P) of N*-LC gradually decreases from 25.48 to 3.92 μm. The corresponding g lum value increases first, reaches the maximum value (−0.38) at 6 wt %, and then decreases slightly. Further, the prepared emissive N*-LC doped with 6 wt % NO2-CS-C6-Chol is injected into an indium-tin oxide (ITO)-coated LC cell, to which a direct current (DC) electric field is applied. The g lum value can be repeatedly shuttled between the “on” and “off” state by adjusting the applied voltage. Meanwhile, owing to the inherent thermal dependence of the liquid crystal phase structure, the g lum value can also be switched between the on and off state by regulating the temperature. Therefore, an electrically controlled and thermocontrolled dual CPL switching device is successfully constructed.

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