Excitation-Dependent Circularly Polarized Luminescence Inversion Driven by Dichroic Competition of Achiral Dyes in Cholesteric Liquid Crystals

Abstract

The development of stimuli-responsive chiral cholesteric liquid crystals (CLCs) materials holds significant potential for achieving three-dimensional (3D) anti-counterfeiting and multi-level information encryption. However, constructing phototunable CLCs systems with easy fabrication and fast response remains a great challenge. Herein, we exploit an excitation-dependent CLCs (ExD-CLCs) material by establishing dynamically photoresponsive dichroic competition between two achiral dyes: a negative dichroic dye (SP-COOH) and a positive dichroic dye (Nile Red, NR) within a CLCs medium. The ExD-CLCs exhibits a negative CPL signal (glum = -0.16) at 650 nm when excited at 365 nm. Remarkably, under excitation at 430 nm, the CPL signal is inverted, and the glum value increases to +0.26. Notably, the helical superstructure and handedness of the ExD-CLCs remain unchanged during this reversal process. The CPL signal reversal is driven by the dichroic competition between the SP-COOH dimer, which displays strong negative dichroism in its open-ring isomer form and silent negative dichroism in its closed-ring isomer form, and the NR dye, which exhibits static positive dichroism. Leveraging these excitation-dependent CPL properties, the quadruplex numerical anti-counterfeiting using ExD-CLCs is achieved.