Excitation‐Dependent Circularly Polarized Luminescence from Helical Assemblies Based on Tartaric Acid‐Derived Acylhydrazones

Here, we combined the merits of emergent excitation‐dependent (ExD) emission and circularly polarized luminescence to develop an excitation‐dependent circularly polarized luminescence (ExD CPL) material showing unique features. A series of acylhydrazones based on a chiral tartaric skeleton was designed and found to self‐assemble into helical nanostructures through non‐covalent bonds. The helical assemblies showed ExD CPL due to the cooperation of chirality transfer and excited state intramolecular proton transfer (ESIPT). Remarkably, not only the emission wavelength could be tuned by the excitation wavelength but the handedness of CPL could be modulated in an inverted or ON/OFF manner as well, thus leading to the first example of an ExD inverted or ON/OFF switchable CPL system. Time‐dependent density functional theory (TD‐DFT) calculations were carried out to explain the inversion of ExD CPL. This work provided a new insight into the unprecedented handedness controllable ExD CPL, which showcased a new paradigm of the advanced CPL materials. Helical assemblies based on chiral tartaric acid derived acylhydrazones intriguingly exhibit excitation‐dependent (ExD) emission through modulation between excited‐state intramolecular proton transfer (ESIPT) and excimer emissions. By virtue of chirality transfer during the self‐assembly process, an unprecedented ExD inverted or ON/OFF circularly polarized luminescence (CPL) switch was developed. This type of advanced CPL material can potentially be applicable in higher‐level anti‐counterfeiting and encryption.