Development of circularly polarized luminescent (CPL) materials with strong emission and high dissymmetry factor of luminescence (g lum) is highly desirable. A series of CPL-active aggregation-induced emission luminogens (AIEgens) have been successfully constructed by incorporating AIEgen dicyanodistyrylbenzene (DCS) into chiral molecule cholesterol. Benefiting from its typical AIE characteristic, DCS allows emission efficiency up to 73.7% in a condensed state. Furthermore, cholesterol units ensure forming chiral liquid crystal in syntax, and increasing the g lum value of CPL from 7 × 10–4 for the amorphous state to 1.1 × 10–1 for the liquid crystal state. This approach paves a general avenue for addressing the major defect well: high g lum always suffers from suppression of emission efficiency.

A luminescent liquid crystal molecule (TPEMes) with efficient solid-state emission is rationally constructed via the chemical conjugation of blue-emitting tetraphenylethene cores and luminescent mesogenic tolane moieties, which are both featured with aggregation-induced emission properties. As for this fluorophore, aggregation-induced energy transfer from the emissive tolane mesogens to the lighting-up tetraphenylethene units endows the molecule pure blue emission in the suspension and bulk state. Combining differential scanning calorimetry, polarized optical microscope, and one-dimensional X-ray diffraction (1D XRD) experiments, the compound TPEMes is deduced to adapt thermodynamically more stable layered crystalline phase and can be “frozen” into a monotropic smectic mesophase due to kinetic reasons. As a result of more dense packing of TPEMes in the crystalline phase indicated by 1D XRD, the luminescence of TPEMes in crystalline phase blue-shifted by 17 nm relative to the metastable mesophase.

Precisely controlling the circularly polarized emission of achiral organic luminescent molecules in an aggregated state is a remaining challenge in this research field, since it should simultaneously overcome the ubiquitous issues of chirality transfer and aggregation‐caused quenching occurring in the aggregated systems. Herein, a facile and universal approach to achieving assembly‐accelerated photocyclization and photocyclization‐enhanced emission of tetraphenylethylene (TPE) derivative in the gel state is reported. This experimental data reveal that the co‐assembled gels exhibit high efficiency of photocyclization (≥100 times more efficient than the TPE‐based derivative in solution) via the hydrogen‐bonding‐driven helical assembly, displaying sharply enhanced emission (with the maximum enhancement of 105 times) after the photocyclization and oxidation under ultraviolet irradiation. Furthermore, inverted circularly polarized luminescence (CPL) is achieved after the photocyclization of TPE‐based gels. The strategy of assembly‐enhanced emission and photomodulated CPL inversion of fluorescent organic systems in the aggregated state can increase the abundance of chiral luminescent soft matters, leading to versatile applications in organic chiroptical optoelectronics and smart flexible displaying devices.

A temperature-sensitive Förster resonance energy transfer system was constructed using a highly emissive liquid crystal co-assembled with Nile red, enabling thermo-optical modulation for controlling and directing light in stimuli-responsive devices.

The study of dynamic supramolecular chirality inversion (SMCI) not only helps to deepen the understanding of chiral transfer and amplification in both living organizations and artificially chemical self-assembly systems but also is useful for the development of smart chiral nanomaterials. However, it is still challenging to achieve the dynamic SMCI of the self-aggregation of metal–organic supramolecular polymers with great potential in asymmetric synthesis, chiroptical switches, and circular polarized luminescence. Here, we successfully developed a hierarchical coassembly system based on the mPAzPCC and various metal ions with effective chirality transfer and temporal-controlled SMCI. Due to the dynamic self-assembly and hierarchical chirality transfer of the Ag+/mPAzPCC complex driven by metallophilic interaction and coordination, morphological transition with nanoribbons, helical nanoribbons, and chiral nanotubules was successively obtained. Interestingly, the SMCI of chiral nanoaggregates was precisely regulated by solvents and metal ions in the Cu2+/mPAzPCC and Mn2+/mPAzPCC system. Besides, temporal-controlled dynamic SMCI switching from helix to bundled helix was clearly revealed in the aggregation of Cu2+/mPAzPCC, Mn2+/mPAzPCC, and Bi3+/mPAzPCC systems. This work provides a metallophilic interaction-mediated helical assembly pathway to dynamically modulate the chirality of metal–organic complex-based assemblies and deepen the understanding of the hierarchically dynamic self-assembly process, which would be of great potential in metal ion-mediated supramolecular asymmetric catalysis and bioinspired chiral sensing.