Herein, structurally regular dendritic trimethylolethane (TME) polyester is robustly obtained by polymerizing with suberic acid. Through properly modeled chain growth behaviors, differences of scaffolds forming between TME and glycerol polyesters are thoroughly discussed. The scaffolds of polyol‐polyesters can be easily controlled by adjusting feed ratio and temperature. However, to achieve regular dendritic scaffolds, apart from the monomer feed ratio of 1/1 and high temperature(80 °C), selection of proper polyols is much more important. TME with three equal primary hydroxyls tends to undergo pure dendritic growth, forming into regular scaffolds while glycerol with secondary hydroxyls is inclined to have linear and grafted growth successively, which results in irregular dendritic scaffolds. However, glycerol polyesters tend to have linear growth under mild temperature (40 °C), hence, regular linear scaffolds can be obtained. Besides, a scaffold determination and control system are built up, giving general guidance of obtaining polol‐polyesters with targeted topologies.

Circularly polarized luminescence (CPL) derived from supramolecular self-assembly chirality has been a fascinating field of research due to its applications in photoactive devices and bioactive probes. Herein, we report a straightforward pathway for the construction of efficient chirality transfer and enhanced circularly polarized phosphorescence based on platinum­(II) metallomesogens via liquid crystal self-organization. Overall, two chiral metallomesogens, the enantiomeric complexes of (S)-Pt-L1 and (R)-Pt-L1, were obtained based on the combination of the rodlike achiral phenylpyridine and point-chiral pyridinic acid derivatives. Experiments with polarizing optical microscopy (POM), differential scanning calorimetry (DSC), and variable-temperature X-ray diffraction show that there are two smectic phases during cooling and heating processes, namely the high temperature SmC* and low temperature SmC phases, and the SmCh* phase. Interestingly, the circular dichroism (CD) and circularly polarized luminescence (CPL) tests reveal that the chirality transfer from the molecule to liquid crystal self-organization does occur indeed in the high temperature SmC* and SmCh* phases. However, both the CD and CPL signals are silent in the low temperature SmC phase, even in the solution, suggesting that chirality transfer depends on the self-organization superstructure of the liquid crystal. Moreover, the dissymmetry factor (|g lum| = 4.0 × 10–2) in the high temperature SmC* phase is 1–2 orders of magnitude higher than that of Pt­(II) complexes previously reported. Also, the elevated photoluminescence quantum yield (ΦPL = 0.46) is obtained for the liquid crystal film, indicating that the enhanced CPL properties can be achieved through self-organization of mesomorphic organoplatinum molecules. Another interesting observation is made that the racemic mixture ((S)-Pt-L1 and (R)-Pt-L1) shows spontaneous chirality separation in the high temperature SmC1 phase.

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Obtaining homochirality from biased symmetry‐breaking of self‐assembly in achiral molecules remains a great challenge due to the lack of ingenious strategies and controlling their handedness. Here, we report the first case of biased symmetry breaking from achiral platinum (II) liquid crystals which self‐organize into an enantiomerically enriched single domain without selection of handedness in twist grain boundary TGB [*] phase. Most importantly, the chiral control of self‐organization can be achieved by using above the homochiral liquid crystal films with determined handedness (P or M) as a template. Moreover, benefiting from self‐assembled superhelix, these complexes exhibit prominent circularly polarized luminescence with high |glum| up to 3.4×10−3 in the TGB [*] mesophase. This work paves a neoteric avenue for the development of chiral self‐assemblies from achiral molecules.

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