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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.

Several new square planar platinum(ii) complexes based on modified 2-phenylpyridine derivatives as the main ligand and picolinic acid as the auxiliary ligand were synthesized and their photophysical properties, and mechanochromic and liquid crystalline behavior were investigated.

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In this paper, we have designed and synthesized a series of neutral liquid-crystalline iridium­(III) complexes based on polycatenar 2,5-diphenylpyridine and pyridyltetrazolate derivatives. Iridium­(III) complexes all display highly emissive behavior with photoluminescence quantum yields in the range of 0.45–0.66 and a maximum emission wavelength at ∼563 nm. Hexagonal columnar mesophases of iridium­(III) complexes can be obtained by changing the number and length of peripheral alkoxyl chains attached to a 2,5-diphenylpyridine ligand (main ligand) and a pyridyltetrazolate ligand (auxiliary ligand). Moreover, experimental results of the charge transport properties for these iridium­(III) complexes, which were measured by the space charge limited-current method, exhibit ambipolar carrier mobility behavior. In particular, the liquid-crystalline iridium­(III) complexes can self-organize into one-dimensional (1D) nanostructure after thermal annealing treatment in their liquid-crystalline phase. The devices based on liquid crystal film display improved charge transport behavior compared with that of the devices based on polycrystalline film, indicating 1D nanostructure is beneficial to charge carrier injection and transportation.