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Organic heterostructures (OHTs) with the desired geometry organization on micro/nanoscale have undergone rapid progress in nanoscience and nanotechnology. However, it is a significant challenge to elucidate the epitaxial-growth process for various OHTs composed of organic units with a lattice mismatching ratio of > 3%, which is unimaginable for inorganic heterostructures. Herein, we have demonstrated a vivid visualization of the morphology evolution of epitaxial-growth based on a doped interfacial-layer, which facilitates the comprehensive understanding of the hierarchical self-assembly of core-shell OHT with precise spatial configuration. Significantly, the barcoded OHT with periodic shells obviously illustrate the shell epitaxial-growth from tips to center parts along the seeded rods for forming the core-shell OHT. Furthermore, the diameter, length, and number of periodic shells were modulated by finely tuning the stoichiometric ratio, crystalline time, and temperature, respectively. This epitaxial-growth process could be generalized to organic systems with facile chemical/structural compatibility for forming the desired OHTs., (© 2024. The Author(s).)

Organic heterostructure nanowires, such as multiblock, core/shell, branch-like and related compounds, have attracted chemists' extensive attention because of their novel physicochemical properties. However, owing to the difficulty in solving the lattice mismatch of distinct molecules, the construction of organic heterostructures at large scale remains challenging, which restricts its wide use in future applications. In this work, we define a concept of lattice-mismatch-free for hierarchical self-assembly of organic semiconductor molecules, allowing for the large-scale synthesis of organic heterostructure nanowires composed of the organic alloys and cocrystals. Thus, various types of organic triblock nanowires are prepared in large scale, and the length ratio of different segments of the triblock nanowires can be precisely regulated by changing the stoichiometric ratio of different components. These results pave the way towards fine synthesis of heterostructures in a large scale and facilitate their applications in organic optoelectronics at micro/nanoscale., (© 2022. The Author(s).)

Rationally designing and precisely constructing the dimensions, configurations and compositions of organic nanomaterials are key issues in material chemistry. Nevertheless, the precise synthesis of organic heterostructure nanomaterials remains challenging owing to the difficulty of manipulating the homogeneous/heterogeneous-nucleation process and the complex epitaxial relationships of combinations of dissimilar materials. Herein, we propose a hierarchical epitaxial-growth approach with the combination of longitudinal and horizontal epitaxial-growth modes for the design and synthesis of a variety of organic superstructure microwires with accurate spatial organisation by regulating the heterogeneous-nucleation crystallisation process. The lattice-matched longitudinal and horizontal epitaxial-growth modes are separately employed to construct the primary organic core/shell and segmented heterostructure microwires. Significantly, these primary organic core/shell and segmented microwires are further applied to construct the core/shell-segmented and segmented-core/shell type's organic superstructure microwires through the implementation of multiple spatial epitaxial-growth modes. This strategy can be generalised to all organic microwires with tailored multiple substructures, which affords an avenue to manipulate their physical/chemical features for various applications.

Organic heterostructures (OHSs) integrating the intrinsic heterostructure characters as well as the organic semiconductor properties have attracted intensive attention in material chemistry. However, the precise bottom-up synthesis of OHSs is still challenging owing to the general occurrence of homogeneous-nucleation and the difficult manipulation of noncovalent interactions. Herein, we present the rational synthesis of the longitudinally/horizontally-epitaxial growth of one-dimensional OHSs including triblock and core/shell nanowires with quantitatively-manipulated microstructure via a hierarchical self-assembly method by regulating the noncovalent interactions: hydrogen bond (-15.66 kcal mol -1 ) > halogen bond (-4.90 kcal mol -1 ) > π-π interaction (-0.09 kcal mol -1 ). In the facet-selective epitaxial growth strategy, the lattice-matching and the surface-interface energy balance respectively facilitate the realization of triblock and core/shell heterostructures. This hierarchical self-assembly approach opens up avenues to the fine synthesis of OHSs. We foresee application possibilities in integrated optoelectronics, such as the nanoscale multiple input/out optical logic gate with high-fidelity signal.