Precise Synthesis of Organic Heterostructures via the Synergy Approach of Polymorphism and Cocrystal Engineering for Optical Applications

Comprehensive Summary Organic heterostructures that can integrate the physiochemical properties of two or more substances have attracted widespread attention in the field of optoelectronics. However, the epitaxial growth process between different organic material molecules is unpredictable, and the precise synthesis of organic heterostructures is still particularly challenging. Herein, through the synergy approach of polymorphism and cocrystal engineering, a series of organic branched heterostructures have been successfully prepared. Interestingly, by simply adjusting the solvent ratio, different crystalline phases of perylene microplates can be epitaxially grown on the perylene‐OFN cocrystal microwires, which provides a feasible approach for the preparation of organic heterostructures. Meanwhile, these as‐prepared organic branched heterostructures can realize multi‐channel and multi‐color emission, and act as optical logic gates, which promotes the multifunctional integrated optoelectronics.