Programmed Twisting in Organic Lateral Heterostructures Driven by a Metastable Crystal Plane

The precise preparation of twisted heterostructures is crucial for optoelectronic applications; however, it remains a significant challenge of precise twist angle control. Here, we report a vapor-phase diffusion-based strategy for the direct growth of organic twisted lateral heterostructures (TLHs) with programmed twist angles. By leveraging distinct melting points of precursor materials and exploiting selective matching of metastable crystal facets, we achieved heteroepitaxial growth with an accurate 45° twisted angle. The ordered and controllable direct epitaxial process of organic crystals driven by high lattice matching induction is simple, efficient, and avoids the introduction of external pollution. The resulting TLHs exhibit excellent structural integrity and uniformity while maintaining superior optical waveguide properties. Furthermore, we demonstrate their potential for optical signal modulation through comprehensive photoconduction characterization. This work establishes a facet-selected epitaxy approach for precise fabrication of twisted architectures and provides a versatile platform for advanced twistronic and photonic applications.