Vertical-assembly of two-dimensional organic crystals with stacked architectures towards interlayer coupling emission.

The precise fabrication of two-dimensional heterostructures, especially vertical heterostructures, is essential for advanced applications but faces significant challenges. Vapor-deposition epitaxial growth is an efficient preparation strategy to produce large-scale and high-quality heterostructures, yet is still limited by uncontrollable epitaxial kinetics and interface defects. Here, we report a fast vapor-deposition strategy to drive vertical-assembly of organic crystals for fabricating twisted vertical heterostructures (TVHs). It is found that precise tuning of deposition temperature enables controllable selection of the vertical epitaxial form. In particular, the high-matching growth modes and the compatible lattice of organic crystals simultaneously improve the yield of TVHs. The twisted stacked architectures combined with anisotropic polarization properties endow interlayer coupling emission with tunable color. This work provides an effective strategy for the kinetic control of vertical heteroepitaxy, and also lays the material preparation foundation for practical modules of integrating photonics.