Layer-by-layer connection for large area single crystal boron nitride multilayer films

Boron nitride (BN) is today considered as one of the most promising materials for many novel applications including bright single photon emission, deep UV opto-electronics, small sized solid-state neutron detector, and high-performance two-dimensional materials, etc. Despite the recent successful fabrication of large-area BN single-crystals (typically <= 5 atomic layers), the scalable growth of thicker single-crystalline BN films still constitutes a great challenge. In this work, we demonstrate an approach to grow large-area multilayer single-crystal BN films by chemical vapor deposition on face-centered cubic Fe-Ni (111) single crystal alloy thin films with different stoichiometric phases. We show that the BN growth is greatly tunable and improved by increasing the Fe content in single-crystal Fe-Ni (111). The formation of pyramid-shaped multilayer BN domains with aligned orientation enables a continuous connection following a layer-by-layer, 'first-meet-first-connect', mosaic stitching mechanism. By means of selected area electron diffraction, micro-photoluminescence spectroscopy in the deep UV and high-resolution transmission electron microscopy, the layer-by-layer connection mechanism is unambiguously evidenced, and the stacking order has been verified to occur as unidirectional AB and ABC stackings, i.e., in the Bernal and rhombohedral BN phase.