Two-Dimensional Wedge-Shaped Magnetic EuS: Insight into the Substrate Step-Guided Epitaxial Synthesis on Sapphire

Rare earth chalcogenides (RECs) with novel luminescence and magnetic properties offer fascinating opportunities for fundamental research and applications. However, controllable synthesis of RECs down to the two-dimensional (2D) limit still has a great challenge. Herein, 2D wedge-shaped ferromagnetic EuS single crystals are successfully synthesized via a facile molten-salt-assisted chemical vapor deposition method on sapphire. Based on the theoretical simulations and experimental measurements, the mechanisms of aligned growth and wedge-shaped growth are systematically proposed. The wedge-shaped growth is driven by a dual-interaction mechanism, where the coupling between EuS and the substrate steps impedes the lateral growth, and the strong bonding of nonlayered EuS itself facilitates the vertical growth. Through temperature-dependent Raman and photoluminescence characterization, the nanoflakes show a large Raman temperature coefficient of -0.030 cm^-1 K^-1 and uncommon increasing band gap with temperature. More importantly, by low-temperature magnetic force microscopy characterization, thickness variation of the magnetic signal is revealed within one sample, indicating the great potential of the wedge-shaped nanoflake to serve as a platform for highly efficient investigation of thickness-dependent magnetic properties. This work sheds new light on 2D RECs and will offer a deep understanding of 2D wedge-shaped materials.