Integration of Bulk and Thin Film Growth Techniques for Novel Quantum Material Synthesis

The recent remarkable advancement of computational algorithms to predict novel quantum materials^1,2 strongly calls for a parallel expansion of experimental capabilities to synthesize these predicted structures. This naturally motivates the development of new synthesis techniques which can help accelerate the discovery of novel quantum materials. Here, we propose a new, easy-to-implement synthesis approach which combines the conventional bulk and thin film growth techniques in a unique way. This approach enables controlled (de-)intercalation of ions within an epitaxial framework akin to soft chemistry methods but at much elevated temperatures, thus establishing an unusual energetic landscape conducive to single-crystal stabilization of novel materials. Remarkably, even within a narrowly explored growth parameter space we identify and experimentally confirm by x-ray diffraction and scanning transmission electron microscopy multiple new crystal structures, demonstrating the power of this novel synthesis technique. The details of this technique along with the structural nature of the newly identified phases will be discussed.

1. Butler, K. T., Davies, D. W., Cartwright, H., Isayev, O. & Walsh, A., Nature 559, 547–555 (2018).

2. Merchant, A. et al., Nature 624, 80–85 (2023).