Abstract Achieving magnetic ordering in low‐dimensional materials remains a key objective in the field of magnetism. Herein, coordination chemistry emerges as a powerful discipline to promote the stabilization of magnetism at the nanoscale. We present a thorough study of exemplary two‐dimensional metal‐organic nanoarchitectures synthesized on a Au(111) substrate, which are rationalized by using surface‐science techniques and theoretical calculations. By tuning the stoichiometry, two distinct phases based on the same molecular linker coordinated with Co atoms are obtained, though featuring a different coordination sphere. Remarkably, our combined experimental and theoretical results suggest that for one phase the Co centers have an out‐of‐plane antiferromagnetic ground state, whereas for the other the Co atoms display in‐plane antiferromagnetism. These results pave new avenues for designing two‐dimensional (2D) metal‐organic magnets and tailoring their inherent magnetic properties.
Mathialagan et al. (Wed,) studied this question.