Defect induced ferromagnetism in a two-dimensional metal−organic framework

Abstract Two-dimensional ferromagnetic materials are potential candidates that can be integrated with the current nanoelectronic and spintronic device architecture. The latest trends in designing spintronic devices are mainly based on two-dimensional (2D) inorganic compounds. Here, we present a study based on first-principles density functional calculations where we design a 2D ferromagnetic material within the family of metal − organic frameworks. Starting from the inorganic CrI 3 compound, we demonstrate that a chromium-based metal − organic compound i.e. Cr(COOH) 3 can be stabilized in a ferromagnetic state compared to the other possible anti-ferromagnetic states. The proposed structure of Cr(COOH) 3 is found to be thermodynamically stable, but it’s dynamic stability could not be verified because of complexity into the structure. The lowest energy magnetic configuration of pure Cr(COOH) 3 turns out to be antiferromagnetic. However, our calculations suggest that the presence of positively charged Cr-vacancy defects can stabilize the ferromagnetic state over antiferromagnetic orderings. The presence of delocalized holes is found to be responsible for favoring the ferromagnetic ordering.