Atomic‐Scale Control of Substrate‐Spin Coupling Via Vertical Manipulation of a 2D Metal‐Organic Framework

ABSTRACT Two‐dimensional (2D) materials with frustrated crystal geometries can host strongly correlated electrons, potentially leading to a range of exotic many‐body quantum phases, such as Mott insulators, quantum spin‐liquids, and Kondo lattices. The ability to control exchange‐coupling within these systems is therefore highly desirable. Here, we use an atomically sharp scanning tunneling microscope probe to vertically manipulate a 2D Mott insulating honeycomb‐kagome metal‐organic framework (MOF) featuring Kondo‐screened local magnetic moments on Ag(111). We show that by controlling the adsorption height of the MOF, we can also controllably and reversibly change the strength of Kondo coupling between the MOF's local spins and the substrate's conduction electrons. This mechanical control of Kondo coupling could be extended to other forms of interlayer exchange coupling, potentially allowing for atomic‐scale design or control of spintronics technologies.