Designer spin order in diradical nanographenes

TL;DR

This paper presents a method to control magnetic ground states in nanographenes by breaking bipartite symmetry and tuning spin density overlap, enabling designer magnetic phases potentially useful for spintronics and quantum computing.

Contribution

It introduces a novel approach combining scanning probe techniques and Hubbard model calculations to engineer magnetic coupling in nanographenes.

Findings

Controlled magnetic coupling sign by symmetry breaking.

Achieved large exchange interaction of 42 meV.

Potential for above-room-temperature magnetic phases.

Abstract

The magnetic properties of carbon materials are at present the focus of an intense research effort in physics, chemistry and materials science due to their potential applications in spintronics and quantum computations. Although the presence of spins in open-shell nanographenes has been recently confirmed, the ability to control magnetic coupling sign has remained elusive, but the most desirable. Here, we demonstrate an effective approach of engineering magnetic ground states in atomically precise open-shell bipartite/nonbipartite nanographenes using combined scanning probe techniques and mean-field Hubbard model calculations. The magnetic coupling sign between two spins has been controlled via breaking bipartite lattice symmetry of nanographenes. In addition, the exchange-interaction strength between two spins has been widely tuned by finely tailoring their spin density overlap, realizing a large exchange-interaction strength of 42 meV. Our demonstrated method provides ample opportunities for designer above-room-temperature magnetic phases and functionalities in graphene nanomaterials.