Quantum spin-engineering in on-surface molecular ferrimagnets

Abstract

The design and control of atomic-scale spin structures constitute major challenges for spin-based quantum technology platforms, including quantum dots, color centers, and molecular spins. Here, we showcase a strategy for designing the quantum properties of molecular spin qubits by combining tip-assisted on-surface assembly with electron spin resonance scanning tunneling microscopy (ESR-STM): We fabricate magnetic dimer complexes that consist of an iron phthalocyanine (FePc) molecule and an organometallic half-sandwich complex formed by the FePc ligand and an attached iron atom, Fe(C<inf>6</inf>H<inf>6</inf>). The total complex forms a mixed-spin (1/2,1) quantum ferrimagnet with a well-separated correlated ground state doublet, which we utilize for coherent control. As a result of the correlation, the quantum ferrimagnet shows an improved spin lifetime (> 1.5 μs) as it is partially protected against inelastic electron scattering. Lastly, the ferrimagnet units also enable intermolecular coupling, that can be used to realize both ferromagnetic or antiferromagnetic structures. Thus, quantum ferrimagnets provide a versatile platform to improve coherent control in general and to study complex magnetic interactions. © The Author(s) 2025.