Quantum spin-engineering in on-surface molecular ferrimagnets

Wantong Huang, Máté Stark, Paul Greule, Kwan Ho Au-Yeung, Daria Sostina, José Reina Gálvez, Christoph Sürgers, Wolfgang Wernsdorfer, Christoph Wolf and Philip Willke ()
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Wantong Huang: Karlsruhe Institute of Technology (KIT)
Máté Stark: Karlsruhe Institute of Technology (KIT)
Paul Greule: Karlsruhe Institute of Technology (KIT)
Kwan Ho Au-Yeung: Karlsruhe Institute of Technology (KIT)
Daria Sostina: Karlsruhe Institute of Technology (KIT)
José Reina Gálvez: Institute for Basic Science (IBS)
Christoph Sürgers: Karlsruhe Institute of Technology (KIT)
Wolfgang Wernsdorfer: Karlsruhe Institute of Technology (KIT)
Christoph Wolf: Institute for Basic Science (IBS)
Philip Willke: Karlsruhe Institute of Technology (KIT)

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: 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(C6H6). 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.

Date: 2025
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DOI: 10.1038/s41467-025-60409-w

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