Abstract
The magnetic properties of nanostructures that consist of a small number of atoms or molecules are typically determined by magnetic exchange interactions. Here, we show that non-magnetic, chemical interactions can have a similarly decisive effect if spin-moment-carrying orbitals extend in space and therefore allow the direct coupling of magnetic properties to wavefunction overlap and the formation of bonding and antibonding orbitals. We demonstrate this for a dimer of metal–molecule complexes on the Au(111) surface. A changing wavefunction overlap between the two monomers drives the surface-adsorbed dimer through a quantum phase transition from an underscreened triplet to a singlet ground state, with one configuration being located extremely close to a quantum critical point.
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Acknowledgements
B.L. and F.B.A. received support by the Deutsche Forschungsgemeinschaft through AN275/7-1. B.L., F.B.A. and M.R. acknowledge support from the NIC Jülich for CPU time under projects no. HHB00 and HMS17.
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R.T., C.W., T.E. and F.S.T. conceived the experiments. T.E. and R.T. conducted the experiments. T.E. analysed the experimental data. T.D., P.K. and M.R. performed density functional and many-body perturbation calculations and analysed the resultant data. B.L., F.S.T. and F.B.A. developed the theoretical model. B.L. and F.B.A. carried out the numerical renormalization group calculations and analysed the resultant data. T.E. prepared the figures. T.E., R.T., F.B.A. and F.S.T. wrote the paper, with significant contributions from all authors.
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Esat, T., Lechtenberg, B., Deilmann, T. et al. A chemically driven quantum phase transition in a two-molecule Kondo system. Nature Phys 12, 867–873 (2016). https://doi.org/10.1038/nphys3737
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DOI: https://doi.org/10.1038/nphys3737
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