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A chemically driven quantum phase transition in a two-molecule Kondo system

Nature Physics volume 12, pages 867–873 (2016)Cite this article

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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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Figure 1: Structure and spectral properties of dimers consisting of Au-PTCDA complexes on the Au(111) surface.
Figure 2: TIAM and chemical interaction of Au-PTCDA dimers.
Figure 3: Spectral functions and ground states of surface-adsorbed Au-PTCDA dimers in the parity-symmetric case (Vo = 0).
Figure 4: Spectral functions of Au-PTCDA dimers in the parity-broken case, analysed with the NRG method.

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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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Authors and Affiliations

  1. Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425 Jülich, Germany

    Taner Esat, Christian Wagner, Ruslan Temirov & F. Stefan Tautz

  2. Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, 52425 Jülich, Germany

    Taner Esat, Christian Wagner, Ruslan Temirov & F. Stefan Tautz

  3. Lehrstuhl für Theoretische Physik II, Technische Universität Dortmund, Otto-Hahn-Strasse 4, 44221 Dortmund, Germany

    Benedikt Lechtenberg & Frithjof B. Anders

  4. Institut für Festkörpertheorie, Westfälische Wilhelms-Universität Münster, 48149 Münster, Germany

    Thorsten Deilmann, Peter Krüger & Michael Rohlfing

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  1. Taner Esat
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Contributions

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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Correspondence to F. Stefan Tautz.

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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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