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Peer-reviewedCC BYNature Physics

Exchange-mediated spin–electric control of single molecules on surfaces

  • Paul Greule1
  • Wantong Huang1
  • Máté Stark1
  • Kwan Ho Au‐Yeung2,1
  • Johannes Schwenk1
  • José Reina Gálvez3
  • C. Sürgers1
  • Wolfgang Wernsdorfer4,1
  • Christoph Wolf5,6
  • Philip Willke2,1
6 affiliations
  1. 1Physikalisches Institut, Karlsruhe Institute of Technology, Karlsruhe, Germany
  2. 2Center for Integrated Quantum Science and Technology, Karlsruhe Institute of Technology, Karlsruhe, Germany
  3. 3Department of Physics, University of Konstanz, Konstanz, Germany
  4. 4Institute for Quantum Materials and Technologies, Karlsruhe, Germany
  5. 5Center for Quantum Nanoscience, Institute for Basic Science, Seoul, Republic of Korea
  6. 6Ewha Womans University, Seoul, Republic of Korea
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Abstract

Individual magnetic molecules are promising building blocks for quantum technologies owing to their chemical tunability, nanoscale dimensions and ability to self-assemble into ordered arrays. However, exploiting their properties in quantum information processing requires precise local control of their spin. Here we demonstrate spin-electric coupling for two molecular spin systems-iron phthalocyanine (FePc) and Fe-FePc complexes-adsorbed on a surface. We use electron spin resonance combined with scanning tunnelling microscopy to locally address them and electrically tune them using an applied bias voltage. These measurements reveal a nonlinear voltage dependence of the resonance frequency, linked to the energetic position of the molecular orbitals. We attribute this effect to a transport-mediated exchange field from the magnetic tip, providing a large, highly localized and broadly applicable spin-electric coupling mechanism. Finally, we demonstrate that the spin-electric coupling enables all-electrical coherent spin control. In Rabi oscillation measurements of both single and coupled Fe-FePc complexes, we show that the spin dynamics can be tuned using the exchange field, demonstrating a pathway towards electrically controlled quantum operations.

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Cite

BibTeXRIS
BibTeX
@article{greule2026exchangemediated,
  title = {{Exchange-mediated spin–electric control of single molecules on surfaces}},
  author = {Paul Greule and Wantong Huang and Máté Stark and Kwan Ho Au‐Yeung and Johannes Schwenk and José Reina Gálvez and C. Sürgers and Wolfgang Wernsdorfer and Christoph Wolf and Philip Willke},
  journal = {Nature Physics},
  year = {2026},
  month = jun,
  doi = {10.1038/s41567-026-03353-w},
  url = {https://doi.org/10.1038/s41567-026-03353-w},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Exchange-mediated spin–electric control of single molecules on surfaces
AU  - Paul Greule
AU  - Wantong Huang
AU  - Máté Stark
AU  - Kwan Ho Au‐Yeung
AU  - Johannes Schwenk
AU  - José Reina Gálvez
AU  - C. Sürgers
AU  - Wolfgang Wernsdorfer
AU  - Christoph Wolf
AU  - Philip Willke
PY  - 2026
DA  - 2026/06/29
JO  - Nature Physics
DO  - 10.1038/s41567-026-03353-w
UR  - https://doi.org/10.1038/s41567-026-03353-w
AB  - Individual magnetic molecules are promising building blocks for quantum technologies owing to their chemical tunability, nanoscale dimensions and ability to self-assemble into ordered arrays. However, exploiting their properties in quantum information processing requires precise local control of their spin. Here we demonstrate spin-electric coupling for two molecular spin systems-iron phthalocyanine (FePc) and Fe-FePc complexes-adsorbed on a surface. We use electron spin resonance combined with scanning tunnelling microscopy to locally address them and electrically tune them using an applied bias voltage. These measurements reveal a nonlinear voltage dependence of the resonance frequency, linked to the energetic position of the molecular orbitals. We attribute this effect to a transport-mediated exchange field from the magnetic tip, providing a large, highly localized and broadly applicable spin-electric coupling mechanism. Finally, we demonstrate that the spin-electric coupling enables all-electrical coherent spin control. In Rabi oscillation measurements of both single and coupled Fe-FePc complexes, we show that the spin dynamics can be tuned using the exchange field, demonstrating a pathway towards electrically controlled quantum operations.
SN  - 1745-2473
SN  - 1745-2481
ER  -