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Quantum coherent spin–electric control in a molecular nanomagnet at clock transitions


Electrical control of spins at the nanoscale offers significant architectural advantages in spintronics, because electric fields can be confined over shorter length scales than magnetic fields1,2,3,4,5. Thus, recent demonstrations of electric-field sensitivities in molecular spin materials6,7,8 are tantalizing, raising the viability of the quantum analogues of macroscopic magneto-electric devices9,10,11,12,13,14,15. However, the electric-field sensitivities reported so far are rather weak, prompting the question of how to design molecules with stronger spin–electric couplings. Here we show that one path is to identify an energy scale in the spin spectrum that is associated with a structural degree of freedom with a substantial electrical polarizability. We study an example of a molecular nanomagnet in which a small structural distortion establishes clock transitions (that is, transitions whose energy is to first order independent of the magnetic field) in the spin spectrum; the fact that this distortion is associated with an electric dipole allows us to control the clock-transition energy to an unprecedented degree. We demonstrate coherent electrical control of the quantum spin state and exploit it to independently manipulate the two magnetically identical but inversion-related molecules in the unit cell of the crystal. Our findings pave the way for the use of molecular spins in quantum technologies and spintronics.

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Fig. 1: The spin–electric coupling experiment.
Fig. 2: SEC dependence on orientation, E field and magnetic field.
Fig. 3: E field selection of molecular subpopulations.

Data availability

Experimental data supporting the conclusions are available at


  1. Kane, B. E. A silicon-based nuclear spin quantum computer. Nature 393, 133–137 (1998).

    Article  ADS  Google Scholar 

  2. Trif, M., Troiani, F., Stepanenko, D. & Loss, D. Spin-electric coupling in molecular magnets. Phys. Rev. Lett. 101, 217201 (2008).

    Article  ADS  Google Scholar 

  3. Laucht, A. et al. Electrically controlling single-spin qubits in a continuous microwave field. Sci. Adv. 1, e1500022 (2015).

    Article  ADS  Google Scholar 

  4. Tosi, G. et al. Silicon quantum processor with robust long-distance qubit couplings. Nat. Commun. 8, 450 (2017).

    Article  ADS  Google Scholar 

  5. Asaad, S. et al. Coherent electrical control of a single high-spin nucleus in silicon. Nature 579, 205–209 (2020).

    Article  ADS  Google Scholar 

  6. Liu, J. et al. Electric field control of spins in molecular magnets. Phys. Rev. Lett. 122, 037202 (2019).

    Article  ADS  Google Scholar 

  7. Fittipaldi, M. et al. Electric field modulation of magnetic exchange in molecular helices. Nat. Mater. 18, 329–334 (2019).

    Article  ADS  Google Scholar 

  8. Robert, J., Parizel, N., Turek, P. & Boudalis, A. K. Polyanisotropic magnetoelectric coupling in an electrically controlled molecular spin qubit. J. Am. Chem. Soc. 141, 19765–19775 (2019).

    Article  Google Scholar 

  9. Palii, A., Clemente-Juan, J. M., Tsukerblat, B. & Coronado, E. Electric field control of the optical properties in magnetic mixed-valence molecules. Chem. Sci. 5, 3598–3602 (2014).

    Article  Google Scholar 

  10. Cardona-Serra, S. et al. Electrically switchable magnetic molecules: inducing a magnetic coupling by means of an external electric field in a mixed-valence polyoxovanadate cluster. Chem. Eur. J. 21, 763–769 (2015).

    Article  Google Scholar 

  11. Gaita-Ariño, A., Luis, F., Hill, S. & Coronado, E. Molecular spins for quantum computation. Nat. Chem. 11, 301–309 (2019).

    Article  Google Scholar 

  12. Atzori, M. & Sessoli, R. The second quantum revolution: role and challenges of molecular chemistry. J. Am. Chem. Soc. 141, 11339–11352 (2019).

    Article  Google Scholar 

  13. Godfrin, C. et al. Operating quantum states in single magnetic molecules: implementation of Grover’s quantum algorithm. Phys. Rev. Lett. 119, 187702 (2017).

    Article  ADS  Google Scholar 

  14. Eerenstein, W., Mathur, N. D. & Scott, J. F. Multiferroic and magnetoelectric materials. Nature 442, 759–765 (2006).

    Article  ADS  Google Scholar 

  15. Matsukura, F., Tokura, Y. & Ohno, H. Control of magnetism by electric fields. Nat. Nanotechnol. 10, 209–220 (2015).

    Article  ADS  Google Scholar 

  16. AlDamen, M. A. et al. Mononuclear lanthanide single molecule magnets based on the polyoxometalates [Ln(W5O18)2]9− and [Ln(β2-SiW11O39)2]13− (LnIII = Tb, Dy, Ho, Er, Tm, and Yb). Inorg. Chem. 48, 3467–3479 (2009).

    Article  Google Scholar 

  17. Shiddiq, M. et al. Enhancing coherence in molecular spin qubits via atomic clock transitions. Nature 531, 348–351 (2016).

    Article  ADS  Google Scholar 

  18. Ghosh, S. et al. Multi-frequency EPR studies of a mononuclear holmium single-molecule magnet based on the polyoxometalate [HoIII(W5O18)2]9−. Dalton Trans. 41, 13697–13704 (2012).

    Article  Google Scholar 

  19. Alvarez, S., Alemany, P., Casanova, D., Cirera, J. & Llunell, M. Shape maps and polyhedral interconversion paths in transition metal chemistry. Coord. Chem. Rev. 249, 1693–1708 (2005).

    Article  Google Scholar 

  20. Frisch, M. J. et al. Gaussian 16 Revision A.03 (Gaussian, 2016).

  21. Sarkar, A. & Rajaraman, G. Modulating magnetic anisotropy in Ln(iii) single-ion magnets using an external electric field. Chem. Sci. 11, 10324–10330 (2020).

    Article  Google Scholar 

  22. Wedge, C. J. et al. Chemical engineering of molecular qubits. Phys. Rev. Lett. 108, 107204 (2012).

    Article  ADS  Google Scholar 

  23. Kintzel, B. et al. Spin-electric coupling in a cobalt(II)-based spin triangle revealed by electric-field-modulated electron spin resonance spectroscopy. Angew. Chem. Int. Ed. 60, 8832–8838 (2021).

    Article  Google Scholar 

  24. Liu, Z. et al. Electric field manipulation enhanced by strong spin-orbit coupling: promoting rare-earth ions as qubits. Natl Sci. Rev. 7, 1557–1563 (2020).

    Article  Google Scholar 

  25. George, R. E., Edwards, J. P. & Ardavan, A. Coherent spin control by electrical manipulation of the magnetic anisotropy. Phys. Rev. Lett. 110, 027601 (2013).

    Article  ADS  Google Scholar 

  26. Mi, X. et al. A coherent spin–photon interface in silicon. Nature 555, 599–603 (2018).

    Article  ADS  Google Scholar 

  27. Fdez. Galvan, I. et al. Openmolcas: from source code to insight. J. Chem. Theory Comput. 15, 5925–5964 (2019).

    Article  Google Scholar 

  28. Ungur, L. & Chibotaru, L. F. Ab initio crystal field for lanthanides. Chem. Eur. J. 23, 3708–3718 (2017).

    Article  Google Scholar 

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This work is supported by the EU (ERC-2014-CoG-647301 DECRESIM, ERC-2018-AdG-788222 MOL-2D, COST Action CA15128 MOLSPIN, the QuantERA project SUMO, and the H2020 research and innovation programme projects SPRING (no. 863098) and FATMOLS (no. 862893)); the Spanish MINECO (grant CTQ2017-89993 co-financed by FEDER and grant MAT2017-89528; the Unit of Excellence ‘María de Maeztu’ CEX2019-000919-M); the Generalitat Valenciana (Prometeo Program of Excellence); and the UK EPSRC (EP/P000479/1). J.J.B. acknowledges support by the Generalitat Valenciana (CDEIGENT/2019/022). J.M. is supported by Magdalen College, Oxford. J.L. is supported by the Royal Society through a University Research Fellowship.

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Authors and Affiliations



J.L., E.C., A.G.-A. and A.A. conceived the study. Materials were synthesized by Y.D. under the supervision of E.C. ESR experiments were conducted by J.L. and J.M. Data analysis was performed by J.L. with input from A.A. Theoretical modelling was done by A.U.; assisted by J.J.B.; guided by A.G.-A.; and in discussion with J.L., E.C. and A.A. All the authors contributed to the manuscript.

Corresponding authors

Correspondence to Junjie Liu, Alejandro Gaita-Ariño or Arzhang Ardavan.

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The authors declare no competing interests.

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Peer review information Nature Physics thanks Nicholas Chilton, Stergios Piligkos and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–20, Discussion and Tables 1–6.

Supplementary Video 1

Electric-field-induced distortion of the crystal structure.

Supplementary Video 2

Electric-field-induced distortion of the optimized structure.

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Liu, J., Mrozek, J., Ullah, A. et al. Quantum coherent spin–electric control in a molecular nanomagnet at clock transitions. Nat. Phys. 17, 1205–1209 (2021).

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