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

Abstract

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 https://doi.org/10.5281/zenodo.5167019.

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Acknowledgements

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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Contributions

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). https://doi.org/10.1038/s41567-021-01355-4

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