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Strong spin–phonon coupling between a single-molecule magnet and a carbon nanotube nanoelectromechanical system

Abstract

Magnetic relaxation processes were first discussed for a crystal of paramagnetic transition ions1. It was suggested that mechanical vibrations of the crystal lattice (phonons) modulate the crystal electric field of the magnetic ion, thus inducing a ‘direct’ relaxation between two different spin states1,2,3. Direct relaxation has also been predicted for single-molecule magnets with a large spin and a high magnetic anisotropy1,4,5,6,7 and was first demonstrated in a Mn12 acetate crystal8. The spin-lattice relaxation time for such a direct transition is limited by the phonon density of states at the spin resonance1. In a three-dimensional system, such as a single-molecule magnet crystal, the phonon energy spectrum is continuous, but in a one-dimensional system, like a suspended carbon nanotube, the spectrum is discrete and can be engineered to an extremely low density of states9. An individual single-molecule magnet, coupled to a suspended carbon nanotube, should therefore exhibit extremely long relaxation times9 and the system's reduced size should result in a strong spin–phonon coupling10,11. Here, we provide the first experimental evidence for a strong spin–phonon coupling between a single molecule spin and a carbon nanotube resonator, ultimately enabling coherent spin manipulation and quantum entanglement10,11.

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Figure 1: Rare-earth SMM.
Figure 2: Longitudinal stretching modes in CNT NEMS.
Figure 3: Strong spin–phonon coupling of a TbPc2-SMM and a CNT NEMS.
Figure 4: Nuclear spin-dependent magnetization reversal of a single TbPc2 coupled to a CNT NEMS.

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Acknowledgements

The authors thank E. Eyraud, D. Lepoittevin, L. Cagnon, R. Haettel, C. Hoarau, V. Reita and P. Rodiere for technical contributions and discussions, T. Fournier, T. Crozes, B. Fernandez, S. Dufresnes and G. Julie for lithography development, and J.P. Cleuziou and N.V. Nguyen for CNT CVD growth development. The authors also thank E. Bonet, C. Thirion and R. Piquerel for help with software development and M. Urdampilleta, S. Thiele, R. Vincent and F. Balestro for fruitful discussions. Samples were fabricated in the Nanofab facility of the Néel Institute. This work is partially supported by the French National Research Agency National Programme in Nanosciences and Nanotechnologies (ANR-PNANO) project MolNanoSpin (no. ANR-08-NANO-002), European Research Council Advanced Grant MolNanoSpin (no. 226558), ICT-2007.8.0 Future Emerging Technologies Open, Quantum Information Processing Specific Targeted Research Project (no. 211284 MolSpinQIP), the German Research Foundation programme TRR 88 ‘3Met’, Cible 2009, and the Nanosciences Foundation of Grenoble. M.G. thanks the Nanoscience Foundation for financial support.

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M.G. and W.W. designed, conducted and analysed the experiments. S.K. and M.R. designed, synthesized and characterized the molecule. M.G. and W.W. co-wrote the paper.

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Correspondence to Wolfgang Wernsdorfer.

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Ganzhorn, M., Klyatskaya, S., Ruben, M. et al. Strong spin–phonon coupling between a single-molecule magnet and a carbon nanotube nanoelectromechanical system. Nature Nanotech 8, 165–169 (2013). https://doi.org/10.1038/nnano.2012.258

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