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Vibrational and electronic dynamics of nitrogen–vacancy centres in diamond revealed by two-dimensional ultrafast spectroscopy

Nature Physics volume 9, pages 744–749 (2013)Cite this article

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Abstract

The optical and material properties of negatively charged nitrogen–vacancy (NV) centres in diamond make them attractive for applications ranging from quantum information to electromagnetic sensing. These properties are strongly dependent on the vibrational manifold associated with the centre, which determines phenomena associated with decoherence, relaxation and spin–orbit coupling. Despite its paramount importance in tuning these properties, the role of the vibrational bath and its effect on the electronic-state dynamics of NV centres in diamond is not fully understood. To elucidate the role of the bath, we present two-dimensional electronic spectroscopic studies of ensembles of negatively charged NV defect centres in diamond (NVD). We observe picosecond non-radiative relaxation within the phonon sideband and find that strongly coupled local modes dominate the vibrational bath. These findings provide a starting point for new insights into dephasing, spin addressing and relaxation in NVD with broad implications for magnetometry, quantum information, nanophotonics, sensing and ultrafast spectroscopy.

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Figure 1: Properties of the negatively charged NVD.
Figure 2: 2DES measurement of NV defect centres.
Figure 3: Vibrational modes associated with emission at the ZPL transition energy.
Figure 4: Comparison between calculated and measured 2DES and linear absorption signals.

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Acknowledgements

The authors thank A. Gali for initially suggesting ultrafast measurements with nitrogen–vacancy-diamond, A. Jarmola for preparing the nitrogen–vacancy-diamond sample, and N. Manson and P. Kehayias for helpful discussions. V.M.H. thanks the National Science and Engineering Research Council of Canada for a postdoctoral fellowship. D.B. was supported by NSF and the AFOSR/DARPA QuASAR programme. The work by V.M.H., T.A.A.O. and G.R.F. was supported by NSF grant CHE-1012168.

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  1. V. M. Huxter

    Present address: Present address: Department of Chemistry and Biochemistry, University of Arizona, Tucson, Arizona 85721, USA,

Authors and Affiliations

  1. Department of Chemistry, Berkeley and Physical Bioscience Division, University of California, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

    V. M. Huxter, T. A. A. Oliver & G. R. Fleming

  2. Department of Physics, Berkeley and Nuclear Science Division, University of California, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

    D. Budker

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Contributions

V.M.H., D.B. and G.R.F. conceived the experiment. D.B. and G.R.F. supervised the project. V.M.H. determined the experimental protocol, wrote and performed the simulation, analysed the data and wrote the manuscript. V.M.H. and T.A.A.O. collected the data. All authors discussed the results and implications and commented on the manuscript at all stages.

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Correspondence to G. R. Fleming.

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Huxter, V., Oliver, T., Budker, D. et al. Vibrational and electronic dynamics of nitrogen–vacancy centres in diamond revealed by two-dimensional ultrafast spectroscopy. Nature Phys 9, 744–749 (2013). https://doi.org/10.1038/nphys2753

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