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Reversible optical data storage below the diffraction limit

Nature Nanotechnology volume 19, pages 202–207 (2024)Cite this article

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An Author Correction to this article was published on 12 January 2024

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Abstract

Colour centres in wide-bandgap semiconductors feature metastable charge states that can be interconverted with the help of optical excitation at select wavelengths. The distinct fluorescence and spin properties in each of these states have been exploited to show storage of classical information in three dimensions, but the memory capacity of these platforms has been thus far limited by optical diffraction. Here we leverage local heterogeneity in the optical transitions of colour centres in diamond (nitrogen vacancies) to demonstrate selective charge state control of individual point defects sharing the same diffraction-limited volume. Further, we apply this approach to dense colour centre ensembles, and show rewritable, multiplexed data storage with an areal density of 21 Gb inch–2 at cryogenic temperatures. These results highlight the advantages for developing alternative optical storage device concepts that can lead to increased storage capacity and reduced energy consumption per operation.

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Fig. 1: Optical spectroscopy and charge control of NV− centres under cryogenic conditions.
Fig. 2: Sub-diffraction NV− ionization and read-out.
Fig. 3: Charge manipulation and non-destructive optical spectroscopy of a four-NV sub-diffraction cluster.
Fig. 4: Multiplexed data storage.

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Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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References

  1. Degen, C. L., Reinhard, F. & Cappellaro, P. Quantum sensing. Rev. Mod. Phys. 89, 035002 (2017).

    MathSciNet  ADS  Google Scholar 

  2. Awschalom, D. D., Hanson, R., Wrachtrup, J. & Zhou, B. B. Quantum technologies with optically interfaced solid-state spins. Nat. Photon. 12, 516–527 (2018).

    CAS  ADS  Google Scholar 

  3. Aslam, N., Waldherr, G., Neumann, P., Jelezko, F. & Wrachtrup, J. Photo-induced ionization dynamics of the nitrogen vacancy defect in diamond investigated by single-shot charge state detection. New J. Phys. 15, 013064 (2013).

    CAS  ADS  Google Scholar 

  4. Lozovoi, A. et al. Optical activation and detection of charge transport between individual colour centres in diamond. Nat. Electron. 4, 717–724 (2021).

    CAS  Google Scholar 

  5. Mizuochi, N. et al. Electrically driven single-photon source at room temperature in diamond. Nat. Photon. 6, 299–303 (2012).

    CAS  ADS  Google Scholar 

  6. Lozovoi, A., Vizkelethy, G., Bielejec, E. & Meriles, C. A. Imaging dark charge emitters in diamond via carrier-to-photon conversion. Sci. Adv. 8, eabl9402 (2022).

    CAS  PubMed  PubMed Central  ADS  Google Scholar 

  7. Shields, B. J., Unterreithmeier, Q. P., De Leon, N. P., Park, H. & Lukin, M. D. Efficient readout of a single spin state in diamond via spin-to-charge conversion. Phys. Rev. Lett. 114, 136402 (2015).

    CAS  PubMed  ADS  Google Scholar 

  8. Hopper, D. A., Lauigan, J. D., Huang, T.-Y. & Bassett, L. C. Real-time charge initialization of diamond nitrogen-vacancy centers for enhanced spin readout. Phys. Rev. Appl. 13, 024016 (2020).

    CAS  ADS  Google Scholar 

  9. Jayakumar, H., Dhomkar, S., Henshaw, J. & Meriles, C. A. Spin readout via spin-to-charge conversion in bulk diamond nitrogen-vacancy ensembles. Appl. Phys. Lett. 113, 122404 (2018).

    ADS  Google Scholar 

  10. Zhang, Q. et al. High-fidelity single-shot readout of single electron spin in diamond with spin-to-charge conversion. Nat. Commun. 12, 1529 (2021).

    CAS  PubMed  PubMed Central  ADS  Google Scholar 

  11. Irber, D. M. et al. Robust all-optical single-shot readout of nitrogen-vacancy centers in diamond. Nat. Commun. 12, 532 (2021).

    CAS  PubMed  PubMed Central  ADS  Google Scholar 

  12. Dhomkar, S., Henshaw, J., Jayakumar, H. & Meriles, C. A. Long-term data storage in diamond. Sci. Adv. 2, e1600911 (2016).

    PubMed  PubMed Central  ADS  Google Scholar 

  13. Dhomkar, S., Jayakumar, H., Zangara, P. R. & Meriles, C. A. Charge dynamics in near-surface, variable-density ensembles of nitrogen-vacancy centers in diamond. Nano Lett. 18, 4046–4052 (2018).

    CAS  PubMed  ADS  Google Scholar 

  14. Wolfowicz, G. et al. Optical charge state control of spin defects in 4H-SiC. Nat. Commun. 8, 1876 (2017).

    PubMed  PubMed Central  ADS  Google Scholar 

  15. Rittweger, E., Han, K. Y., Irvine, S. E., Eggeling, C. & Hell, S. W. STED microscopy reveals crystal colour centres with nanometric resolution. Nat. Photon. 3, 144–147 (2009).

    CAS  ADS  Google Scholar 

  16. Huang, B., Wang, W., Bates, M. & Zhuang, X. Three-dimensional super-resolution imaging by stochastic optical reconstruction microscopy. Science 319, 810–813 (2008).

    CAS  PubMed  PubMed Central  ADS  Google Scholar 

  17. Pfender, M., Aslam, N., Waldherr, G., Neumann, P. & Wrachtrup, J. Single-spin stochastic optical reconstruction microscopy. Proc. Natl Acad. Sci. USA 111, 14669–14674 (2014).

    CAS  PubMed  PubMed Central  ADS  Google Scholar 

  18. Rittweger, E., Wildanger, D. & Hell, S. W. Far-field fluorescence nanoscopy of diamond color centers by ground state depletion. Eur. Phys. Lett. 86, 14001 (2009).

    ADS  Google Scholar 

  19. Han, K. Y., Kim, S. K., Eggeling, C. & Hell, S. W. Metastable dark states enable ground state depletion microscopy of nitrogen vacancy centers in diamond with diffraction-unlimited resolution. Nano Lett. 10, 3199–3203 (2010).

    CAS  PubMed  ADS  Google Scholar 

  20. Chen, X. et al. Subdiffraction optical manipulation of the charge state of nitrogen vacancy center in diamond. Light. Sci. Appl. 4, e230 (2015).

    CAS  Google Scholar 

  21. Lamon, S., Wu, Y., Zhang, Q., Liu, X. & Gu, M. Nanoscale optical writing through upconversion resonance energy transfer. Sci. Adv. 7, eabe2209 (2021).

    CAS  PubMed  PubMed Central  ADS  Google Scholar 

  22. Harke, B. et al. Polymerization inhibition by triplet state absorption for nanoscale lithography. Adv. Mater. 25, 904–909 (2013).

    CAS  PubMed  PubMed Central  Google Scholar 

  23. Gan, Z., Cao, Y., Evans, R. A. & Gu, M. Three-dimensional deep sub-diffraction optical beam lithography with 9 nm feature size. Nat. Commun. 4, 2061 (2013).

    PubMed  ADS  Google Scholar 

  24. Li, L., Gattass, R. R., Gershgoren, E., Hwang, H. & Fourkas, J. T. Achieving λ/20 resolution by one-color initiation and deactivation of polymerization. Science 324, 910–913 (2009).

    CAS  PubMed  ADS  Google Scholar 

  25. Wollhofen, R., Katzmann, J., Hrelescu, C., Jacak, J. & Klar, T. A. 120 nm resolution and 55 nm structure size in STED-lithography. Opt. Express 21, 10831–10840 (2013).

    CAS  PubMed  ADS  Google Scholar 

  26. Fischer, J., von Freymann, G. & Wegener, M. The materials challenge in diffraction-unlimited direct-laser-writing optical lithography. Adv. Mater. 22, 3578–3582 (2010).

    CAS  PubMed  Google Scholar 

  27. Tamarat, P. H. et al. Spin-flip and spin-conserving optical transitions of the nitrogen-vacancy centre in diamond. New J. Phys. 10, 045004 (2008).

    ADS  Google Scholar 

  28. Manson, N. B., Harrison, J. P. & Sellars, M. J. Nitrogen-vacancy center in diamond: model of the electronic structure and associated dynamics. Phys. Rev. B 74, 104303 (2006).

    ADS  Google Scholar 

  29. Maze, J. R. et al. Properties of nitrogen-vacancy centers in diamond: the group theoretic approach. New J. Phys. 13, 025025 (2011).

    ADS  Google Scholar 

  30. Doherty, M. W. et al. The nitrogen-vacancy colour centre in diamond. Phys. Rep. 528, 1–45 (2013).

    CAS  ADS  Google Scholar 

  31. Sipahigil, A. et al. Indistinguishable photons from separated silicon-vacancy centers in diamond. Phys. Rev. Lett. 113, 113602 (2014).

    CAS  PubMed  ADS  Google Scholar 

  32. Bersin, E. et al. Individual control and readout of qubits in a sub-diffraction volume. npj Quant. Inf. 5, 38 (2019).

    ADS  Google Scholar 

  33. Fu, K.-M. C. et al. Observation of the dynamic Jahn-Teller effect in the excited states of nitrogen-vacancy centers in diamond. Phys. Rev. Lett. 103, 256404 (2009).

    PubMed  ADS  Google Scholar 

  34. Baier, S. et al. Orbital and spin dynamics of single neutrally-charged nitrogen-vacancy centers in diamond. Phys. Rev. Lett. 125, 193601 (2020).

    CAS  PubMed  ADS  Google Scholar 

  35. Edmonds, A. M. et al. Characterization of CVD diamond with high concentrations of nitrogen for magnetic-field sensing applications. Mater. Quant. Technol. 1, 025001 (2021).

    ADS  Google Scholar 

  36. Oberg, L. M. et al. Spin coherent quantum transport of electrons between defects in diamond. Nanophotonincs 8, 1975–1984 (2019).

    CAS  Google Scholar 

  37. Doherty, M. W. et al. Towards a room-temperature spin quantum bus in diamond via optical spin injection, transport and detection. Phys. Rev. X 6, 041035 (2016).

    Google Scholar 

  38. McCullian, B. A., Cheung, H. F. H., Chen, H. Y. & Fuchs, G. D. Quantifying the spectral diffusion of N-V centers by symmetry. Phys. Rev. Appl. 18, 064011 (2022).

    CAS  ADS  Google Scholar 

  39. Zhang, Z.-H. et al. Optically detected magnetic resonance in neutral silicon vacancy centers in diamond via bound exciton states. Phys. Rev. Lett. 125, 237402 (2020).

    CAS  PubMed  ADS  Google Scholar 

  40. Kazimierczuk, T., Fröhlich, D., Scheel, S., Stolz, H. & Bayer, M. Giant Rydberg excitons in the copper oxide Cu2O. Nature 514, 343–347 (2014).

    CAS  PubMed  ADS  Google Scholar 

  41. Monge, R. et al. Spin dynamics of a solid-state qubit in proximity to a superconductor. Nano Lett. 23, 422–428 (2023).

    CAS  PubMed  ADS  Google Scholar 

  42. Balasubramanian, G. et al. Nanoscale imaging magnetometry with diamond spins under ambient conditions. Nature 455, 648–651 (2008).

    CAS  PubMed  ADS  Google Scholar 

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Acknowledgements

We acknowledge useful discussions with D. Irber, F. Reinhard and A. Lozovoi. R.M. and C.A.M. acknowledge support from the National Science Foundation through grant NSF-1914945; T.D. and C.A.M. acknowledge support from the National Science Foundation through grant NSF-2216838. R.M. acknowledges support from NSF-2316693. We all acknowledge the access to the facilities and research infrastructure of the National Science Foundation CREST IDEALS, grant NSF-2112550.

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Author notes

  1. These authors contributed equally: Richard Monge, Tom Delord.

Authors and Affiliations

  1. Department of Physics, City College of New York, CUNY, New York, NY, USA

    Richard Monge, Tom Delord & Carlos A. Meriles

  2. Graduate Center, CUNY, New York, NY, USA

    Richard Monge & Carlos A. Meriles

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  1. Richard Monge
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Contributions

R.M., T.D. and C.A.M. conceived the experiments. R.M. and T.D. conducted the experiments and analysed the data with C.A.M.’s assistance. C.A.M. supervised the project and wrote the manuscript with input from all authors.

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Correspondence to Carlos A. Meriles.

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Supplementary Figs. 1–16, Discussion Sections 1–8 and references.

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Monge, R., Delord, T. & Meriles, C.A. Reversible optical data storage below the diffraction limit. Nat. Nanotechnol. 19, 202–207 (2024). https://doi.org/10.1038/s41565-023-01542-9

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