Article

Tunable room-temperature single-photon emission at telecom wavelengths from sp3 defects in carbon nanotubes

Received:
Accepted:
Published online:

Abstract

Generating quantum light emitters that operate at room temperature and at telecom wavelengths remains a significant materials challenge. To achieve this goal requires light sources that emit in the near-infrared wavelength region and that, ideally, are tunable to allow desired output wavelengths to be accessed in a controllable manner. Here, we show that exciton localization at covalently introduced aryl sp3 defect sites in single-walled carbon nanotubes provides a route to room-temperature single-photon emission with ultrahigh single-photon purity (99%) and enhanced emission stability approaching the shot-noise limit. Moreover, we demonstrate that the inherent optical tunability of single-walled carbon nanotubes, present in their structural diversity, allows us to generate room-temperature single-photon emission spanning the entire telecom band. Single-photon emission deep into the centre of the telecom C band (1.55 µm) is achieved at the largest nanotube diameters we explore (0.936 nm).

  • Subscribe to Nature Photonics for full access:

    $59

    Subscribe

Additional access options:

Already a subscriber?  Log in  now or  Register  for online access.

References

  1. 1.

    & Single-photon sources. Rep. Prog. Phys. 68, 1129–1179 (2005).

  2. 2.

    et al. Diamond-based single-photon emitters. Rep. Prog. Phys. 74, 076501 (2011).

  3. 3.

    et al. Quantum computing with defects. MRS Bull. 38, 802–807 (2013).

  4. 4.

    & Nitrogen-vacancy centers: physics and applications. MRS Bull. 38, 127–133 (2013).

  5. 5.

    , & Solid-state single-photon emitters. Nat. Photon. 10, 631–641 (2016).

  6. 6.

    et al. Single-photon emission at 1.5 µm from an InAs/InP quantum dot with highly suppressed multi-photon emission probabilities. Appl. Phys. Lett. 109, 132106 (2016).

  7. 7.

    et al. Optically active quantum dots in monolayer WSe2. Nat. Nanotech. 10, 491–496 (2015).

  8. 8.

    et al. Single quantum emitters in monolayer semiconductors. Nat. Nanotech. 10, 497–501 (2015).

  9. 9.

    et al. Single photon emitters in exfoliated WSe2 structures. Nat. Nanotech. 10, 503–506 (2015).

  10. 10.

    , , , & Voltage-controlled quantum light from an atomically thin semiconductor. Nat. Nanotech. 10, 507–512 (2015).

  11. 11.

    , , , & Quantum emission from hexagonal boron nitride monolayers. Nat. Nanotech. 11, 37–41 (2016).

  12. 12.

    , , , & Room-temperature single-photon generation from solitary dopants of carbon nanotubes. Nat. Nanotech. 10, 671–675 (2015).

  13. 13.

    et al. Robust multicolor single photon emission from point defects in hexagonal boron nitride. ACS Nano 10, 7331–7338 (2016).

  14. 14.

    , , & Photon antibunching in the photoluminescence spectra of a single carbon nanotube. Phys. Rev. Lett. 100, 217401 (2008).

  15. 15.

    , & Quantum light signatures and nanosecond spectral diffusion from cavity-embedded carbon nanotubes. Nano Lett. 12, 1934–1941 (2012).

  16. 16.

    et al. Bright, long-lived and coherent excitons in carbon nanotube quantum dots. Nat. Nanotech. 8, 502–505 (2013).

  17. 17.

    , , , & Ubiquity of exciton localization in cryogenic carbon nanotubes. Nano Lett. 16, 2958–2962 (2016).

  18. 18.

    , , , & Oxygen doping modifies near-infrared band gaps in fluorescent single-walled carbon nanotubes. Science 330, 1656–1659 (2010).

  19. 19.

    et al. Electronic structure and chemical nature of oxygen dopant states in carbon nanotubes. ACS Nano 8, 10782–10789 (2014).

  20. 20.

    , , , & Solid-state approach for fabrication of photostable, oxygen-doped carbon nanotubes. Adv. Funct. Mater. 25, 6157–6164 (2015).

  21. 21.

    et al. Structure-assigned optical spectra of single-walled carbon nanotubes. Science 298, 2361–2366 (2002).

  22. 22.

    , & Carbon nanotube photonics and optoelectronics. Nat. Photon. 2, 341–350 (2008).

  23. 23.

    et al. Fully integrated quantum photonic circuit with an electrically driven light source. Nat. Photon. 10, 727–732 (2016).

  24. 24.

    et al. Ultralow mode-volume photonic crystal nanobeam cavities for high-efficiency coupling to individual carbon nanotube emitters. Nat. Commun. 5, 5580 (2014).

  25. 25.

    et al. Widely tunable single-photon source from a carbon nanotube in the Purcell regime. Phys. Rev. Lett. 116, 247402 (2016).

  26. 26.

    et al. Broadband tunable, polarization-selective and directional emission of (6,5) carbon nanotubes coupled to plasmonic crystals. Nano Lett. 16, 3278–3284 (2016).

  27. 27.

    et al. Photoluminescence imaging of solitary dopant sites in covalently doped single-wall carbon nanotubes. Nanoscale 7, 20521–20530 (2015).

  28. 28.

    et al. Brightening of carbon nanotube photoluminescence through the incorporation of sp3 defects. Nat. Chem. 5, 840–845 (2013).

  29. 29.

    et al. Tuning of the photoluminescence and upconversion photoluminescence properties of single-walled carbon nanotubes by chemical functionalization. Nanoscale 8, 16916–16921 (2016).

  30. 30.

    et al. Experimental realization of an absolute single-photon source based on a single nitrogen vacancy center in diamond. Optica 4, 71–76 (2017).

  31. 31.

    et al. Single-photon emission in telecommunication band from an InAs quantum dot grown on InP with molecular-beam epitaxy. Appl. Phys. Lett. 103, 061114 (2013).

  32. 32.

    , & A single molecule as a high-fidelity photon gun for producing intensity-squeezed light. Nat. Photon. 11, 58–62 (2017).

  33. 33.

    et al. Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes. Nat. Commun. 4, 2152 (2013).

  34. 34.

    & Diamond nanophotonics. Adv. Opt. Mater. 2, 911–928 (2014).

  35. 35.

    et al. Photoluminescence dynamics of aryl sp3 defect states in single-walled carbon nanotubes. ACS Nano 10, 8355–8365 (2016).

  36. 36.

    et al. Disorder limited exciton transport in colloidal single-wall carbon nanotubes. Nano Lett. 12, 5091–5096 (2012).

  37. 37.

    et al. Luminescence properties of individual empty and water-filled single-walled carbon nanotubes. ACS Nano 6, 2649–2655 (2012).

  38. 38.

    et al. Polyfluorene-sorted, carbon nanotube array field-effect transistors with increased current density and high on/off ratio. ACS Nano 8, 11614–11621 (2014).

  39. 39.

    et al. Molecularly tunable fluorescent quantum defects. J. Am. Chem. Soc. 138, 6878–6885 (2016).

  40. 40.

    , , & Emergence of new red-shifted carbon nanotube photoluminescence based on proximal doped-site design. Sci. Rep. 6, 28393 (2016).

  41. 41.

    et al. Photoluminescence imaging of polyfluorene surface structures on semiconducting carbon nanotubes: implications for thin film exciton transport. ACS Nano 10, 11449–11458 (2016).

  42. 42.

    et al. Role of surfactants and salt in aqueous two-phase separation of carbon nanotubes toward simple chirality isolation. ACS Nano 8, 1619–1628 (2014).

  43. 43.

    et al. Isolation of specific small-diameter single-wall carbon nanotube species via aqueous two-phase extraction. Adv. Mater. 26, 2800–2804 (2014).

  44. 44.

    et al. Industrial-scale separation of high-purity single-chirality single-wall carbon nanotubes for biological imaging. Nat. Commun. 7, 12056 (2016).

  45. 45.

    , & Optical excitation of carbon nanotubes drives localized diazonium reactions. J. Phys. Chem. Lett. 7, 3690–3694 (2016).

Download references

Acknowledgements

This work was conducted in part at the Center for Integrated Nanotechnologies, a US Department of Energy, Office of Science user facility and supported in part by Los Alamos National Laboratory Directed Research and Development funds. This effort was also supported at AIST in part by the Japan Society for the Promotion of Science (JSPS) KAKENHI grant numbers JP16H07103 and JP25220602. National Renewable Energy Laboratory (NREL) researchers were supported by the Solar Photochemistry Program of the US Department of Energy, Office of Science, Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences, under contract no. DE-AC36-08GO28308 to NREL. W.G. and J.K. acknowledge support from the Robert A. Welch Foundation through grant no. C-1509.

Author information

Affiliations

  1. Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA

    • Xiaowei He
    • , Nicolai F. Hartmann
    • , Xuedan Ma
    • , Younghee Kim
    • , Han Htoon
    •  & Stephen K. Doorn
  2. Chemical and Materials Science Center, National Renewable Energy Laboratory, 1617 Cole Boulevard, Golden, Colorado 80401, USA

    • Rachelle Ihly
    •  & Jeffrey L. Blackburn
  3. Department of Electrical and Computer Engineering, Rice University, Houston, Texas 77005, USA

    • Weilu Gao
    •  & Junichiro Kono
  4. Department of Physics, Tokyo Metropolitan University, Hachioji, Tokyo 192-0372, Japan

    • Yohei Yomogida
  5. Nanomaterials Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki 305-8565, Japan

    • Atsushi Hirano
    • , Takeshi Tanaka
    •  & Hiromichi Kataura

Authors

  1. Search for Xiaowei He in:

  2. Search for Nicolai F. Hartmann in:

  3. Search for Xuedan Ma in:

  4. Search for Younghee Kim in:

  5. Search for Rachelle Ihly in:

  6. Search for Jeffrey L. Blackburn in:

  7. Search for Weilu Gao in:

  8. Search for Junichiro Kono in:

  9. Search for Yohei Yomogida in:

  10. Search for Atsushi Hirano in:

  11. Search for Takeshi Tanaka in:

  12. Search for Hiromichi Kataura in:

  13. Search for Han Htoon in:

  14. Search for Stephen K. Doorn in:

Contributions

H.H. and S.K.D. conceived and designed the experiment. X.H., under the supervision of H.H. and S.K.D. and with assistance from X.M. and Y.K., performed all spectroscopy studies and data analysis and, with N.F.H. under the supervision of S.K.D., performed nanotube separation and functionalization. R.I. and J.L.B. provided PFO-bpy-wrapped (6,5) SWCNT material. Y.Y., A.H., T.T., H.K., W.G. and J.K. provided (10,3) SWCNT material. X.H., H.H. and S.K.D. prepared the manuscript with assistance from all other co-authors.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to Han Htoon or Stephen K. Doorn.

Supplementary information

PDF files

  1. 1.

    Supplementary information

    Supplementary information