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

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).

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Figure 1: Illustration of exciton localization and wavelength-tunable defect-state emission (E11* and E11*) in aryl-functionalized SWCNTs of varying (n,m).
Figure 2: Photoluminescence characteristics and photon antibunching properties of sp3 defect-state emission (E11* and E11*) from aryl-functionalized (6,5), (7,5) and (10,3) SWCNTs.
Figure 3: Global trends in single-photon emission statistics and dynamics over the complete range of SWCNT (n,m) and observed E11* emission wavelengths.

References

  1. 1

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

    ADS  Article  Google Scholar 

  2. 2

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

    ADS  Article  Google Scholar 

  3. 3

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

    Article  Google Scholar 

  4. 4

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

    Article  Google Scholar 

  5. 5

    Aharonovich, I., Englund, D. & Toth, M. Solid-state single-photon emitters. Nat. Photon. 10, 631–641 (2016).

    ADS  Article  Google Scholar 

  6. 6

    Miyazawa, T. 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).

    ADS  Article  Google Scholar 

  7. 7

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

    ADS  Article  Google Scholar 

  8. 8

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

    ADS  Article  Google Scholar 

  9. 9

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

    ADS  Article  Google Scholar 

  10. 10

    Chakraborty, C., Kinnischtzke, L., Goodfellow, K. M., Beams, R. & Vamivakas, A. N. Voltage-controlled quantum light from an atomically thin semiconductor. Nat. Nanotech. 10, 507–512 (2015).

    ADS  Article  Google Scholar 

  11. 11

    Tran, T. T., Bray, K., Ford, M. J., Toth, M. & Aharonovich, I. Quantum emission from hexagonal boron nitride monolayers. Nat. Nanotech. 11, 37–41 (2016).

    ADS  Article  Google Scholar 

  12. 12

    Ma, X., Hartmann, N. F., Baldwin, J. K. S., Doorn, S. K. & Htoon, H. Room-temperature single-photon generation from solitary dopants of carbon nanotubes. Nat. Nanotech. 10, 671–675 (2015).

    ADS  Article  Google Scholar 

  13. 13

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

    Article  Google Scholar 

  14. 14

    Hoegele, A., Galland, C., Winger, M. & Imamoglu, A. Photon antibunching in the photoluminescence spectra of a single carbon nanotube. Phys. Rev. Lett. 100, 217401 (2008).

    ADS  Article  Google Scholar 

  15. 15

    Walden-Newman, W., Sarpkaya, I. & Strauf, S. Quantum light signatures and nanosecond spectral diffusion from cavity-embedded carbon nanotubes. Nano Lett. 12, 1934–1941 (2012).

    ADS  Article  Google Scholar 

  16. 16

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

    ADS  Article  Google Scholar 

  17. 17

    Hofmann, M. S., Noe, J., Kneer, A., Crochet, J. J. & Hogele, A. Ubiquity of exciton localization in cryogenic carbon nanotubes. Nano Lett. 16, 2958–2962 (2016).

    ADS  Article  Google Scholar 

  18. 18

    Ghosh, S., Bachilo, S. M., Simonette, R. A., Beckingham, K. M. & Weisman, R. B. Oxygen doping modifies near-infrared band gaps in fluorescent single-walled carbon nanotubes. Science 330, 1656–1659 (2010).

    ADS  Article  Google Scholar 

  19. 19

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

    Article  Google Scholar 

  20. 20

    Ma, X., Baldwin, J. K. S., Hartmann, N. F., Doorn, S. K. & Htoon, H. Solid-state approach for fabrication of photostable, oxygen-doped carbon nanotubes. Adv. Funct. Mater. 25, 6157–6164 (2015).

    Article  Google Scholar 

  21. 21

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

    ADS  Article  Google Scholar 

  22. 22

    Avouris, P., Freitag, M. & Perebeinos, V. Carbon nanotube photonics and optoelectronics. Nat. Photon. 2, 341–350 (2008).

    ADS  Article  Google Scholar 

  23. 23

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

    ADS  Article  Google Scholar 

  24. 24

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

    ADS  Article  Google Scholar 

  25. 25

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

    ADS  Article  Google Scholar 

  26. 26

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

    ADS  Article  Google Scholar 

  27. 27

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

    ADS  Article  Google Scholar 

  28. 28

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

    Article  Google Scholar 

  29. 29

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

    Article  Google Scholar 

  30. 30

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

    ADS  Article  Google Scholar 

  31. 31

    Liu, X. 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).

    ADS  Article  Google Scholar 

  32. 32

    Chu, X.-L., Gotzinger, S. & Sandoghdar, V. A single molecule as a high-fidelity photon gun for producing intensity-squeezed light. Nat. Photon. 11, 58–62 (2017).

    ADS  Article  Google Scholar 

  33. 33

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

    ADS  Article  Google Scholar 

  34. 34

    Aharonovich, I. & Neu, E. Diamond nanophotonics. Adv. Opt. Mater. 2, 911–928 (2014).

    Article  Google Scholar 

  35. 35

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

    Article  Google Scholar 

  36. 36

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

    ADS  Article  Google Scholar 

  37. 37

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

    Article  Google Scholar 

  38. 38

    Brady, G. J. 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).

    Article  Google Scholar 

  39. 39

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

    Article  Google Scholar 

  40. 40

    Shiraki, T., Shiraishi, T., Juhasz, G. & Nakashima, N. Emergence of new red-shifted carbon nanotube photoluminescence based on proximal doped-site design. Sci. Rep. 6, 28393 (2016).

    ADS  Article  Google Scholar 

  41. 41

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

    Article  Google Scholar 

  42. 42

    Subbaiyan, N. K. 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).

    Article  Google Scholar 

  43. 43

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

    Article  Google Scholar 

  44. 44

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

    ADS  Article  Google Scholar 

  45. 45

    Powell, L. R., Piao, Y. & Wang, Y. Optical excitation of carbon nanotubes drives localized diazonium reactions. J. Phys. Chem. Lett. 7, 3690–3694 (2016).

    Article  Google Scholar 

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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.

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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.

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Correspondence to Han Htoon or Stephen K. Doorn.

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He, X., Hartmann, N., Ma, X. et al. Tunable room-temperature single-photon emission at telecom wavelengths from sp3 defects in carbon nanotubes. Nature Photon 11, 577–582 (2017). https://doi.org/10.1038/nphoton.2017.119

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