Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

Exceptionally clean single-electron transistors from solutions of molecular graphene nanoribbons

Abstract

Only single-electron transistors with a certain level of cleanliness, where all states can be properly accessed, can be used for quantum experiments. To reveal their exceptional properties, carbon nanomaterials need to be stripped down to a single element: graphene has been exfoliated into a single sheet, and carbon nanotubes can reveal their vibrational, spin and quantum coherence properties only after being suspended across trenches1,2,3. Molecular graphene nanoribbons4,5,6 now provide carbon nanostructures with single-atom precision but suffer from poor solubility, similar to carbon nanotubes. Here we demonstrate the massive enhancement of the solubility of graphene nanoribbons by edge functionalization, to yield ultra-clean transport devices with sharp single-electron features. Strong electron–vibron coupling leads to a prominent Franck–Condon blockade, and the atomic definition of the edges allows identifying the associated transverse bending mode. These results demonstrate how molecular graphene can yield exceptionally clean electronic devices directly from solution. The sharpness of the electronic features opens a path to the exploitation of spin and vibrational properties in atomically precise graphene nanostructures.

This is a preview of subscription content, access via your institution

Access options

Rent or buy this article

Get just this article for as long as you need it

$39.95

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Synthetic design.
Fig. 2: Debundling of the molecular nanoribbons.
Fig. 3: Enhancement of the quantum transport.
Fig. 4: Electron–vibron coupling in nanoribbons with enhanced solubility.

Data availability

The data supporting the findings of this study are available within the Article and its Supplementary Information, and are deposited and available online within the Bodleian Library of Oxford. No custom code is used.

References

  1. Cao, J., Wang, Q. & Dai, H. Electron transport in very clean, as-grown suspended carbon nanotubes. Nat. Mater. 4, 745–749 (2005).

    Article  CAS  Google Scholar 

  2. Jarillo-Herrero, P., Sapmaz, S., Dekker, C., Kouwenhoven, L. P. & van der Zant, H. S. Electron–hole symmetry in a semiconducting carbon nanotube quantum dot. Nature 429, 389–392 (2004).

    Article  CAS  Google Scholar 

  3. Minot, E. D., Yaish, Y., Sazonova, V. & Mceuen, P. L. Determination of electron orbital magnetic moments in carbon nanotubes. Nature 428, 536–539 (2004).

    Article  CAS  Google Scholar 

  4. Cai, J. et al. Atomically precise bottom-up fabrication of graphene nanoribbons. Nature 466, 470–473 (2010).

    Article  CAS  Google Scholar 

  5. Narita, A. et al. Synthesis of structurally well-defined and liquid-phase-processable graphene nanoribbons. Nat. Chem. 6, 126–132 (2014).

    Article  CAS  Google Scholar 

  6. Yang, W., Lucotti, A., Tommasini, M. & Chalifoux, W. A. Bottom-up synthesis of soluble and narrow graphene nanoribbons using alkyne benzannulations. J. Am. Chem. Soc. 138, 9137–9144 (2016).

    Article  CAS  Google Scholar 

  7. Li, X., Wang, X., Zhang, L., Lee, S. & Dai, H. Chemically derived, ultrasmooth graphene nanoribbon semiconductors. Science 319, 1229–1232 (2008).

    Article  CAS  Google Scholar 

  8. Jiao, L., Wang, X., Diankov, G., Wang, H. & Dai, H. Facile synthesis of high-quality graphene nanoribbons. Nat. Nano. 5, 321–325 (2010).

    Article  CAS  Google Scholar 

  9. Wang, X. et al. Graphene nanoribbons with smooth edges behave as quantum wires. Nat. Nano 6, 563–567 (2011).

    Article  CAS  Google Scholar 

  10. Jiao, L., Zhang, L., Wang, X., Diankov, G. & Dai, H. Narrow graphene nanoribbons from carbon nanotubes. Nature 458, 877–880 (2009).

    Article  CAS  Google Scholar 

  11. Laird, E. A. et al. Quantum transport in carbon nanotubes. Rev. Mod. Phys. 87, 703–764 (2015).

    Article  CAS  Google Scholar 

  12. Hanson, R., Kouwenhoven, L. P., Petta, J. R., Tarucha, S. & Vandersypen, L. M. K. Spins in few-electron quantum dots. Rev. Mod. Phys. 79, 1217–1265 (2007).

    Article  CAS  Google Scholar 

  13. Llinas, J. P. et al. Short-channel field-effect transistors with 9-atom and 13-atom wide graphene nanoribbons. Nat. Commun. 8, 633 (2017).

    Article  Google Scholar 

  14. Nguyen, G. D. et al. Atomically precise graphene nanoribbon heterojunctions from a single molecular precursor. Nat. Nano. 12, 1077–1082 (2017).

    Article  CAS  Google Scholar 

  15. Bischoff, D. et al. Localized charge carriers in graphene nanodevices. Appl. Phys. Rev. 2, 031301 (2015).

    Article  Google Scholar 

  16. Ponomarenko, L. A. et al. Chaotic Dirac billiard in graphene quantum dots. Science 320, 356–358 (2008).

    Article  CAS  Google Scholar 

  17. Slota, M. et al. Magnetic edge states and coherent manipulation of graphene nanoribbons. Nature 557, 691–695 (2018).

    Article  CAS  Google Scholar 

  18. Yang, J. et al. The influence of the molecular packing on the room temperature phosphorescence of purely organic luminogens. Nat. Commun. 9, 840 (2018).

    Article  Google Scholar 

  19. Tan, P. H. et al. Photoluminescence spectroscopy of carbon nanotube bundles: evidence for exciton energy transfer. Phys. Rev. Lett. 99, 137402 (2007).

    Article  CAS  Google Scholar 

  20. Richter, N. et al. Charge transport mechanism in networks of armchair graphene nanoribbons. Sci. Rep. 10, 1988 (2020).

    Article  CAS  Google Scholar 

  21. Shylau, A. A., Kłos, J. W. & Zozoulenko, I. V. Capacitance of graphene nanoribbons. Phys. Rev. B 80, 205402 (2009).

    Article  Google Scholar 

  22. Gehring, P. et al. Distinguishing lead and molecule states in graphene-based single-electron transistors. ACS Nano 11, 5325–5331 (2017).

    Article  CAS  Google Scholar 

  23. Leturcq, R. et al. Franck–Condon blockade in suspended carbon nanotube quantum dots. Nat. Phys. 5, 327–331 (2009).

    Article  CAS  Google Scholar 

  24. Sapmaz, S., Jarillo-Herrero, P., Blanter, Y. M., Dekker, C. & Van Der Zant, H. S. J. Tunneling in suspended carbon nanotubes assisted by longitudinal phonons. Phys. Rev. Lett. 96, 026801 (2006).

    Article  CAS  Google Scholar 

  25. Zhou, G., Cen, C., Wang, S., Deng, M. & Prezhdo, O. V. Electron–phonon scattering is much weaker in carbon nanotubes than in graphene nanoribbons. J. Phys. Chem. Lett. 10, 7179–7187 (2019).

    Article  CAS  Google Scholar 

  26. Savin, A. V. & Kivshar, Y. S. Localized vibrations of graphene nanoribbons. Low. Temp. Phys. 42, 703–710 (2016).

    Article  CAS  Google Scholar 

  27. Thomas, J. O. et al. Understanding resonant charge transport through weakly coupled single-molecule junctions. Nat. Commun. 10, 4628 (2019).

    Article  Google Scholar 

  28. Droth, M. & Burkard, G. Acoustic phonons and spin relaxation in graphene nanoribbons. Phys. Rev. B 84, 155404 (2011).

    Article  Google Scholar 

Download references

Acknowledgements

We thank the European Union (ERC-CoG-773048-MMGNRs), the Royal Society (University Research Fellowship and grant), the Engineering and Physical Sciences Research Council (EP/N017188/1-QuEEN), the Norwegian State Educational Loan Fund (Keeley and Norwegian scholarships to Wadham College Oxford) and the Max Planck Gesellshaft (MPG) for financial support. We thank University of Norwich for the use of the atomic force microscopy instrument and Oxford-Advanced Research Computing (ARC) for computational time.

Funding

Open access funding provided by Max Planck Society.

Author information

Authors and Affiliations

Authors

Contributions

W.N., A.N., Y.M. and J.L. synthesized the nanoribbons and performed the photoluminescence measurements. J.N. and A.G. performed the atomic force microscopy measurements. A.L., P.G., A.G., C.S.L., J.M. and T.P. nanofabricated the devices. S.S., A.G., T.P., J.N. and A.L. performed the transport measurements. F.K. calculated the vibrations. S.S. and L.B. performed the data analysis and wrote the manuscript. All authors contributed to the final version of the manuscript.

Corresponding authors

Correspondence to Xinliang Feng or Lapo Bogani.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Materials thanks Hongjie Dai and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–20, Table 1 and Discussion.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Niu, W., Sopp, S., Lodi, A. et al. Exceptionally clean single-electron transistors from solutions of molecular graphene nanoribbons. Nat. Mater. 22, 180–185 (2023). https://doi.org/10.1038/s41563-022-01460-6

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41563-022-01460-6

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing