Giant intrinsic photoresponse in pristine graphene

Matters Arising to this article was published on 17 February 2020

Abstract

When the Fermi level is aligned with the Dirac point of graphene, reduced charge screening greatly enhances electron–electron scattering1,2,3,4,5. In an optically excited system, the kinematics of electron–electron scattering in Dirac fermions is predicted to give rise to novel optoelectronic phenomena6,7,8,9,10,11. In this paper, we report on the observation of an intrinsic photocurrent in graphene, which occurs in a different parameter regime from all the previously observed photothermoelectric or photovoltaic photocurrents in graphene12,13,14,15,16,17,18,19,20: the photocurrent emerges exclusively at the charge neutrality point, requiring no finite doping. Unlike other photocurrent types that are enhanced near p–n or contact junctions, the photocurrent observed in our work arises near the edges/corners. By systematic data analyses, we show that the phenomenon stems from the unique electron–electron scattering kinematics in charge-neutral graphene. Our results not only highlight the intriguing electron dynamics in the optoelectronic response of Dirac fermions, but also offer a new scheme for photodetection and energy harvesting applications based on intrinsic, charge-neutral Dirac fermions.

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Fig. 1: Intrinsic long-range edge photocurrent in charge-neutral graphene with different geometries.
Fig. 2: Distance and gate dependence of the CNP photocurrent in graphene.
Fig. 3: Collection of the edge photocurrent in graphene within a Shockley–Ramo-type scheme.
Fig. 4: Suppression of photocurrent relaxation in charge-neutral graphene.

References

  1. 1.

    Neto, A. C., Guinea, F., Peres, N., Novoselov, K. S. & Geim, A. K. The electronic properties of graphene. Rev. Mod. Phys. 81, 109–162 (2009).

    Article  Google Scholar 

  2. 2.

    Sarma, S. D., Adam, S., Hwang, E. & Rossi, E. Electronic transport in two-dimensional graphene. Rev. Mod. Phys. 83, 407–470 (2011).

    Article  Google Scholar 

  3. 3.

    Kotov, V. N., Uchoa, B., Pereira, V. M., Guinea, F. & Neto, A. C. Electron–electron interactions in graphene: current status and perspectives. Rev. Mod. Phys. 84, 1067–1126 (2012).

    CAS  Article  Google Scholar 

  4. 4.

    Crossno, J. et al. Observation of the Dirac fluid and the breakdown of the Wiedemann–Franz law in graphene. Science 351, 1058–1061 (2016).

    CAS  Article  Google Scholar 

  5. 5.

    Bandurin, D. et al. Negative local resistance caused by viscous electron backflow in graphene. Science 351, 1055–1058 (2016).

    CAS  Article  Google Scholar 

  6. 6.

    Fritz, L., Schmalian, J., Müller, M. & Sachdev, S. Quantum critical transport in clean graphene. Phys. Rev. B 78, 085416 (2008).

    Article  Google Scholar 

  7. 7.

    Foster, M. S. & Aleiner, I. L. Slow imbalance relaxation and thermoelectric transport in graphene. Phys. Rev. B 79, 085415 (2009).

    Article  Google Scholar 

  8. 8.

    Tomadin, A., Brida, D., Cerullo, G., Ferrari, A. C. & Polini, M. Nonequilibrium dynamics of photoexcited electrons in graphene: collinear scattering, Auger processes, and the impact of screening. Phys. Rev. B 88, 035430 (2013).

    Article  Google Scholar 

  9. 9.

    Brida, D. et al. Ultrafast collinear scattering and carrier multiplication in graphene. Nat. Commun. 4, 1987 (2013).

    CAS  Article  Google Scholar 

  10. 10.

    Junck, A., Refael, G. & von Oppen, F. Current amplification and relaxation in Dirac systems. Phys. Rev. B 90, 245110 (2014).

    CAS  Article  Google Scholar 

  11. 11.

    Lewandowski, C. & Levitov, L. Photoexcitation cascade and quantum-relativistic jets in graphene. Phys. Rev. Lett. 120, 076601 (2018).

    CAS  Article  Google Scholar 

  12. 12.

    Lee, E. J., Balasubramanian, K., Weitz, R. T., Burghard, M. & Kern, K. Contact and edge effects in graphene devices. Nat. Nanotech. 3, 486–490 (2008).

    CAS  Article  Google Scholar 

  13. 13.

    Park, J., Ahn, Y. & Ruiz-Vargas, C. Imaging of photocurrent generation and collection in single-layer graphene. Nano Lett. 9, 1742–1746 (2009).

    CAS  Article  Google Scholar 

  14. 14.

    Xu, X., Gabor, N. M., Alden, J. S., van der Zande, A. M. & McEuen, P. L. Photo-thermoelectric effect at a graphene interface junction. Nano Lett. 10, 562–566 (2009).

    Article  Google Scholar 

  15. 15.

    Gabor, N. M. et al. Hot carrier-assisted intrinsic photoresponse in graphene. Science 334, 648–652 (2011).

    CAS  Article  Google Scholar 

  16. 16.

    Sun, D. et al. Ultrafast hot-carrier-dominated photocurrent in graphene. Nat. Nanotech. 7, 114–118 (2012).

    CAS  Article  Google Scholar 

  17. 17.

    Freitag, M., Low, T., Xia, F. & Avouris, P. Photoconductivity of biased graphene. Nat. Photon. 7, 53–59 (2013).

    CAS  Article  Google Scholar 

  18. 18.

    Tielrooij, K. et al. Photoexcitation cascade and multiple hot-carrier generation in graphene. Nat. Phys. 9, 248–252 (2013).

    CAS  Article  Google Scholar 

  19. 19.

    Graham, M. W., Shi, S.-F., Ralph, D. C., Park, J. & McEuen, P. L. Photocurrent measurements of supercollision cooling in graphene. Nat. Phys. 9, 103–108 (2013).

    CAS  Article  Google Scholar 

  20. 20.

    Ma, Q. et al. Competing channels for hot-electron cooling in graphene. Phys. Rev. Lett. 112, 247401 (2014).

    Article  Google Scholar 

  21. 21.

    König-Otto, J. et al. Slow noncollinear Coulomb scattering in the vicinity of the Dirac point in graphene. Phys. Rev. Lett. 117, 087401 (2016).

    Article  Google Scholar 

  22. 22.

    Sun, D. et al. Coherent control of ballistic photocurrents in multilayer epitaxial graphene using quantum interference. Nano Lett. 10, 1293–1296 (2010).

    CAS  Article  Google Scholar 

  23. 23.

    Sun, D. et al. Current relaxation due to hot carrier scattering in graphene. New J. Phys. 14, 105012 (2012).

    Article  Google Scholar 

  24. 24.

    Woessner, A. et al. Near-field photocurrent nanoscopy on bare and encapsulated graphene. Nat. Commun. 7, 10783 (2016).

    CAS  Article  Google Scholar 

  25. 25.

    Cao, H. et al. Photo-Nernst current in graphene. Nat. Phys. 12, 236–239 (2016).

    CAS  Article  Google Scholar 

  26. 26.

    Wu, S. et al. Multiple hot-carrier collection in photo-excited graphene moire superlattices. Sci. Adv. 2, e1600002 (2016).

    Article  Google Scholar 

  27. 27.

    Kim, Y. D. et al. Focused-laser-enabled p–n junctions in graphene field-effect transistors. ACS Nano 7, 5850–5857 (2013).

    CAS  Article  Google Scholar 

  28. 28.

    Rao, G., Freitag, M., Chiu, H.-Y., Sundaram, R. S. & Avouris, P. Raman and photocurrent imaging of electrical stress-induced p–n junctions in graphene. ACS Nano 5, 5848–5854 (2011).

    CAS  Article  Google Scholar 

  29. 29.

    Song, J. C. & Levitov, L. S. Shockley–Ramo theorem and long-range photocurrent response in gapless materials. Phys. Rev. B 90, 075415 (2014).

    Article  Google Scholar 

  30. 30.

    Van Ostaay, J., Akhmerov, A., Beenakker, C. & Wimmer, M. Dirac boundary condition at the reconstructed zigzag edge of graphene. Phys. Rev. B 84, 195434 (2011).

    Article  Google Scholar 

  31. 31.

    Allen, M. T. et al. Spatially resolved edge currents and guided-wave electronic states in graphene. Nat. Phys. 12, 128–133 (2015).

    Article  Google Scholar 

  32. 32.

    Shalom, M. B. et al. Quantum oscillations of the critical current and high-field superconducting proximity in ballistic graphene. Nat. Phys. 12, 318–322 (2016).

    Article  Google Scholar 

  33. 33.

    Song, J. C., Tielrooij, K. J., Koppens, F. H. & Levitov, L. S. Photoexcited carrier dynamics and impact-excitation cascade in graphene. Phys. Rev. B 87, 155429 (2013).

    Article  Google Scholar 

Download references

Acknowledgements

We thank L. Levitov, V. Phong, F. Koppens, K.-J. Tielrooij, M. Lundeberg, A. Woessner and O. Shtanko for discussions. We also thank Y. Sun and B. Han for help with device fabrication. Work in the P.J.-H. group was partly supported by the Center for Excitonics, an Energy Frontier Research Center funded by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) under award number DESC0001088 (fabrication and measurement) and partly through AFOSR grant number FA9550-16-1-0382 (data analysis), as well as the Gordon and Betty Moore Foundation’s EPiQS Initiative through grant number GBMF4541 to P.J.-H. This work made use of the MRSEC Shared Experimental Facilities at MIT, supported by the National Science Foundation (NSF) under award number DMR-14-19807 and of Harvard CNS, supported by NSF ECCS under award number 1541959. Y.C., Y.L., T.P., W.F., J.K., S.-Y.X. and N.G. acknowledge funding support by the STC Center for Integrated Quantum Materials, NSF grant number DMR-1231319. Y.L. and T.P. also acknowledge the US Army Research Office through the MIT Institute for Soldier Nanotechnologies, under award number W911NF-18-2-0048. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, JSPS KAKENHI grant numbers JP18K19136 and the CREST (JPMJCR15F3), JST. N.M.G. is supported by the Air Force Office of Scientific Research Young Investigator Program (YIP) award no. FA9550-16-1-0216 and by the NSF Division of Materials Research CAREER award no. 1651247. N.M.G. also acknowledges support through a Cottrell Scholar Award, and through the Canadian Institute for Advanced Research (CIFAR) Azrieli Global Scholar Award. J.C.W.S. acknowledges support from the Singapore National Research Foundation (NRF) under NRF fellowship award NRF-NRFF2016-05 and a Nanyang Technological University (NTU) start-up grant (NTU-SUG).

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Contributions

Q.M. and N.M.G. conceived the experiment. Q.M. and N.L.N. fabricated the devices. Y.L. fabricated additional devices shown in the Supplementary Information under the supervision of T.P. Q.M., T.H.D. and N.M.G. carried out the photocurrent measurements. Q.M., C.H.L. and Y.C. analysed and simulated the data under supervision from P.J-.H. W.F. and J.K. grew the CVD graphene. K.W. and T.T. synthesized the BN crystals. J.C.W.S. and J.F.K. contributed to theoretical discussions. Q.M., C.H.L., J.C.W.S., S.-Y.X., N.G. and P.J-.H. co-wrote the paper with input from all the authors.

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Correspondence to Nathaniel M. Gabor or Pablo Jarillo-Herrero.

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Ma, Q., Lui, C.H., Song, J.C.W. et al. Giant intrinsic photoresponse in pristine graphene. Nature Nanotech 14, 145–150 (2019). https://doi.org/10.1038/s41565-018-0323-8

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