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.

Controlling inelastic light scattering quantum pathways in graphene

Abstract

Inelastic light scattering spectroscopy has, since its first discovery1,2, been an indispensable tool in physical science for probing elementary excitations, such as phonons3, magnons4 and plasmons5 in both bulk and nanoscale materials. In the quantum mechanical picture of inelastic light scattering, incident photons first excite a set of intermediate electronic states, which then generate crystal elementary excitations and radiate energy-shifted photons6. The intermediate electronic excitations therefore have a crucial role as quantum pathways in inelastic light scattering, and this is exemplified by resonant Raman scattering6 and Raman interference7,8. The ability to control these excitation pathways can open up new opportunities to probe, manipulate and utilize inelastic light scattering. Here we achieve excitation pathway control in graphene with electrostatic doping. Our study reveals quantum interference between different Raman pathways in graphene: when some of the pathways are blocked, the one-phonon Raman intensity does not diminish, as commonly expected, but increases dramatically. This discovery sheds new light on the understanding of resonance Raman scattering in graphene. In addition, we demonstrate hot-electron luminescence9 in graphene as the Fermi energy approaches half the laser excitation energy. This hot luminescence, which is another form of inelastic light scattering, results from excited-state relaxation channels that become available only in heavily doped graphene.

Access options

Rent or Buy article

Get time limited or full article access on ReadCube.

from$8.99

All prices are NET prices.

Figure 1: Controlling the optical transitions in graphene with ion-gel gating.
Figure 2: Controlling inelastic light scattering with electrostatic doping.
Figure 3: Quantum interference between graphene Raman pathways.
Figure 4: Hot luminescence in graphene.

Accession codes

Primary accessions

Protein Data Bank

Data deposits

Coordinates and structure factors have been deposited in the Protein Data Bank with accession code 2L5A.

References

  1. 1

    Raman, C. V. A change of wave-length in light scattering. Nature 121, 619 (1928)

    CAS  ADS  Article  Google Scholar 

  2. 2

    Landsberg, G. & Mandelstam, L. Eine neue Erscheinung bei der Lichtzerstreuung in Krystallen. Naturwissenschaften 16, 557 (1928)

    CAS  Article  Google Scholar 

  3. 3

    Rao, A. M. et al. Diameter-selective Raman scattering from vibrational modes in carbon nanotubes. Science 275, 187–191 (1997)

    CAS  Article  Google Scholar 

  4. 4

    Devereaux, T. P. & Hackl, R. Inelastic light scattering from correlated electrons. Rev. Mod. Phys. 79, 175–233 (2007)

    CAS  ADS  Article  Google Scholar 

  5. 5

    Goñi, A. R. et al. One-dimensional plasmon dispersion and dispersionless intersubband excitations in GaAs quantum wires. Phys. Rev. Lett. 67, 3298–3301 (1991)

    ADS  Article  Google Scholar 

  6. 6

    Cardona, M. Light Scattering in Solids I 2nd edn (Springer, 1982)

    Google Scholar 

  7. 7

    Ralston, J. M., Wadsack, R. L. & Chang, R. K. Resonant cancelation of Raman scattering from CdS and Si. Phys. Rev. Lett. 25, 814–818. (1970)

  8. 8

    Basko, D. M. Calculation of the Raman G peak intensity in monolayer graphene: role of Ward identities. N. J. Phys. 11, 095011 (2009)

    Article  Google Scholar 

  9. 9

    Elsaesser, T., Shah, J., Rota, L. & Lugli, P. Initial thermalization of photoexcited carriers in GaAs studied by femtosecond luminescence spectroscopy. Phys. Rev. Lett. 66, 1757–1760 (1991)

    CAS  ADS  Article  Google Scholar 

  10. 10

    Novoselov, K. S. et al. Two-dimensional gas of massless Dirac fermions in graphene. Nature 438, 197–200 (2005)

    CAS  ADS  Article  Google Scholar 

  11. 11

    Zhang, Y. B., Tan, Y. W., Stormer, H. L. & Kim, P. Experimental observation of the quantum Hall effect and Berry's phase in graphene. Nature 438, 201–204 (2005)

    CAS  ADS  Article  Google Scholar 

  12. 12

    Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006)

    CAS  ADS  Article  Google Scholar 

  13. 13

    Pimenta, M. A. et al. Studying disorder in graphite-based systems by Raman spectroscopy. Phys. Chem. Chem. Phys. 9, 1276–1291 (2007)

    CAS  Article  Google Scholar 

  14. 14

    Das, A. et al. Monitoring dopants by Raman scattering in an electrochemically top-gated graphene transistor. Nature Nanotechnol. 3, 210–215 (2008)

    CAS  Article  Google Scholar 

  15. 15

    Dresselhaus, M. S., Jorio, A., Hofmann, M., Dresselhaus, G. & Saito, R. Perspectives on carbon nanotubes and graphene Raman spectroscopy. Nano Lett. 10, 751–758 (2010)

    CAS  ADS  Article  Google Scholar 

  16. 16

    Pisana, S. et al. Breakdown of the adiabatic Born-Oppenheimer approximation in graphene. Nature Mater. 6, 198–201 (2007)

    CAS  ADS  Article  Google Scholar 

  17. 17

    Yan, J., Zhang, Y. B., Kim, P. & Pinczuk, A. Electric field effect tuning of electron-phonon coupling in graphene. Phys. Rev. Lett. 98, 166802 (2007)

    ADS  Article  Google Scholar 

  18. 18

    Li, Z. Q. et al. Dirac charge dynamics in graphene by infrared spectroscopy. Nature Phys. 4, 532–535 (2008)

    CAS  ADS  Article  Google Scholar 

  19. 19

    Wang, F. et al. Gate-variable optical transitions in graphene. Science 320, 206–209 (2008)

    CAS  ADS  Article  Google Scholar 

  20. 20

    Zhang, Y. et al. Direct observation of a widely tunable bandgap in bilayer graphene. Nature 459, 820–823 (2009)

    CAS  ADS  Article  Google Scholar 

  21. 21

    Cho, J. H. et al. Printable ion-gel gate dielectrics for low-voltage polymer thin-film transistors on plastic. Nature Mater. 7, 900–906 (2008)

    CAS  ADS  Article  Google Scholar 

  22. 22

    Kim, B. J. et al. High-performance flexible graphene field effect transistors with ion gel gate dielectrics. Nano Lett. 10, 3464–3466 (2010)

    CAS  ADS  Article  Google Scholar 

  23. 23

    Lui, C. H., Mak, K. F., Shan, J. & Heinz, T. F. Ultrafast photoluminescence from graphene. Preprint at 〈http://arXiv.org/abs/1006.5769〉 (2010)

  24. 24

    Stoehr, R. J., Kolesov, R., Pflaum, J. & Wrachtrup, J. Fluorescence of laser created electron-hole plasma in graphene. Preprint at 〈http://arXiv.org/abs/1006.5434〉 (2010)

  25. 25

    Dresselhaus, M. S., Dresselhaus, G., Saito, R. & Jorio, A. Raman spectroscopy of carbon nanotubes. Phys. Rep. 409, 47–99 (2005)

    ADS  Article  Google Scholar 

  26. 26

    Basko, D. M., Piscanec, S. & Ferrari, A. C. Electron-electron interactions and doping dependence of the two-phonon Raman intensity in graphene. Phys. Rev. B 80, 165413 (2009)

    ADS  Article  Google Scholar 

  27. 27

    Kashuba, O. & Fal'ko, V. I. Signature of electronic excitations in the Raman spectrum of graphene. Phys. Rev. B 80, 241404(R) (2009)

    ADS  Article  Google Scholar 

  28. 28

    Ilani, S., Donev, L. A. K., Kindermann, M. & McEuen, P. L. Measurement of the quantum capacitance of interacting electrons in carbon nanotubes. Nature Phys. 2, 687–691 (2006)

    CAS  ADS  Article  Google Scholar 

  29. 29

    Wang, C. J., Shim, M. & Guyot-Sionnest, P. Electrochromic nanocrystal quantum dots. Science 291, 2390–2392 (2001)

    CAS  ADS  Article  Google Scholar 

  30. 30

    Li, X. S. et al. Large-area synthesis of high-quality and uniform graphene films on copper foils. Science 324, 1312–1314 (2009)

    CAS  ADS  Article  Google Scholar 

Download references

Acknowledgements

This work was supported by the US Department of Energy, Laboratory Directed Research and Development Program of Lawrence Berkeley National Laboratory under contract no. DE-AC02-05CH11231 (C.-F.C. and F.W.), by the Office of Basic Energy Sciences under contract nos DE-AC02-05CH11231 (B.W.B. and R.A.S.), DE-AC03-76SF0098 (Materials Science Division) (C.G., A.Z.) and DE-AC02-05CH11231 (Advanced Light Source), and by ONR MURI award N00014-09-1-1066 (J.H., C.-H.P., S.G.L., M.F.C.). C.-F.C. also acknowledges fellowship support from the National Science Council and National Tsing Hua University, Taiwan, under awards NSC98-2811-M-007-008 and NSC98-2120-M-007-004.

Author information

Affiliations

Authors

Contributions

F.W. designed the experiment; C.-F.C. and J.H. carried out optical measurements; B.G., C.G. and B.W.B. contributed to sample growth and fabrication; and C.-H.P., S.G.L. and F.W. performed theoretical analysis. All authors discussed the results and wrote the paper together.

Corresponding author

Correspondence to Feng Wang.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

The file contains Supplementary Data and Supplementary Figures 1-3 with legends. (PDF 361 kb)

PowerPoint slides

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Chen, CF., Park, CH., Boudouris, B. et al. Controlling inelastic light scattering quantum pathways in graphene. Nature 471, 617–620 (2011). https://doi.org/10.1038/nature09866

Download citation

Further reading

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

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