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.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 51 print issues and online access
$199.00 per year
only $3.90 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Raman, C. V. A change of wave-length in light scattering. Nature 121, 619 (1928)
Landsberg, G. & Mandelstam, L. Eine neue Erscheinung bei der Lichtzerstreuung in Krystallen. Naturwissenschaften 16, 557 (1928)
Rao, A. M. et al. Diameter-selective Raman scattering from vibrational modes in carbon nanotubes. Science 275, 187–191 (1997)
Devereaux, T. P. & Hackl, R. Inelastic light scattering from correlated electrons. Rev. Mod. Phys. 79, 175–233 (2007)
Goñi, A. R. et al. One-dimensional plasmon dispersion and dispersionless intersubband excitations in GaAs quantum wires. Phys. Rev. Lett. 67, 3298–3301 (1991)
Cardona, M. Light Scattering in Solids I 2nd edn (Springer, 1982)
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)
Basko, D. M. Calculation of the Raman G peak intensity in monolayer graphene: role of Ward identities. N. J. Phys. 11, 095011 (2009)
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)
Novoselov, K. S. et al. Two-dimensional gas of massless Dirac fermions in graphene. Nature 438, 197–200 (2005)
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)
Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006)
Pimenta, M. A. et al. Studying disorder in graphite-based systems by Raman spectroscopy. Phys. Chem. Chem. Phys. 9, 1276–1291 (2007)
Das, A. et al. Monitoring dopants by Raman scattering in an electrochemically top-gated graphene transistor. Nature Nanotechnol. 3, 210–215 (2008)
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)
Pisana, S. et al. Breakdown of the adiabatic Born-Oppenheimer approximation in graphene. Nature Mater. 6, 198–201 (2007)
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)
Li, Z. Q. et al. Dirac charge dynamics in graphene by infrared spectroscopy. Nature Phys. 4, 532–535 (2008)
Wang, F. et al. Gate-variable optical transitions in graphene. Science 320, 206–209 (2008)
Zhang, Y. et al. Direct observation of a widely tunable bandgap in bilayer graphene. Nature 459, 820–823 (2009)
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)
Kim, B. J. et al. High-performance flexible graphene field effect transistors with ion gel gate dielectrics. Nano Lett. 10, 3464–3466 (2010)
Lui, C. H., Mak, K. F., Shan, J. & Heinz, T. F. Ultrafast photoluminescence from graphene. Preprint at 〈http://arXiv.org/abs/1006.5769〉 (2010)
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)
Dresselhaus, M. S., Dresselhaus, G., Saito, R. & Jorio, A. Raman spectroscopy of carbon nanotubes. Phys. Rep. 409, 47–99 (2005)
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)
Kashuba, O. & Fal'ko, V. I. Signature of electronic excitations in the Raman spectrum of graphene. Phys. Rev. B 80, 241404(R) (2009)
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)
Wang, C. J., Shim, M. & Guyot-Sionnest, P. Electrochromic nanocrystal quantum dots. Science 291, 2390–2392 (2001)
Li, X. S. et al. Large-area synthesis of high-quality and uniform graphene films on copper foils. Science 324, 1312–1314 (2009)
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
Authors and Affiliations
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
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)
Rights 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
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nature09866
This article is cited by
-
Transfer learning for inverse design of tunable graphene-based meta-surfaces
Journal of Materials Science (2024)
-
Quantum interference directed chiral raman scattering in two-dimensional enantiomers
Nature Communications (2022)
-
Full 2π tunable phase modulation using avoided crossing of resonances
Nature Communications (2022)
-
Axial Higgs mode detected by quantum pathway interference in RTe3
Nature (2022)
-
Tunable broadband polarization converters based on coded graphene metasurfaces
Scientific Reports (2021)
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.