Controlling inelastic light scattering quantum pathways in graphene

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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.

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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.

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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.

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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.

Correspondence to Feng Wang.

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

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