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dc.contributor.authorHároz, Erik H.
Duque, Juan G.
Barros, Eduardo B.
Telg, Hagen
Simpson, Jeffrey R.
Walker, Angela R. Hight
Khripin, Constantine Y.
Fagan, Jeffrey A.
Tu, Xiaomin
Zheng, Ming
Kono, Junichiro
Doorn, Stephen K.
dc.date.accessioned 2015-07-09T15:30:05Z
dc.date.available 2015-07-09T15:30:05Z
dc.date.issued 2015
dc.identifier.citation Hároz, Erik H., Duque, Juan G., Barros, Eduardo B., et al.. "Asymmetric excitation profiles in the resonance Raman response of armchair carbon nanotubes." Physical Review B, 91, (2015) American Physical Society: 205446. http://dx.doi.org/10.1103/PhysRevB.91.205446.
dc.identifier.urihttps://hdl.handle.net/1911/80859
dc.description.abstract We performed tunable resonance Raman spectroscopy on samples highly enriched in the (5,5), (6,6), (7,7), and (8,8) armchair structures of metallic single-wall carbon nanotubes. We present Raman excitation profiles (REPs) for both the radial breathing mode and G-band phonons of these species. G-band excitation profiles are shown to resolve the expected incoming and outgoing resonances of the scattering process. Notably, the profiles are highly asymmetric, with the higher-energy outgoing resonance weaker than the incoming resonance. These results are comparable to the asymmetric excitation profiles observed previously in semiconducting nanotubes, introduce a different electronic type, and broaden the structural range over which the asymmetry is found to exist. Modeling of the behavior with a third-order quantum model that accounts for the k dependence in energies and matrix elements, without including excitonic effects, is found to be insufficient for reproducing the observed asymmetry. We introduce an alternative fifth-order model in which the REP asymmetry arises from quantum interference introduced by phonon-mediated state mixing between the EM11 and K-momentum excitons. Such state mixing effectively introduces a nuclear coordinate dependence in the transition dipole moment and thus may be viewed as a non-Condon effect from a molecular perspective. This result unifies a molecularlike picture of nanotube transitions (introduced by their excitonic nature) with a condensed matter approach for describing their behavior.
dc.language.iso eng
dc.publisher American Physical Society
dc.rights Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
dc.title Asymmetric excitation profiles in the resonance Raman response of armchair carbon nanotubes
dc.type Journal article
dc.contributor.funder U.S. Department of Energy, Office of Basic Energy Sciences
dc.contributor.funder Welch Foundation
dc.contributor.funder National Science Foundation
dc.contributor.funder National Council for Scientific and Technological Development
dc.citation.journalTitle Physical Review B
dc.citation.volumeNumber 91
dc.type.dcmi Text
dc.identifier.doihttp://dx.doi.org/10.1103/PhysRevB.91.205446
dc.identifier.grantID DEFG02-06ER46308 (U.S. Department of Energy, Office of Basic Energy Sciences)
dc.identifier.grantID C-1509 (Welch Foundation)
dc.identifier.grantID 470492/2012-0 (National Council for Scientific and Technological Development)
dc.identifier.grantID 245640/2012-6 (National Council for Scientific and Technological Development)
dc.identifier.grantID CMS-060950 (National Science Foundation)
dc.type.publication publisher version
dc.citation.firstpage 205446


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