12,986 research outputs found
Exciton resonances quench the photoluminescence of zigzag carbon nanotubes
We show that the photoluminescence intensity of single-walled carbon
nanotubes is much stronger in tubes with large chiral angles - armchair tubes -
because exciton resonances make the luminescence of zigzag tubes intrinsically
weak. This exciton-exciton resonance depends on the electronic structure of the
tubes and is found more often in nanotubes of the +1 family. Armchair tubes do
not necessarily grow preferentially with present growth techniques; they just
have stronger luminescence. Our analysis allows to normalize photoluminescence
intensities and find the abundance of nanotube chiralities in macroscopic
samples.Comment: 4 pages and 2 supplementary pages; 6 figure
Modeling Surface-Enhanced Spectroscopy With Perturbation Theory
Theoretical modeling of surface-enhanced Raman scattering (SERS) is of central importance for unraveling the interplay of underlying processes and a predictive design of SERS substrates. In this work we model the plasmonic enhancement mechanism of SERS with perturbation theory. We consider the excitation of plasmonic modes as an integral part of the Raman process and model SERS as higher-order Raman scattering. Additional resonances appear in the Raman cross section which correspond to the excitation of plasmons at the wavelengths of the incident and the Raman-scattered light. The analytic expression for the Raman cross section can be used to explain the outcome of resonance Raman measurements on SERS analytes as we demonstrate by comparison to experimental data. We also implement the theory to calculate the optical absorption cross section of plasmonic nanoparticles. From a comparison to experimental cross sections, we show that the coupling matrix elements need to be renormalized by a factor that accounts for the depolarization by the bound electrons and interband transitions in order to obtain the correct magnitude. With model calculations we demonstrate that interference of different scattering channels is key to understand the excitation energy dependence of the SERS enhancement for enhancement factors below 103
Symmetry properties of vibrational modes in graphene nanoribbons
We present symmetry properties of the lattice vibrations of graphene
nanoribbons with pure armchair (AGNR) and zigzag edges (ZGNR). In
non-symmorphic nanoribbons the phonon modes at the edge of the Brillouin zone
are twofold degenerate, whereas the phonon modes in symmorphic nanoribbons are
non-degenerate. We identified the Raman-active and infrared-active modes. We
predict 3N and 3(N+1) Raman-active modes for N-ZGNRs and N-AGNRs, respectively
(N is the number of dimers per unit cell). These modes can be used for the
experimental characterization of graphene nanoribbons. Calculations based on
density functional theory suggest that the frequency splitting of the LO and TO
in AGNRs (corresponding to the E2g mode in graphene) exhibits characteristic
width and family dependence. Further, all graphene nanoribbons have a
Raman-active breathing-like mode, the frequency of which is inversely
proportional to the nanoribbon width and thus might be used for experimental
determination of the width of graphene nanoribbons.Comment: 10 pages, 5 figure
Theory of double-resonant Raman spectra in graphene: intensity and line shape of defect-induced and two-phonon bands
We calculate the double resonant (DR) Raman spectrum of graphene, and
determine the lines associated to both phonon-defect processes, and two-phonons
ones. Phonon and electronic dispersions reproduce calculations based on density
functional theory corrected with GW. Electron-light, -phonon, and -defect
scattering matrix elements and the electronic linewidth are explicitly
calculated. Defect-induced processes are simulated by considering different
kind of idealized defects. For an excitation energy of eV, the
agreement with measurements is very good and calculations reproduce: the
relative intensities among phonon-defect or among two-phonon lines; the
measured small widths of the D, , 2D and lines; the line shapes; the
presence of small intensity lines in the 1800, 2000 cm range. We
determine how the spectra depend on the excitation energy, on the light
polarization, on the electronic linewidth, on the kind of defects and on their
concentration. According to the present findings, the intensity ratio between
the and 2D lines can be used to determine experimentally the electronic
linewidth. The intensity ratio between the and lines depends on the
kind of model defect, suggesting that this ratio could possibly be used to
identify the kind of defects present in actual samples. Charged impurities
outside the graphene plane provide an almost undetectable contribution to the
Raman signal
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