Intersubband Exciton Relaxation Dynamics in Single-Walled Carbon Nanotubes

Manzoni, Cristian; Alessio, Giovanni; Menna, Enzo; Meneghetti, Moreno; Lanzani, Guglielmo; Cerullo, Giulio

doi:10.1103/physrevlett.94.207401

Cited by 186 publications

(192 citation statements)

References 33 publications

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“…This is consistent with previous experimental studies 27,28 showing a intersubband coupling rate on the order of 20 ps −1 .…”

Section: Intersubband Transitionssupporting

confidence: 93%

“…This means that the S 22 population becomes negligible within a ps even though a small up-conversion from the S 11 state can be seen in the very early delays. Note that the same ultra-fast disappearance of the S 22 population is observed upon direct pumping of the S 22 transition or at higher energy (not shown), which confirms that the dynamics of the two types of excitons is very different, the upper one showing a much reduced lifetime 27,28 . We emphasize that the dynamics of ∆f 22 is quite singular as compared to the dynamics of the change of absorption of this band.…”

Section: ∆γsupporting

confidence: 63%

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Intraband and intersubband many-body effects in the nonlinear optical response of single-wall carbon nanotubes

Langlois¹,

Parret²,

Chassagneux³

et al. 2015

Phys. Rev. B

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We report on the nonlinear optical response of a mono-chiral sample of (6,5) single-wall carbon nanotubes by means of broad-band two-color pump-probe spectroscopy with selective excitation of the S11 excitons. By using a moment analysis of the transient spectra, we show that all the nonlinear features can be accurately accounted for by elementary deformations of the linear absorption spectrum. The photo-generation of S11 excitons induces a broadening and a blue shift of both the S11 and S22 excitonic transitions. In contrast, only the S11 transition shows a reduction of oscillator strength, ruling out population up-conversion. These nonlinear signatures result from many-body effects, including phase-space filling, wave-function renormalization and exciton collisions. This framework is sufficient to interpret the magnitude of the observed nonlinearities and stress the importance of intersubband exciton interactions. Remarkably, we show that these intersubband interactions have the same magnitude as the intraband ones and bring the major contribution to the photo-bleaching of the S22 excitonic transition upon S11 excitation through energy shift and broadening.

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“…This is consistent with previous experimental studies 27,28 showing a intersubband coupling rate on the order of 20 ps −1 .…”

Section: Intersubband Transitionssupporting

confidence: 93%

Section: ∆γsupporting

confidence: 63%

Intraband and intersubband many-body effects in the nonlinear optical response of single-wall carbon nanotubes

Langlois¹,

Parret²,

Chassagneux³

et al. 2015

Phys. Rev. B

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“…This corresponds to a dephasing time on the order of a few femtoseconds. This is consistent with the upper bound set by the very fast relaxation times observed in time-resolved spectroscopy for upper transitions [9,36]. However, this line-width remains almost one order of magnitude smaller than the binding energy of such excitons, which probably explains the observation of bound states.…”

Section: Semi-conducting Nanotubessupporting

confidence: 73%

Excitonic signatures in the optical response of single‐wall carbon nanotubes

Voisin¹,

Berger²,

Berciaud³

et al. 2012

Physica Status Solidi (b)

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The optical properties of single-wall carbon nanotubes (SWNTs) are dominated by the excitonic character of the transitions even at room temperature. The very peculiar properties of these excitons arise from both the one-dimensional (1D) nature of carbon nanotubes and from the electronic properties of graphene from which nanotubes are made. We first propose a brief qualitative review of the structure of the excitonic manifold and emphasize the role of dark states. We describe recent experimental investigations of this excitonic structure by means of temperature dependent PL measurements. We investigate the case of upper sub-bands and show that high-order optical transitions remain excitonic for large diameter nanotubes. A careful investigation of Rayleigh scattering spectra at the single nanotube level reveals clear exciton-phonon side-bands and Lorentzian line profiles for all semi-conducting nanotubes. In contrast, metallic nanotubes show an ambivalent behavior which is related to the reduced excitonic binding energy.Schematic of the exciton manifold in single-wall carbon nanotubes.

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“…The lowest frequency coherent phonons that can be photoexcited in SWNTs using ultrafast laser pulses are coherent RBM phonons with phonon wavevector q = 0 corresponding to a mode in which the diameter of the nanotube periodically expands and contracts. These coherent RBM phonons have been studied experimentally by several groups [51][52][53][54][55][56]. In addition to the lower frequency coherent RBM modes, higher frequency q = 0 coherent G mode phonons have also been observed [57,58].…”

Section: Introductionmentioning

confidence: 96%

Theory of coherent phonons in carbon nanotubes and graphene nanoribbons

Sanders

Nugraha

Sato

et al. 2013

J. Phys.: Condens. Matter

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We survey our recent theoretical studies on the generation and detection of coherent radial breathing mode (RBM) phonons in single-walled carbon nanotubes and coherent radial breathing like mode (RBLM) phonons in graphene nanoribbons. We present a microscopic theory for the electronic states, phonon modes, optical matrix elements and electron-phonon interaction matrix elements that allows us to calculate the coherent phonon spectrum. An extended tight-binding (ETB) model has been used for the electronic structure and a valence force field (VFF) model has been used for the phonon modes. The coherent phonon amplitudes satisfy a driven oscillator equation with the driving term depending on the photoexcited carrier density. We discuss the dependence of the coherent phonon spectrum on the nanotube chirality and type, and also on the graphene nanoribbon mod number and class (armchair versus zigzag). We compare these results with a simpler effective mass theory where reasonable agreement with the main features of the coherent phonon spectrum is found. In particular, the effective mass theory helps us to understand the initial phase of the coherent phonon oscillations for a given nanotube chirality and type. We compare these results to two different experiments for nanotubes: (i) micelle suspended tubes and (ii) aligned nanotube films. In the case of graphene nanoribbons, there are no experimental observations to date. We also discuss, based on the evaluation of the electron-phonon interaction matrix elements, the initial phase of the coherent phonon amplitude and its dependence on the chirality and type. Finally, we discuss previously unpublished results for coherent phonon amplitudes in zigzag nanoribbons obtained using an effective mass theory.

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Intersubband Exciton Relaxation Dynamics in Single-Walled Carbon Nanotubes

Cited by 186 publications

References 33 publications

Intraband and intersubband many-body effects in the nonlinear optical response of single-wall carbon nanotubes

Intraband and intersubband many-body effects in the nonlinear optical response of single-wall carbon nanotubes

Excitonic signatures in the optical response of single‐wall carbon nanotubes

Theory of coherent phonons in carbon nanotubes and graphene nanoribbons

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