Effects of Energy Exchange on Vibrational Dephasing Times in Raman Scattering

Harris, Charles B.; Shelby, R. M.; Cornelius, P. A.

doi:10.1103/physrevlett.38.1415

Cited by 193 publications

(49 citation statements)

References 8 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…(2) was used to determine the temperature variation of the low-frequency oscillator, and the complex frequency of the CO stretch mode was obtained from the parameters derived from FTIR data. Our best estimates for the low-frequency reservoir coupling rates, yc = 167 (24) GHz and yL= 145 ( 52) GHz, give the solid lines shown in fig. 3, and give the adsorbate temperature 436 variation shown in fig.…”

Section: Resultsmentioning

confidence: 99%

Vibrational response of surface adsorbates to femtosecond substrate heating

Culver

Jahn

et al. 1993

Chemical Physics Letters

View full text Add to dashboard Cite

Section: Resultsmentioning

confidence: 99%

Vibrational response of surface adsorbates to femtosecond substrate heating

Culver

Jahn

et al. 1993

Chemical Physics Letters

View full text Add to dashboard Cite

“…This more careful approach differs from the derivation above in three important respects: 1) The presence of more than one pair of exchanging modes can be readily represented. 2) Additional dephasing mechanisms are included by adding more terms to the force autocorrelation functions (A.2).…”

mentioning

confidence: 99%

“…The important points to note are: 1) Both the width and shift (3) display the same apparent ''activation energy", E., which is equal to the…”

mentioning

confidence: 99%

See 1 more Smart Citation

A critical test of vibrational dephasing theories in solids using spontaneous Raman scattering in isotopically mixed crystals

Marks

Cornelius

Harris

1980

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

A series of experiments have been conducted in order to evaluate the relative importance of several recent theories of vibrational dephasing in solids. The theories are discussed briefly, and are used to interpret the temperature dependence of the C–H and C–D stretch bands in the spontaneous Raman spectra of h14- and d14-1,2,4,5-tetramethyl benzene (durene). The infrared spectra of these same molecules are also reported in the region of the combination bands involving C–H (or C–D) stretches and low-frequency modes. The results support the applicability of the model of Harris et al., [C. B. Harris, R. M. Shelby and P. A. Cornelius, Phys. Rev. Lett. 38, 1415 (1977); Chem Phys. Lett. 57, 8 (1978); R. M. Shelby, C. B. Harris, and P. A. Cornelius, J. Chem. Phys. 70, 34 (1979)], based on energy exchange in anharmonically coupled low-frequency modes. This theory is then used, in connection with Raman spectra obtained in isotopically mixed samples of durene, to elucidate the vibrational dynamics underlying the dephasing. It is found that the results are consistent with the hypothesis that some low-frequency modes in this molecule are significantly delocalized or ’’excitonic’’ in character, and that this delocalization may be studied by means of Raman spectroscopy on the low-frequency modes themselves, as well as by exchange analysis of the coupled high-frequency modes. These conclusions represent a generalization and extension of the previously published exchange model [R. M. Shelby, C. B. Harris, and P. A. Cornelius, J. Chem Phys. 70, 34 (1979)].

show abstract

“…16 The temperature dependence of the observed dephasing rate clearly exhibits a thermally activated component, indicating the presence of the "exchange-modulation" mechanism. 17 Namely, the G-band phonon mode dephases via anharmonicity-induced coupling with a lower frequency mode. Our quantitative analysis provides evidence that the lower frequency mode responsible for the decay of G-band phonons is the RBM.…”

mentioning

confidence: 99%

Dephasing ofG-band phonons in single-wall carbon nanotubes probed via impulsive stimulated Raman scattering

et al. 2012

View full text Add to dashboard Cite

We study the coherent dynamics of G-band phonons in single-wall carbon nanotubes through impulsive stimulated Stokes and anti-Stokes Raman scattering. The probe energy dependence of the phonon amplitude as well as the preferential occurrence between Stokes and anti-Stokes components in response to chirpedpulse excitation are well explained within our model. The temperature dependence of the observed dephasing rate clearly exhibits a thermally activated component, with an activation energy that coincides with the frequency of the radial breathing mode (RBM). This fact provides a clear picture for the dephasing of G-band phonons by random frequency modulation via interaction with the RBM through anharmonicity. Optical phonons often play major roles in dynamical phenomena in solids. Due to their strong coupling with electrons, they are behind virtually all energy and phase relaxation processes that occur in the presence of high electric fields and/or nonequilibrium carrier distributions. Recently, much attention has been paid to nonperturbative electronoptical-phonon coupling in single-wall carbon nanotubes (SWCNTs).1-3 Such strong coupling is believed to be responsible for the current saturation behaviors observed in high-field electronic transport 4,5 as well as for the appearance of a broad and red-shifted Raman feature due to Kohn anomalies. 6 In both cases, dynamical quantities of optical phonons such as lifetimes and dephasing times are the key parameters that characterize the processes.Raman scattering spectroscopy has been an indispensable tool for characterizing the electronic structure of carbonbased nanomaterials such as SWCNTs.7 While an extensive literature exists on CW Raman studies, time-domain vibrational measurements directly probing lattice dynamics in SWCNTs have only recently begun. [8][9][10][11][12][13][14] Real-time observations of coherent oscillations have been made of both the low-frequency (100-300 cm −1 ) radial-breathing mode (RBM) and the high-frequency (1550-1600 cm −1 ) phonon mode, the so-called G band, providing important insight into chirality dependence, 8 generation mechanisms, 12,15 and electron-phonon coupling strength.13 A population lifetime of 1.1 ± 0.2 ps was also measured for optical phonons in SWCNTs at room temperature using time-resolved anti-Stokes Raman spectroscopy.11 However, exactly how optical phonons decay in energy and phase in SWCNTs is still an open question.Here, we report results of coherent phonon spectroscopy of SWCNTs using spectrally resolved and temperaturedependent ultrafast pump-probe spectroscopy. A pump pulse initiates coherent lattice vibrations, and then a delayed, spectrally broad probe pulse is incident on the sample, where it induces additional lattice vibrations through impulsive stimulated Raman scattering. The probe photon-energy dependence of phonon amplitude for both transformed-limited and chirped pulses can be well explained within our model based on impulsive stimulated Stokes Raman scattering (SSRS) and anti-Stokes Raman scattering (S...

show abstract

Effects of Energy Exchange on Vibrational Dephasing Times in Raman Scattering

Cited by 193 publications

References 8 publications

Vibrational response of surface adsorbates to femtosecond substrate heating

Vibrational response of surface adsorbates to femtosecond substrate heating

A critical test of vibrational dephasing theories in solids using spontaneous Raman scattering in isotopically mixed crystals

Dephasing ofG-band phonons in single-wall carbon nanotubes probed via impulsive stimulated Raman scattering

Contact Info

Product

Resources

About