Raman profile with consideration for Condon and non-Condon terms

Tehver, I.

doi:10.1016/0030-4018(81)90399-0

Cited by 33 publications

(7 citation statements)

References 2 publications

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“…When moving off the resonance region, the Raman scattering arises just due to the violation of the Condon approximation: in other words, due to the dependence of the electronic transition matrix element on the vibrational coordinates. As has been shown [12], in the linear approximation (…”

Section: Basic Formulaementioning

confidence: 85%

Transform relations for CARS excitation profiles

Tehver

2005

phys. stat. sol. (c)

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PACS 33.20.Wr, 42.65.Dr The calculation of resonance CARS (coherent anti-Stokes Raman scattering) excitation spectra will be greatly simplified by applying the transform theory, which relates the scattering amplitudes to the recorded absorption spectrum. Based on transform relations, it is shown that the red shift of CEP arises due to the violation of the Condon approximation when the dependence of the electronic transition matrix element on the vibrational coordinates is taken into account. It leads to two competing mechanisms -a constructive interference (due to the non-Condon terms) in addition to the destructive interference (due to the Franck-Condon coupling) in the Raman amplitude. The interference of these two mechanisms can essentially affect the shape of the coherent Raman excitation profile. A simulation of the measured coherent excitation profile (CEP) of the resonance CARS of ZnPc in a polymer film is carried out.

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Section: Basic Formulaementioning

confidence: 85%

Transform relations for CARS excitation profiles

Tehver

2005

phys. stat. sol. (c)

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“…where κ ± j = 1 ± m j ξ j with the finite values of m j takes into account the first non-Condon effect [49] (due to Jahn-Teller interaction). (1) (ω)] 2 is obtained from the relationship between complex susceptibility and…”

Section: Cars Field For Mesoscopic Particlementioning

confidence: 99%

“…This formula is complex due to the homogeneous damping rates, γ of the excited state and of the vibrational states describing one-photon, two-photon and three-photon quasi-resonances. The main reason we use Eqn (2) is that we can apply the available transform theory results of Tehver [31,49] who has used this expression as the starting point to obtain the transform formula which relatesχ (3) pqrs and the absorption spectrum. The transform theory is convenient for studying the spectral properties of CARS in complex molecules and has proven record of good agreement with experiment.…”

Section: Cars Susceptibility and Polarization Via Transform Theorymentioning

confidence: 99%

Theory of coherent anti‐Stokes Raman scattering for mesoscopic particle with complex molecules: angular‐dependent spectrum

Ooi

2009

J Raman Spectroscopy

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We present a microscopic theory of nonlinear scattering of mesoscopic particle that may be composed of complex molecules. We predict that the spectrum of the scattered field depends on the angle of observation. Transform theory is used to compute the third-order susceptibility for coherent anti-Stokes Raman scattering (CARS) of molecules with known absorption spectrum and vibrational modes. By incorporating the theory into an integral scattering formula, we develop a rigorous theory which leads to powerful numerical experimentation of nonlinear optical process in mesoscopic systems composed of complex molecules and driven by laser pulses with arbitrary shape and spectral content. We obtain an expression for spectral dependent CARS field which includes multiple internal reflection and refraction of the incident fields via Mie theory. The theory is used to study the variations of the CARS spectra and intensity on laser parameters and direction of detection. High-resolution spectra computed for hybrid CARS scheme shows that the relative intensities of the characteristic peaks in the CARS spectrum depend on the direction of detection. This effect can be explained by the interference between the linear response (absorption and dispersion) and the four-wave mixing process in the mesoscopic medium. The theory is useful for nonlinear spectroscopy, microscopy and nanophotonics involving small particles.

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“…According to the above expressions, the excitation proÐles of Raman scattering (REPs) and also CARS and CSRS (CEPs) can be calculated via standard Fourier integrals for the Fourier amplitudes (4), (5) and (7). In many cases these amplitudes can easily be expressed via the Fourier integral of absorption, as will be shown below.…”

Section: Resonance Raman Amplitudes In the Time Representationmentioning

confidence: 99%

“…As already mentioned, the equations for A(t) can also be used in the calculation of CEPs (CARS/CSRS excitation proÐles) [Eqns (8) and (9)]. In the case of weak excitation, one can simply take the Fourier amplitude in A3 (t) Eqns (5) and (7) equal to A(t). Below we examine the e †ect of excitation intensity on taking into account A3 (t), the macroscopic energy of the vibrational mode excited in CARS and CSRS processes.…”

Section: Effect Of Excitation Intensity On the Transform Laws For Carmentioning

confidence: 99%

Spontaneous and Coherent Resonance Raman Scattering by Multimode Systems; Transform Laws for Excitation Profiles

Hizhnyakov

Tehver

1997

J. Raman Spectrosc.

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The time-domain theory of the excitation proÐles of resonance Raman scattering as well as CARS and CSRS of multimode systems is presented. In the time representation, the transform laws between absorption and scattering amplitudes are simpler than in the frequency representation. In particular, the advantage is manifest in the case of more complicated vibronic models, inhomogeneous media or when the e †ect of excitation intensity should be taken into account.

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Raman profile with consideration for Condon and non-Condon terms

Cited by 33 publications

References 2 publications

Transform relations for CARS excitation profiles

Transform relations for CARS excitation profiles

Theory of coherent anti‐Stokes Raman scattering for mesoscopic particle with complex molecules: angular‐dependent spectrum

Spontaneous and Coherent Resonance Raman Scattering by Multimode Systems; Transform Laws for Excitation Profiles

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