Transform method in resonance Raman scattering: effect of mode mixing

Tehver, I.; Kaasik, Helle; Hizhnyakov, V.

doi:10.1002/jrs.894

Cited by 12 publications

(7 citation statements)

References 23 publications

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“…As an alternative explanation, we attribute the peculiar excitation profiles of the two modes to Duschinsky‐rotation 19, 20, which was not considered in our calculations. The Duschinsky‐rotation implies mode mixing that arises from the off‐diagonal elements of the quadratic vibronic coupling.…”

Section: Resultsmentioning

confidence: 97%

The anomaly of the $\nu$₁‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II

Tschirner

Brose

Schenderlein

et al. 2009

Physica Status Solidi (b)

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We have studied the resonance Raman spectra of b-carotene in solution and in protein-complexes using laser excitation at various wavelengths in the visible region. Main focus was laid on the n 1 -band, which shows an anomalous behaviour upon variation of the excitation wavelength resulting in a frequency shift of the peak maximum. This shift is due to different excitation profiles of two closely spaced modes as shown previously for b-carotene in solution. In this work, we have extended the studies to the antenna pigment in photosystems I and II (PS I and PS II).

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Section: Resultsmentioning

confidence: 97%

The anomaly of the $\nu$₁‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II

Tschirner

Brose

Schenderlein

et al. 2009

Physica Status Solidi (b)

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“…Here y 1 and y 2 are the normal coordinates in the final state, and j is the angle of the Duschinsky rotation. In this model the Fourier transform at T ¼ 0 equals [18,23] …”

Section: Two Mixed Modes: Test Of the Proposed Methodsmentioning

confidence: 99%

“…Refs. [18,19]); this, however, is not sufficient for the application to crystals. In this communication, we propose another approach, which is based on the path-integral-type consideration of the time evolution of the optical centre in the final state.…”

Section: Introductionmentioning

confidence: 94%

Theory of optical spectra of impurity centres in crystals: general consideration of quadratic vibronic coupling

Hizhnyakov

Holmar

Tehver

2007

Journal of Luminescence

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“…This method allows one to calculate the Fourier-transform of the optical spectrum via the Fourier-transforms of the one-and twophonon amplitudes of the resonance Raman scattering. Previously this method was used for investigation of the effect of mode mixing in the resonant Raman scattering [11][12].…”

Section: Optical Transition To a State With Soft Phonon Dynamicsmentioning

confidence: 99%

Multiphonon processes in impurity centres: nonperturbative theory

Hizhnyakov

Boltrushko

Kaasik

et al. 2005

Physica Status Solidi (a)

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A nonperturbative theory of the multiphonon relaxation of a strongly excited local vibration is developed. It is found that for a high initial level, the relaxation first accelerates in time, and later starts to slow down. The experimental evidence of such a non-monotonous relaxation is given by the hot luminescence in solid Xe. A theory of optical transitions in a center with strongly reduced local springs in the final electronic state is also developed. In this case a resonant increase of the local density of states of low-frequency phonons takes place, and a low frequency pseudo-local mode emerges. Appearance of such a mode in the final state means that a strong mode mixing takes place at the transition. This results in strong increase of the mean number of created low-frequency phonons. As a consequence, the zero-phonon transition practically disappears and the long-wave part of the phonon sideband is strongly enhanced, resulting in formation of so-called lambda-shaped spectrum. Multiphonon relaxation of local modePhysical processes in solids usually involve the relaxation of the vibrational energy. For example, optical excitation of F-centers or other centers in ionic crystals and self-trapped excitons usually leads to excitation of strong vibrations. In CARS experiments one usually excites strong long-wave coherent vibration, which decays via multiphonon anharmonic interaction into other phonons. Laser methods allow one to achieve also direct excitation of non-coherent vibrations of impurity molecules in crystals. The subsequent processes are essentially determined by the relaxation of these vibrations. The vibrational quanta of light molecules may exceed many times the maximal energy of phonons. In such a case the vibrational relaxation takes place as a multiphonon emission. Usually this process is considered in the frames of the perturbation theory, by applying the Fermi Golden Rule [1 -5]. However, this theory works only if the energy of the mode is small. Here we apply another method [6 -7], which works for the large energy of the mode, supposing that the relaxation rate remains less than the frequency ω l of the mode.In [6][7] it is taken into account that a strongly excited mode can be considered classically. Then the mode causes a perturbation of phonons which is quasi-periodical in time. The Coleman theorem [8] reads that the zero-point state and the operators of bosons interacting with a classical field are not invariant with respect to the transformation which changes the classical field. It means that the transformed destruction operators are not the zero operators for the initial zero-point state. This corresponds to the fact that classical field which changes in time leads to emission of phonons.

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Transform method in resonance Raman scattering: effect of mode mixing

Cited by 12 publications

References 23 publications

The anomaly of the $\nu$₁‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II

The anomaly of the $\nu$₁‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II

Theory of optical spectra of impurity centres in crystals: general consideration of quadratic vibronic coupling

Multiphonon processes in impurity centres: nonperturbative theory

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Transform method in resonance Raman scattering: effect of mode mixing

Cited by 12 publications

References 23 publications

The anomaly of the $\nu$1‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II

The anomaly of the $\nu$1‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II

Theory of optical spectra of impurity centres in crystals: general consideration of quadratic vibronic coupling

Multiphonon processes in impurity centres: nonperturbative theory

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The anomaly of the $\nu$₁‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II

The anomaly of the $\nu$₁‐resonance Raman band of bβ‐carotene in solution and in photosystem I and II