Dynamics of the time-resolved stimulated Raman scattering spectrum in presence of transient vibronic inversion of population on the example of optically excited trans-β-apo-8'-carotenal

We have studied the effect of transient vibrational inversion of population in trans-β-apo-8(')-carotenal on the time-resolved femtosecond stimulated Raman scattering (TR-FSRS) signal. The experimental data are interpreted by applying a quantum mechanical approach, using the formalism of projec...

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Bibliographic Details
Published in:The Journal of chemical physics 2014-05, Vol.140 (20), p.204312-204312
Main Authors: Kardaś, T M, Ratajska-Gadomska, B, Lapini, A, Ragnoni, E, Righini, R, Di Donato, M, Foggi, P, Gadomski, W
Format: Article
Language:English
Subjects:
ATOMIC AND MOLECULAR PHYSICS
ELECTRONIC STRUCTURE
GROUND STATES
INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
NANOSCIENCE AND NANOTECHNOLOGY
PROJECTION OPERATORS
Quantum mechanics
RAMAN EFFECT
Raman spectra
SPECTRA
TIME RESOLUTION
TRANSIENTS
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Summary:We have studied the effect of transient vibrational inversion of population in trans-β-apo-8(')-carotenal on the time-resolved femtosecond stimulated Raman scattering (TR-FSRS) signal. The experimental data are interpreted by applying a quantum mechanical approach, using the formalism of projection operators for constructing the theoretical model of TR-FSRS. Within this theoretical frame we explain the presence of transient Raman losses on the Stokes side of the TR-FSRS spectrum as the effect of vibrational inversion of population. In view of the obtained experimental and theoretical results, we conclude that the excited S2 electronic level of trans-β-apo-8(')-carotenal relaxes towards the S0 ground state through a set of four vibrational sublevels of S1 state.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.4879060