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Chemical Physics Letters

The effect of fluctuations on emission spectra: practical distinctions between raman and fluorescence spectra

Robin M. Hochstrasser, Frank A. Novak

Published May 1, 1977• 30 citations
Publisher
DOI
10.1016/0009-2614(77)80200-5

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Absorption and emission spectroscopies of homogeneous and inhomogeneously broadened multilevel systems in strong light fields

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A method is introduced to calculate for a model set of molecular levels the spectral line shapes expected for a variety of conventional laser experiments including absorption, hole burning, fluorescence line narrowing, and Raman scattering. The method allows the incident laser field to have arbitrary intensity. Furthermore, the effects of model Gaussian or Lorenzian inhomogeneous distributions are readily incorporated. Earlier results for a two-level system are easily obtained and new results are presented for inhomogeneously broadened two and three level systems, and for the effects of pure dephasing on the strong field spectra. In particular we have described the differences between fluorescence and Raman in strong fields, and the effect of strong fields on the spontaneous emission of inhomogeneously broadened transitions. Some predictions are made regarding line narrowing experiments in the strong-field limit.

The Journal of Chemical Physics•Oct 1, 1984•32 citations
Abstract A practical approach to understanding light scattering processes in the condensed phase is presented. First a theoretical discussion of the various parameters in resonance light scattering is given and there is a special emphasis on our simplified approach to this question. As with other approaches the two level density matrix in association with a quantum regression theorem leads to two types of emission from an ensemble of molecules at finite temperature (T2 ≠ 2T1). We have called one of these fluorescence and the other sharper emission Raman scattering because it results directly from the presence of a coherent polarization in the medium. A brief discussion of time dependent scattering is also given. An experiment that reproduces the main features of the theory is described for resonance scattering from azulene in naphthalene at 30 K. For all values of the laser frequency (near resonance) both a sharp (Raman) and diffuse (fluorescent) component occurs in the emission spectrum. These spectra when interpreted by the simplified theory yield a value of T2 = 0.7 ps from fluorescence linewidth, and T2 = 0.8 ps from the incoherent to coherent scattering ratio, for the 0–0 two level system of azulene in naphthalene. A discussion of practical aspects of the influence of inhomogeneous line broadening is also presented.
A method is introduced to calculate for a model set of molecular levels the spectral line shapes expected for a variety of conventional laser experiments including absorption, hole burning, fluorescence line narrowing, and Raman scattering. The method allows the incident laser field to have arbitrary intensity. Furthermore, the effects of model Gaussian or Lorenzian inhomogeneous distributions are readily incorporated. Earlier results for a two-level system are easily obtained and new results are presented for inhomogeneously broadened two and three level systems, and for the effects of pure dephasing on the strong field spectra. In particular we have described the differences between fluorescence and Raman in strong fields, and the effect of strong fields on the spontaneous emission of inhomogeneously broadened transitions. Some predictions are made regarding line narrowing experiments in the strong-field limit.