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Optics and Spectroscopy

Modeling of the Evans holes in inhomogeneously broadened absorption and Raman scattering bands

V. P. Bulychev, Tatjana D. Kolomiitsova, D. N. Shchepkin

Published May 1, 1994• 5 citations
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A molecular dynamics analysis of resonance emission: Optical dephasing and inhomogeneous broadening of CH3I in CH4 and Ar

R. Fan, Ted Kalbfleisch, L. D. Ziegler

The spontaneous resonance emission of CH3I in high pressures (800–1600 psi) of CH4 and Ar excited in the region of the Rydberg B-state origin (∼201 nm) are reported. These emission spectra consist of narrow Raman-like (RL) and broad fluorescence-like (FL) spectral features. The observed ratio of the Raman/fluorescence intensity in these high pressure solutions is a function of the excitation wavelength as the incident radiation is tuned through the pressure broadened electronic origin band. Molecular dynamics simulations are implemented for the analysis of the observed emission spectral shapes and their excitation frequency dependence. The four-time dipole correlation functions required for the calculation of this nonlinear polarization derived signal are successfully approximated by a product of two two-time dipole correlation functions for these chromophore-bath systems (factorization approximation). The complex emission band shapes and their excitation frequency dependence are captured by this approach. The dispersion in the RL/FL emission redistribution is due to the multiple time scales inherent to the decay of the resonant optical coherence of these pressure-broadened absorptions. The wavelength dependent pure-dephasing rate is determined by the nonlinear shape of the solute–solvent difference potential. The observational time scale dependence of the spectroscopic homogeneous and inhomogeneous line broadening labels is clearly demonstrated and contrasted here for absorption and Raman scattering.

The Journal of Chemical Physics•Mar 15, 1996•20 citations
Abstract This chapter focuses on spectroscopic applications of time dependent quantum mechanics focusing on molecular spectroscopy in condensed phases. (1) Molecular spectroscopy in the dressed state picture. (2) Resonance Raman scattering. (3) Resonance energy transfer. (4) Collective excitation and emission. (5) Thermal relaxation and dephasing (the Bloch equations, relaxation of a prepared state, dephasing (decoherence), the absorption lineshape, homogeneous and inhomogeneous broadening, motional narrowing, thermal effects in resonance Raman scattering). (6) A case study: Resonance Raman scattering and fluorescence from Azulene in a Naphthalene matrix. (7) Probing inhomogeneous bands (hole-burning spectroscopy, photon echoes, single-molecule spectroscopy. (8) Optical response functions.
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 spontaneous resonance emission of CH3I in high pressures (800–1600 psi) of CH4 and Ar excited in the region of the Rydberg B-state origin (∼201 nm) are reported. These emission spectra consist of narrow Raman-like (RL) and broad fluorescence-like (FL) spectral features. The observed ratio of the Raman/fluorescence intensity in these high pressure solutions is a function of the excitation wavelength as the incident radiation is tuned through the pressure broadened electronic origin band. Molecular dynamics simulations are implemented for the analysis of the observed emission spectral shapes and their excitation frequency dependence. The four-time dipole correlation functions required for the calculation of this nonlinear polarization derived signal are successfully approximated by a product of two two-time dipole correlation functions for these chromophore-bath systems (factorization approximation). The complex emission band shapes and their excitation frequency dependence are captured by this approach. The dispersion in the RL/FL emission redistribution is due to the multiple time scales inherent to the decay of the resonant optical coherence of these pressure-broadened absorptions. The wavelength dependent pure-dephasing rate is determined by the nonlinear shape of the solute–solvent difference potential. The observational time scale dependence of the spectroscopic homogeneous and inhomogeneous line broadening labels is clearly demonstrated and contrasted here for absorption and Raman scattering.