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Proceedings of the Estonian Academy of Sciences Physics Mathematics

TRANSFORM RELATIONSHIP BETWEEN ABSORPTION AND RESONANCE RAMAN SCATTERING IN INHOMOGENEOUS MEDIA

Imbi Tehver

Published Feb 16, 1993• 1 citation
Publisher

Abstract

A relationship between the absorption spectrum and the corresponding Raman excitation spectrum of molecules/impurity centers in inhomogeneous media has been derived for the case when the inhomogeneous broadening is smaller than the homogeneous one.This is a generalization of the basic transform relationship found earlier for an ensemble of identical molecules.1.

DOI
10.3176/phys.math.1993.2.04

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A relationship between the absorption spectrum and the corresponding Raman excitation spectrum of molecules/impurity centers in inhomogeneous media has been derived for the case when the inhomogeneous broadening is smaller than the homogeneous one.This is a generalization of the basic transform relationship found earlier for an ensemble of identical molecules.1.
Abstract The amplitudes and the excitation profiles of coherent resonant Raman scattering (coherent anti‐Stokes and Stokes Raman scattering (CARS and CSRS)) by impurity centers in crystals and/or molecules in solutions are studied, taking into account the coherence of the excited mode and the inhomogeneity of the environment. The CARS and CSRS excitation profiles can directly be related to one‐photon absorption when using the transform theory known from spontaneous resonant Raman scattering. The enlargement of the amplitude of the active mode reveals itself in an enhancement of the vibrational overtones. At large amplitudes, a splitting in the profiles caused by the contribution of two turning points of a strong coherent vibration is observed. The inhomogeneous broadening is different in the excitation profiles of CARS and CSRS. The overlapping contributions to spectrally narrow and broad transitions lead to Fano peculiarities. The effects are illustrated by model calculations. Copyright © 2011 John Wiley & Sons, Ltd.
The resonant absorption of light by an ensemble of absorbers decreases when the resonance is inhomogeneously broadened. Recovering the lost absorption cross section is of great importance for various applications of light-matter interactions, particularly in quantum optics, but no recovery mechanism has yet been identified and successfully demonstrated. Here, we formulate the limit set by the inhomogeneity on the absorption, and present a mechanism able to circumvent this limit and fully recover the homogeneous absorption of the ensemble. We experimentally study this mechanism using two different level schemes in atomic vapors and demonstrate up to fivefold enhancement of the absorption above the inhomogeneous limit. Our scheme relies on light shifts induced by auxiliary fields and is thus applicable to various physical systems and inhomogeneity mechanisms.
Because of inevitable size distribution, shape variations, different concentration of impurities and defects, and fluctuations of local environment and charge distribution, every ensemble of nanocrystals dispersed in some solid or liquid medium possesses inhomogeneously broadened absorption and emission spectra. Therefore, a number of properties inherent in molecular and atomic inhomogeneously broadened spectra can be a priori foreseen for nanocrystals. These include spectral hole-burning, fluorescence line narrowing under selective excitation, and decay time distribution. At the same time, spectrally selective techniques developed for inhomogeneously broadened molecular and atomic structures have been successfully applied to nanocrystals providing evaluation of individual parameters smeared as a result of inhomogeneous broadening. This chapter gives a brief overview of specific phenomena inherent in all spectrally inhomogeneous media and a survey of the relevant experimental techniques including nonlinear pump-and-probe spectroscopy, fluorescence excitation spectroscopy, and single molecule spectroscopy. Population-induced optical nonlinearity and spectral hole-burning Every real system consisting of particles with discrete energy levels exhibits absorption saturation under intense optical excitation. The only example of a nonsaturable system is an ensemble of ideal harmonic oscillators that possess an infinite number of equally spaced energy levels, optical transitions allowed only for a couple of neighboring levels, and the probability of optical transitions being proportional to the level number (Stepanov and Gribkovskii 1963).
An analysis and model calculations are presented to clarity how both the electronic and vibrational inhomogeneities with no correlation between them influence the most relevant resonant steady-state third-order nonlinear optical mixing processes (CARS, CSRS, polarization spectroscopy and Raman gain (loss)).It is shown that all these processes may be divided into three groups: 1) processes yielding almost homogeneous spectra: both inhomogeneities are greatly reduced; 2) processes yielding quasihomo- geneous spectra: inhomogeneities are present, but the electronic one is not manifest in the spectrum; 3) processes yielding completely inhomogeneous spectra.The suppression of inhomogeneous broadening allows to study the excited electronic states and the ultrafast relaxation processes in inhomogeneous media more effectively than in linear spectroscopy. * About another steady-state frequency domain technique byhot luminescence measurements for the study of ultrafast energy relaxation see.e. g. f l4 ].ЁЁЗТТ NSV TEADUSTE AKADEEMIA TOIMETISED.30.
Optical spectroscopy provides a useful tool for probing the structure and dynamics of solids. Over the years, optical methods have evolved from absorption spectroscopy to more complex methods such as spectral hole burning, photon echoes, and luminescence line narrowing. The absorption spectrum provides information about inhomogeneous broadening, while the latter approaches provide information about the systematics of the homogeneous line shape information that is often obscured by inhomogeneous broadening. When external perturbations such as strain or electric fields are applied, details of the local site can be obtained. Recently, the ultimate limit of optical spectroscopy has been attained, in which the spectral properties of individual single impurity molecules in a solid can be measured, with all ensemble averaging removed. This novel regime has provided additional, previously unobtainable, information on a highly local scale, such as the direct observation of the spectral shifting of a single molecule produced by configurational transitions of the host. It is to be expected that further surprises await us in this new frontier of single-molecule spectroscopy in solids.