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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Effects of Matrix Correlations on Inhomogeneous Spectral Distributions: Rare Gas and Polymeric Systems

L. Kador, Peter Geissinger, D. Haarer

Published Jan 1, 1994• 0 citations
Publisher

Abstract

Inhomogeneous distributions of spectral lines are a ubiquitous phenomenon in nature. In the optical spectroscopy of dye molecules embedded in transparent solids, the inhomogeneous widths are usually much larger than the corresponding homogeneous linewidths of single molecules.
DOI
10.1364/shbs.1994.the2

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Abstract In recent years different microscopic and spectroscopic techniques were successfully employed to detect the fluorescence signals of single dye molecules in the condensed phase. In low temperature solids the fluorescence excitation line of a single dopant molecule is a high resolution optical probe of its local nanoenvironment. As inhomogeneous contributions and ensemble averaging are absent, many effects hidden when looking at large populations of molecules become observable. Two important research areas in single molecule spectroscopy deal with the investigation of quantum optical effects and the spectral jumping behaviour of single molecule excitation lines caused by fluctuations of two‐level systems inherent to disordered solids. Rather than delivering a complete presentation, we will focus on some selected examples which emphasize the unique features of spectroscopy with a single absorber.
At very low temperatures, the spread in the different environments of matrix embedded dye molecules results in an inhomogeneously broadened S1 ← S0 band. Spectroscopic techniques based on the appearence of optical zero phonon lines, such as fluorescence line narrowing, spectral hole-burning, and single molecule spectroscopy provide an experimental resolution limited by the homogeneous linewidth. From the investigation of the homogeneous line width as a function of different parameters (time, temperature) information on the guest host interactions responsible for the observed linewidth is obtained. Spectrally narrow features are extremely sensitive probes for external perturbations, such as electric fields, magnetic fields, or hydrostatic pressure.
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.
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).
The concept of the homogeneous spectral linewidth of an impurity center is more complicated in disordered media such as organic glasses and polymers than it is in crystals. In amorphous media the local environments for impurity centers are continuously changing with time. As a result transition frequencies of individual centers diffuse within the inhomogeneous broadened spectral contour, which is called spectral diffusion. When the timescale for spectral diffusion processes is much longer than the dephasing time, it is possible to distinguish homogeneous dephasing from spectral diffusion. On the other hand, when the timescales of spectral diffusion and dephasing processes are comparable these phenomena become indistinguishable.
The inhomogeneous broadening caused by dipole–dipole interactions between molecules having strongly allowed optical transitions is considered for the case in which the chromophores are randomly distributed at low concentration in a transparent matrix. Model calculations show that absorption in the wings of the spectrum is caused almost exclusively by strongly interacting pairs of chromophores. This result has important implications for the interpretation of recent experiments in which the spectra of single dye molecules have been observed in organic matrices. The generalized lineshape in these wings is shown to be proportional to the inverse square of the detuning from line center. The line shape is also somewhat asymmetric, with the red wing being more intense than the blue.