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The Journal of Chemical Physics

Color effects in pressure-tuned hole-burned spectra

Gerhard Gradl, J. Zollfrank, W. Breinl, J. Friedrich

Published Jun 15, 1991• 43 citations
Publisher

Abstract

We applied hydrostatic pressure to spectral holes burned into a resorufin doped ethanol/methanol glass. We found that the line shift is perfectly linear with pressure and showed a pronounced dependence on the burn frequency as predicted by theory [J. Chem. Phys. 90, 3274 (1989)]. We exploited the burn frequency dependence to determine the solvent shift of the dye probe and the compressibility of the alcohol glass used. On the other hand, the behavior of the hole width under pressure shows features not predicted by theory: The broadening is, like the line shift, dependent on the burn frequency within the inhomogeneous band, yet in a nonlinear fashion. We attribute the color effect in the pressure induced broadening of the hole to a breakdown of the Gaussian approximation.

DOI
10.1063/1.460148

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We applied hydrostatic pressure to spectral holes burned into a resorufin doped ethanol/methanol glass. We found that the line shift is perfectly linear with pressure and showed a pronounced dependence on the burn frequency as predicted by theory [J. Chem. Phys. 90, 3274 (1989)]. We exploited the burn frequency dependence to determine the solvent shift of the dye probe and the compressibility of the alcohol glass used. On the other hand, the behavior of the hole width under pressure shows features not predicted by theory: The broadening is, like the line shift, dependent on the burn frequency within the inhomogeneous band, yet in a nonlinear fashion. We attribute the color effect in the pressure induced broadening of the hole to a breakdown of the Gaussian approximation.
External perturbations such as, for instance, hydrostatic pressure in general give rise to a shift and a concomitant broadening of persistent hole-burning spectra. The magnitude of both effects usually varies with the optical frequency in the inhomogeneous absorption band. Within the framework of a stochastic theory of dye-matrix interaction, an extended Gaussian approximation is used to derive general analytical expressions for the variation of both the shift and the broadening parameter. The results are compared with numerical calculations. Furthermore, the obtained expressions are generalized to take correlations between the matrix molecules into account.
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.
First preliminary persistent spectral hole-burning (PSHB) investigations of dye-molecules adsorbed onto the disordered surfaces of metal oxide powders or porous glasses1,2,3 indicated that these systems seem to behave quite similar to doped glasses. The optical absorption is strongly inhomogeneously broadened due to the disorder of the surface and at 1.5 K holewidths in the 1 cm1 range - even an order of magnitude broader than in glasses - have been reported. In the following we will give a short summary of our latest more detailed investigations of surface adsorbed dye-molecules which on the one hand reaffirm that these systems indeed behave in many respects as 3-D disordered systems but on the other hand point to some remarkable specific features of adsorbed dye-molecules.
Fluorescence excitation spectra of single terrylene molecules in p-terphenyl crystals were investigated at low temperatures. The line shifts due to hydrostatic pressure and external electric fields were measured, with the electric field strength oriented either parallel or perpendicular to the k vector of the laser light. A linear Stark effect was found for most molecules, indicating local environments of low symmetry. In sites X1 and X3 (and XY, a photoproduct state), spectral hole burning was observed. Whereas the holes are stable in sites X1 and XY, they decay with a time constant of some minutes in X3. Pressure experiments were performed on the stable hole spectra in sites X1 and XY. In weakly doped samples, holes composed of very few molecular lines were generated with halfwidths distinctly narrower than twice the homogeneous linewidth.
For next generation high density optical storage, extensive studies on persistent spectral hole burning (PSHB) have been performed, because they have a large potential for a high density frequency-domain optical data storage. PSHB has been observed at room temperature in Sm-doped crystals and glasses. Among them, glasses are considered to be more favorable than single crystals, due to their wide inhomogeneous line width and easy process for mass production. In the study, we developed a new glass mixture which shows room temperature PSHB with a inhomogeneous line width broadened up to 70 cm/sup -1/. The PSHB was characterized by investigating the time decay pattern of fluorescence and the excitation spectra.