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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Hole-Burning of Dye-Molecules Adsorbed on Metal Oxide Powders

Th. Basché, Christoph Bräuchle

Published Jan 1, 1991• 0 citations
Publisher

Abstract

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.

DOI
10.1364/pshb.1991.sb3

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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.
Permanent and transient hole-burning experiments carried out on various types of amorphous systems at temperatures between 0.3 and 20 K are presented. Optical dephasing on organic molecules in glasses and polymers measured on different time scales are discussed in relation to spectral diffusion processes and compared to the literature. The pure dephasing time appears to be proportional to the excited state lifetime of the guest. Organic molecules adsorbed on the surface of porous silica glass show that their homogeneous linewidth is an order of magnitude larger than in polymers and glasses in the bulk, but follows the same temperature dependence. Hole-burning results on bacteriochlorophyll in various disordered hosts are compared to those on a isolated light-harvesting photosynthetic pigment-protein complex (B800–850). From the holewidth in the latter the energy transfer rate between aggregated bacteriochlorophyll pigments is determined and compared to time-resolved spectroscopy results in the literature.
So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.
Recently, the interests in optical memory based on persistent spectral hole burning (PSHB) are increased because of its possibility of the application to high density optical memory. PSHB was observed for an organic dye doped in polymer and rear earth or transition metal doped in inorganic crystal or glasses up to now. Since PSHB was observed by two Russian groups (Gorokhovskii et al. and Kharlamov et al.) for free base phthalocyanine in a n-octane Shpol'skii matrix1 and for perylene and 9-aminoacridine molecules in glassy ethanol matrix2, PSHB materials are studied primarily for the polymer doped with an organic dye. But such materials can make hole only at very low temperature. Room temperature PSHB phenomena were observed on Sm2+ doped fluoride crystals3-5 and glasses6 recently, however these materials' Гih(inhomogeneous line width)/Гh(homogeneous line width)'s which are the parameters of data multiplicity in PSHB optical memory are an order of unity. For the application of PSHB materials to optical memory, high operating temperature, high Гih/Гh, and rapid reaction rate are wanted. Glass has a superiority on the view point of optical memory application because of its broad inhomogeneous line width and productivity. Our group has discovered room temperature PSHB for Sm2+ in borate glass systems whose Гih/Гh is 24.7 PSHB for rear earth metal in glass matrix has not been studied seriously, yet. It is thought that the study of the relationship between the optical hole and glass structure is necessary.
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.