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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Persistent Spectral Hole-Burning of Dye Molecules Adsorbed on Heterogeneous Surfaces

Christoph Bräuchle, Bernd Sauter, R. Kettner

Published Jan 1, 1992• 0 citations
Publisher

Abstract

In this talk we review our recent results on dye-surface systems investigated by persistent spectral hole-burning. Dye-surface systems are an interesting class of hole-burning materials. In most dye-surface systems investigated by us stable holes can be burnt and detected at unusual high temperatures [1,2,3]. In addition, the understanding of the interaction between adsorbed molecules and the heterogeneous surface may provide new insights in processes important in catalysis.

DOI
10.1364/shbl.1992.tuc3

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In this talk we review our recent results on dye-surface systems investigated by persistent spectral hole-burning. Dye-surface systems are an interesting class of hole-burning materials. In most dye-surface systems investigated by us stable holes can be burnt and detected at unusual high temperatures [1,2,3]. In addition, the understanding of the interaction between adsorbed molecules and the heterogeneous surface may provide new insights in processes important in catalysis.
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.
An overview of recent results concerning molecular doped solids is presented. The hole burning performances and the photophysics of polymer and xerogel-based systems are compared. Three areas are considered in more detail: the problem of electron-phonon coupling, the one of high-temperature persistent spectral hole burning materials, and the search for new frequency-selective photosensitive systems for fast optical pulse processing at 800 nm. This comparison demonstrates that molecular doped polymers and molecular doped xerogels have similar hole burning behavior but mechanisms in these systems can be different. However, in respect of the areas considered, inorganic hosts based on silicate xerogels or porous glasses have shown the best results. Moreover, all the possibilities of hybrid xerogels created by combining inorganic and organic capabilities or by grafting organic species to the host have not yet been revealed.
The persistent spectral hole-burning (PSHB) phenomenon has been known since 1974. It is still an important research area for the study of the intimacy of complex molecular systems in the solid state, revealing high-resolution spectra, photophysics, photochemistry, and dynamics of molecular doped amorphous media, organic as well as inorganic. From another point of view, PSHB allows the engraving of any spectral structures in the inhomogeneous absorption band profile of molecular doped amorphous hosts or ion doped crystals cooled down to liquid helium temperatures. Therefore, a PSHB material is programmable in the spectral domain and consequently it can be transformed in an optical processor capable of achieving user-defined optical functions. Some aspects of both fields are illustrated in the present paper. Concerning the search for efficient PSHB materials, the hole-burning performances and the photophysics of polymer and xerogel based systems are compared. The problem of high-temperature persistent spectral hole-burning materials and the search for new frequency selective photosensitive systems for fast optical pulse processing at 800nm are considered. Regarding the points treated, inorganic hosts based on silicate xerogels or porous glasses have shown the best results. Moreover, by combining inorganic and organic capabilities or by grafting organic species to the host, hybrid xerogels have not yet revealed all possibilities. Also, the interest of two-photon materials for engraving spectral features with near-infrared or infrared light is developed. As an introduction to possible applications of PSHB material, the basics of spectro-temporal holography are remembered and a demonstrative experiment using a naphthalocyanine-doped polymer film is described, proving that the temporal aberration free recompression of ultrashort light pulses is feasible, therefore opening a way for applications in ultrashort light pulse shaping. Aspects for a comparison between cw hole-burning and femtosecond spectro-temporal experiments are considered, and prospects for coherent control of light fields or photochemical processes are also evoked.
Abstract : Fundamental limits on frequency-domain optical storage using persistent spectral hole-burning follow from both the expected configuration of the storage system and from physical effects such as the photophysics of the light-induced reaction in the material, photon quantum (shot) noise, and statistical fluctuations in additive random quantities. When frequency-domain reading and writing in focused spots is considered, the large class of single-photon materials can be shown to have serious limitations from a single-to-noise point of view. This has stimulated interest in photon-grated material which effectively have a threshold in the writing process, controlled by a second light beam of a different color. Fundamental statistical limits on persistent spectral hole-burning can also be illustrated using recent measurements of statistical fine structure in solids. Other recent experiments in which the absorption spectrum of a single absorbing molecule in a solid was measured represent an extreme limit on persistent spectral hole-burning effects.
Persistent spectral hole burning is a useful tool to detect zero-phonon line and phonon sideband of organic dye molecules doped in glasses and polymers, which are usually covered under inhomogeneous broadening. These observation bring us information on the electron-phonon interaction such as Debye-Waller factor a in these molecular systems. From the viewpoint of the issue of materials designing for wavelength-multiplexed optical memory and also with naive interest to obtain efficient sharp holes, we have paid much attention to the molecular systems in the category of rather weaker inter/intra-molecular coupling.