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IBM Journal of Research and Development

Photochemical Hole Burning in Free-Base Porphyrin and Chlorin in n-Alkane Matrices

Silvia Volker, R. M. Macfarlane

Published Sep 1, 1979• 74 citations
Publisher

Abstract

In inhomogeneously broadened lines, selective photochemistry with narrow band lasers leads to photochemical hole burning. We describe this phenomenon with particular reference to free-base porphyrin (H2P) and chlorin molecules in n-alkane matrices at low temperatures. It is shown that hole burning, which is permanent at low temperatures, can be used to study homogeneous optical dephasing processes as a function of temperature, to measure fast vibronic relaxation, and to assign complex vibronic spectra. Some of the parameters that are important to the potential use of photochemical hole burning for information storage in inhomogeneously broadened lines are measured and discussed.

DOI
10.1147/rd.235.0547

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Aug 13, 1993•0 citations
In inhomogeneously broadened lines, selective photochemistry with narrow band lasers leads to photochemical hole burning. We describe this phenomenon with particular reference to free-base porphyrin (H2P) and chlorin molecules in n-alkane matrices at low temperatures. It is shown that hole burning, which is permanent at low temperatures, can be used to study homogeneous optical dephasing processes as a function of temperature, to measure fast vibronic relaxation, and to assign complex vibronic spectra. Some of the parameters that are important to the potential use of photochemical hole burning for information storage in inhomogeneously broadened lines are measured and discussed.
Many investigations have been done on the field of frequency domain optical memories based on photochemical hole burning (PHB). This effect offers an extra dimension for the organization of an optical memory. At cryogenic temperatures several solid state materials such as aggregate color centers in alkali halide crystals exhibit inhomogeneously broadened absorption lines. In such an absorption line permanent narrow holes can be burnt by photochemical processes induced by exposure to intense laser radiation with a wavelength within the inhomogeneously broadened line.
The study of optical relaxation processes in solids at low temperature has progressed tremendously in the last 20 years due to the development of coherent optical techniques. The latter would not have been possible without the advent of narrow-band tunable lasers, on the one hand, and lasers with very short pulses (picoseconds, femtosecoods) on the other hand. Such coherent techniques are necessary because spectral line shapes of solids doped with guest molecules are seldom determined by dynamical interactions but principally by strain or structural disorder. This gives rise to inhomogeneous broadening, rlOh, which in crystalline hosts at low temperature varies between ' 0.1 and 10 cm -I, whereas in glasses it may amount to � 100-500 em-I. One of the techniques to achieve narrowing of spectral lines is site­ selection spectroscopy (1-3). A sub-ensemble of molecules within thc inhomogeneously broadened absorption band is selectively excited by mcans of a narrow-band laser, and the fluorescence or phosphoresccnce signal is detected with a high-resolution monochromator and/or a Fabry­ Perot interferometer. Fluorescence line-narrowing ( I) is a special case of this technique (for a review see 3). The intrinsic or homogeneous spectral linewidth, r hom, which yields information on the relaxation processes of the excited state, is given by the effective optical dephasing time, T2:
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.
Photochemical hole burning (PHB) is a topic of attracting increasing interest from spectroscopic viewpoints as well as from the practical prospects for ultra-high-density frequency-domain optical storage. Recent advances in PHB study are reviewed mainly focusing on the effects of chemical structure of guest ions and molecules as well as host matrices on the efficiency of hole formation and its temperature dependence, low energy excitation modes and Debye-Waller factors in amorphous matrices, and the mechanism of photon-gated PHB.
Persistent spectral hole burning (PSHB) was performed for several porphyrin molecules imbedded in polymer hosts and rare-earth ion Sm2+ doped in BaFCl0.5Br0.5 matrix. Power saturation and broadening effects for hole depth and width were observed. The dynamical process of hole formation was measured and explanation by population rate equations was given. Quantum efficiency of photochemical hole burning was investigated. For BaFCl0.5Br0.5:Sm2+ the capacity of data storage was estimated according to the result of multiple hole burning.