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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Molecular Computing

Urs P. Wild, Alois Renn

Published Jan 1, 1991• 0 citations
Publisher

Abstract

Each dye molecule embedded in an amorphous material such as a a polymer host experiences a specific molecular environment which strongly influences its electronic transition energies. At low temperatures the different microenvironments result in an inhomogeneously broadened absorption band. The invention of the laser brought new spectroscopic techniques based on energy selection, such as fluorescence line narrowing and spectral hole-burning [1]. These techniques enable convenient addressing of thousands of molecular subsets selected by their transition energy.

DOI
10.1364/pshb.1991.thc1

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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.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations
Each dye molecule embedded in an amorphous material such as a a polymer host experiences a specific molecular environment which strongly influences its electronic transition energies. At low temperatures the different microenvironments result in an inhomogeneously broadened absorption band. The invention of the laser brought new spectroscopic techniques based on energy selection, such as fluorescence line narrowing and spectral hole-burning [1]. These techniques enable convenient addressing of thousands of molecular subsets selected by their transition energy.
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.
The use of persistent spectral hole burning in optical data storage allows an increase of the storage density up to a factor of 1000 compared to the common spatial matrix of optical bits.1 The information is stored by burning at low temperature a sequence of narrow spectral holes in the inhomogeneously broadened optical transition of optical centers, e.g. dye molecules embedded in an amorphous polymer, with a tunable narrow-bandwidth laser. One bit of information is encoded by the presence or absence of a hole at a given location in frequency space. The information is read by observing the absorption or the fluorescence of the storage material using a laser with tunable frequency. One of the problems of spectral hole burning data storage arises from the fact that for addressing the memory locations the laser frequency has to be changed over a large frequency range with high accuracy and speed.
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.