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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Light-induced broadening in hole-burning systems: Reversible and irreversible contributions

W. Richter, K. Barth

Published Jan 1, 1992• 0 citations
Publisher

Abstract

The profile of a persistent spectral hole can be used to very sensitively detect induced broadening processes that are caused by infrared radiation absorbed in the host matrix /1,2/. Both, the hole area and the hole width are affected to an extent which depends on the frequency of the irradiated IR-light. The excitation of specific vibrations in the host matrix leads to the observed broadening and filling phenomena of a hole spectrum which are highly selective with respect to different vibrational modes.

DOI
10.1364/shbl.1992.tub22

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STIN•Nov 3, 1989•0 citations
The profile of a persistent spectral hole can be used to very sensitively detect induced broadening processes that are caused by infrared radiation absorbed in the host matrix /1,2/. Both, the hole area and the hole width are affected to an extent which depends on the frequency of the irradiated IR-light. The excitation of specific vibrations in the host matrix leads to the observed broadening and filling phenomena of a hole spectrum which are highly selective with respect to different vibrational modes.
The change in the profile of a spectral hole can be used to detect tunneling processes in glassy matrices as well as light-induced changes of molecular configurations. The broadening of photochemical holes as well as hole-filling processes are very sensitive probes for molecular rearrangements arround the embedded dye molecules /1/. Light-induced spectral diffusion in polymeric systems is highly selective with respect to the optical excitation of vibrational modes of the surrounding molecular groups.
Persistent spectral hole-burning (PHB) of inhomogeneously broadened absorption lines in solids occurs when a homogeneous class of absorbing centers in resonance with a narrowband laser beam undergoes a photolnduced change in optical absorption that persists for times longer than any excited state lifetime. Persistent spectral holes for impurity centers in solids can provide important information about guest–light and guest–host interactions, such as dephasing, Zeeman and Stark splittings, and photochemical reaction mechanisms.
One very exciting application of laser spectroscopy would be to use the high-resolution capabilities of today’s lasers and the phenomenon of persistent spectral hole-burning to form a frequency domain optical storage system.1 In such a system, bits of information would be stored by locally modifying (in the frequency domain) the shape of an inhomogeneously broadened absorption line of an absorber in a solid at low temperatures. Because typical homogeneous widths are 1000X (or more) narrower than typical inhomogeneous widths, as many as 1000 bits could be written in one diffraction-limited 1-μm spot In a sample, yielding the impressive storage density of 1011 bits/cm2.
The persistent spectral hole-burning (PSHB) phenomenon was observed in semiconductor quantum dots, CdSe , CuCl , and CuBr , embedded in glass and crystal. In inhomogeneously broadened exciton absorption spectra of these dots, the narrow bleaching hole and its associated structure are made by the narrowband laser excitation and are conserved for more than several hours at 2 K after the laser irradiation. The observation of the PSHB phenomenon in these four kinds of samples shows the generality of the phenomenon in semiconductor quantum dots and requires the existence of more than one ground-state configurations of the total system consisting of quantum dots and surrounding matrix. It means that not only the size distribution but also these ground-state configurations give inhomoge-neous broadening to semiconductor quantum dots. Thermally annealing and light-induced hole-filling phenomena were observed. Hole-burning and hole-filling mechanisms are discussed. Quantum dots consisting of 103–104 atoms behave like molecules or ions in matrix to give the PSHB phenomenon.
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.