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Persistant Spectral Hole-Burning: Photon-Gating and Fundamental Statistical Limits

W. E. Moerner

Published Nov 3, 1989• 0 citations
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Abstract

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.

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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 (PHB) has been proposed as the essential element of a frequency domain optical storage system1 in which the frequency at which a hole is burned in an inhomogeneously broadened absorption line at low temperatures serves as an additional dimension for the storage of digital information. Essentially all of the mechanisms studied until recently have been single-photon mechanisms, i.e., the photoionduced change leading to hole-burning (writing) for a given center occurs with a certain fixed probability after the absorption of one photon. Such linear, monophotonic processes suffer from the drawback that the act of detecting holes (reading) can also produce changes in the absorption line. Recent modeling studies of the generalized single-photon process2 have shown that thousands to tens of thousands of reads can be obtained from single-photon mechanisms only when the material possesses high quantum efficiency and low absorption cross section. These restrictive requirements do not apply for photon-gated hole-burning mechanisms, i.e., those mechanisms for which hole-burning occurs only in the presence of an additional “gating” light source, because for these mechanisms, reading is performed in the absence of the gating light and is therefore nondestructive.
To determine the complete set of required materials properties for a viable frequency-domain optical-storage system based on persistent spectral hole burning, we have performed analytic and computer simulations of the writing performance, signal-to-noise ratio, and number of reads that can be obtained from single-photon or monophotonic (no threshold) hole-burning mechanisms with realistic spot sizes and reading and writing times. We find that acceptable reading performance occurs only for materials with high quantum efficiencies, low absorption cross sections, and high solubilities. This work for the first time clearly defines the parameter space of single-photon materials that can be utilized in a frequency-domain optical-storage system.
Persistent spectral hole-burning (PHB) is a phenomenon that allows an additional dimension, the frequency at which spectral holes are written, to be used to encode digital data. PHB can be used to store a large number of bits of information in the volume irradiated by a focused laser beam, leading to a possible future storage technology, frequency domain optical storage. A large number of photochemical and photophysical mechanisms have led to the production of spectral holes; a wealth of information has been learned about host-guest interactions, dephasing, and solid-state photochemistry at low temperatures. The general structure of a frequency domain optical store places a set of constraints on the engineering of such a system as well as on the materials used as recording media. The dynamics of the hole-burning process are crucial; for monophotonic mechanisms in particular, a set of stringent constraints can be derived that limit the applicability of this class of materials. Recent discoveries of two-color, photon-gated hole-burning offer special promise for nondestructive reading and improved performance.
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.