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Conference on Lasers and Electro-Optics

TWO-COLOR, PHOTON-GATED SPECTRAL HOLE-BURNING

W. E. Moerner, Manfred Gehrtz, Howard W. H. Lee, R. M. Macfarlane, Ernesto E. Marinero, Robert M. Shelby, Albrecht Winnacker

Published Jan 1, 1985• 0 citations

Abstract

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.

DOI: 10.1364/cleo.1985.thz6

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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.

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We have observed photon-gated spectral hole burning, i.e., hole burning that occurs only in the presence of an additional gating-light source. Gating enhancement factors of 10(4) were observed. In BaClF:Sm(2+) this involves two step photoionization of Sm(2+) and leads to persistent holes in the (4)F(0) --> (5)D(0) (687.9-nm) and (7)F(0) --> (5)D(1) (629.7-nm) absorption lines. The hole widths of 25 MHz at 2 K are much narrower than the inhomogeneous broadening of 16 GHz. The action spectrum of the gating shows a threshold behavior around 2.5 eV. Erasing studies show that Sm(3)+ acts as a trap for the released electrons. A remarkable and novel feature is that the holes can be recovered after temperature cycling to 300 K.

Optics Letters•Jul 1, 1985•234 citations

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.

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.

Persistent spectral hole-burning (PHB) permits use of the optical frequency for encoding digital information through the presence and absence of spectral holes that are burned in inhomogeneously broadened absorption lines at low temperatures. The combination of spectral and spatial data recording can make storage densities of 1010 bits/cm2 possible. The most challenging innovation needed to achieve a practical storage system is presented by the complex materials requirements1 on a successful storage medium.

Persistent spectral hole-burning (PHB, also called photochemical hole-burning) permits use of the optical frequency for encoding digital information through the presence and absence of spectral holes that are burned in inhomogeneously broadened absorption lines at low (liquid helium) temperatures. The optical frequency or wavelength at which a given hole is burned acts as an additional dimension for data storage, hence this optical recording scheme has been called Frequency Domain Optical Storage (FDOS). The combination of spectral and spatial data-recording can make storage densities in excess of 1010 bits/cm2 possible; furthermore, since rotation of the recording medium is not necessary, shorter random access times will result. The future success of the FDOS concept will rely on progress in several technological and engineering areas as well as on advances in several critical materials areas1.

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.

Photochemical Hole Burning (PHB) has attracted considerable interest not only as a tool for high resolution spectroscopy of amorphous solid at low temperature but also as a possible means for freguency-domain high-density optical storage.1) Many recent investigations have been devoted to a photon-gated mechanism because it allows nondestructive readout in utilizing PHB for a practical optical memory system. The mechanisms of previously reported photon-gated PHB systems are two-step photoionization, photodecomposition, and photoinduced donor-acceptor electron transfer reactions.1)

We have observed photon-gated spectral hole burning, i.e., hole burning that occurs only in the presence of an additional gating-light source. Gating enhancement factors of 10(4) were observed. In BaClF:Sm(2+) this involves two step photoionization of Sm(2+) and leads to persistent holes in the (4)F(0) --> (5)D(0) (687.9-nm) and (7)F(0) --> (5)D(1) (629.7-nm) absorption lines. The hole widths of 25 MHz at 2 K are much narrower than the inhomogeneous broadening of 16 GHz. The action spectrum of the gating shows a threshold behavior around 2.5 eV. Erasing studies show that Sm(3)+ acts as a trap for the released electrons. A remarkable and novel feature is that the holes can be recovered after temperature cycling to 300 K.