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Photon gated persistent spectral hole burning for the meso-tetra-p-tolyl-Zn-tetrabenzoporphyrin/chloroform system in poly(methylmethacrylate): temperature dependence

W. Patrick Ambrose, W. E. Moerner

Published May 21, 1990• 0 citations
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Abstract

Persistent spectral hole burning has been utilized as both a tool for studying relaxation processes in amorphous solids1 and a means for possibly achieving high density frequency domain optical storage.2 In photon-gated hole burning, two photons (ideally of different wavelengths) are required to induce the photochemical reaction leading to hole formation. In effect, the first photon produces the site selection, and the second photon acts as a gate on the photochemistry.

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Persistent spectral hole burning has been utilized as both a tool for studying relaxation processes in amorphous solids1 and a means for possibly achieving high density frequency domain optical storage.2 In photon-gated hole burning, two photons (ideally of different wavelengths) are required to induce the photochemical reaction leading to hole formation. In effect, the first photon produces the site selection, and the second photon acts as a gate on the photochemistry.
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)
Photochemical spectral hole-burning (PSHB) has attracted particular attention in the past decade because of its potential for frequency domain optical storage. In order to apply PSHB to a practical optical memory, the material should have high burning temperature, high thermal stability, erasability and high frequency multiplexing. Two ways are possible to increase the storage density: one is to narrow the homogeneous line width, the other is to broaden the inhomogeneous line width. In previous works, the larger inhomogeneous line width (greater than 1,000 cm–1) has been reached in polymethylmethacrylate (PMMA) doped with two kinds of Zn-benzoporphyrin derivatives with roughly the same hole-burning efficiencies [1]. In this paper, the authors investigate systematically the optical properties of Zn-benzoporphyrin derivatives, their hole-burning mechanisms, thermal stability and electron-phonon coupling in cellulose acetate (CA) and in PMMA matrices. The choice of CA was motivated mainly by the fact this polymer allows to prepare samples with excellent optical quality.
In photon-gated spectral hole burning, a hole is formed via a higher excited state produced by simultaneous laser irradiation at two different wavelengths1). One is the wavelength-selective light which promotes the ground state molecules to the first excited state, and the other is the gating light which promotes the excited molecules to the higher excited reaction sate. Only the wavelength-selective light is required to read out spectral holes and the recorded holes are not destroyed. Moreover, the gating light pumps the molecules up to the reaction state effectively, which may break through the bottleneck effect and enhance the recording sensitivity.
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.