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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Influence of matrix-dopant interactions for all-optical memorization in doped xerogels

F.F.L. Bentivegna, Michael Canva, Alain Brun, Fréderic Chaput, Jean‐Pierre Boilot

Published Oct 13, 1994• 0 citations
Publisher

Abstract

We show that including highly polarizable dopants in the pores of a xerogel matrix leads to interesting optical properties and applications, such as an all-optical molecular memory device. By submitting the sample to ultrashort linearly polarized optical pulses, we demonstrate that the dopants tend to align along the direction of the electric field of the optical wave like in classical optical Kerr effect, and that the new alignment of the molecules is partially maintained. We study the influence of the matrix-dopant interactions on this phenomenon. For example, for rhodamine-like molecules, we establish that the alignment ability as well as the relaxation times depend strongly on the structure of the gel network and on the coupling intensity between the host matrix and the guest molecule.

DOI
10.1117/12.188998

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We show that including highly polarizable dopants in the pores of a xerogel matrix leads to interesting optical properties and applications, such as an all-optical molecular memory device. By submitting the sample to ultrashort linearly polarized optical pulses, we demonstrate that the dopants tend to align along the direction of the electric field of the optical wave like in classical optical Kerr effect, and that the new alignment of the molecules is partially maintained. We study the influence of the matrix-dopant interactions on this phenomenon. For example, for rhodamine-like molecules, we establish that the alignment ability as well as the relaxation times depend strongly on the structure of the gel network and on the coupling intensity between the host matrix and the guest molecule.
We have studied the behavior of organic molecules (Rhodamine 640) that are encaged in a matrix synthesized by the sol-gel process. By applying a strong optical-polarized electric field, we can control the alignment of the molecules within the sample and locally create a birefringent effect. Using this sample in a Kerr experiment, we obtained a transmission ratio of 6%. Since the birefringent effect lasts at least several days, this type of sample could be used in an optical process for storage of information. Moreover, we show that such information can be deleted and rewritten repetitively.
The properties of molecule-optical elements such as lenses or prisms based on the interaction of molecules with optical fields depend in a crucial way on the molecular quantum state and its alignment created by the optical field. Herein, we consider the effects of state-dependent alignment in estimating the optical dipole force acting on the molecules and, to this end, introduce an effective polarizability which takes proper account of molecular alignment and is directly related to the alignment-dependent optical dipole force. We illustrate the significance of including molecular alignment in the optical dipole force by a trajectory study that compares previously used approximations with the present approach. The trajectory simulations were carried out for an ensemble of linear molecules subject to either propagating or standing-wave optical fields for a range of temperatures and laser intensities. The results demonstrate that the alignment-dependent effective polarizability can serve to provide correct estimates of the optical dipole force, on which a state-selection method applicable to nonpolar molecules could be based. We note that an analogous analysis of the forces acting on polar molecules subject to an inhomogeneous static electric field reveals a similarly strong dependence on molecular orientation.
We report on the ability to tailor the optical dipole force for molecules by tuning their effective polarizability with strong field alignment using polarized fields. We have measured a difference of 20% in the dipole force on cold CS2 molecules when changing from linear to near-circular polarization using peak field intensities of 5.7x10(11) W cm(-2). A variation in the focal length with laser polarization of a molecular-optical lens formed by a single focused laser beam was also measured. This provides a new way of modifying this force for many molecules.
An overview of recent results concerning molecular doped solids is presented. The hole burning performances and the photophysics of polymer and xerogel-based systems are compared. Three areas are considered in more detail: the problem of electron-phonon coupling, the one of high-temperature persistent spectral hole burning materials, and the search for new frequency-selective photosensitive systems for fast optical pulse processing at 800 nm. This comparison demonstrates that molecular doped polymers and molecular doped xerogels have similar hole burning behavior but mechanisms in these systems can be different. However, in respect of the areas considered, inorganic hosts based on silicate xerogels or porous glasses have shown the best results. Moreover, all the possibilities of hybrid xerogels created by combining inorganic and organic capabilities or by grafting organic species to the host have not yet been revealed.
Relaxation processes of dye molecules doped in polymer hosts have been understood by various kinds of interaction, such as the dipole-dipole interaction between molecules, the interaction with the two-level systems (TLS) in the host polymer and the electron-phonon interaction. The study on these interactions has been conducted to search for new efficient materials for the photonic device such as, for example, an optical memory. We present how the charge-transfer (CT)-like interaction between a donor and an acceptor molecule affect the dephasing property in the dye/polymer system. The CT-like interaction has not been investigated in dye-doped polymer system so far. We detect the effect of the CT-like interaction by using a degenerate four-wave-mixing technique (photon echoes) since it can conveniently probe the weak interactions between molecules as the change of the polarization decay rate. The sample system we employed is the cresyl violet (CV) doped polymers (polyvinyl alcohol (PVA) and polymethyl methacrylate (PMMA)), to which the nitrobenzene molecules are introduced to induce the interaction with the CV molecule.