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

Spatial Light Modulation By Nonlinearly Absorbing Molecules

Shammai Speiser, David Dantsker, Meir Orenstein

Published Jan 31, 1989• 0 citations
Publisher

Abstract

A novel spatial light modulator (SLM) based on nonlinear absorption of light by excited molecules is suggested. A kinetic analysis is applied to calculate the relative populations of molecular levels in singlet and triplet manifolds. It is shown that for many actual cases a probe light can be modulated by propagating through a medium excited by another light source.

DOI
10.1117/12.950000

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A novel spatial light modulator (SLM) based on nonlinear absorption of light by excited molecules is suggested. A kinetic analysis is applied to calculate the relative populations of molecular levels in singlet and triplet manifolds. It is shown that for many actual cases a probe light can be modulated by propagating through a medium excited by another light source.
A novel spatial light modulator (SLM) based on nonlinear absorption of light by excited molecules is suggested. A kinetic analysis is applied to calculate the relative populations of molecular levels in singlet and triplet manifolds. It is shown that for many actual cases a probe light can be modulated by propagating through a medium excited by another light source. The dependence of the molecular SLM on the photophysical parameters of the SLM medium is discussed. The same type of molecular nonlinearities can be utilized for optical bistability, as is demonstrated for some dyes.
We already discussed the bistable behavior of a Fabry Perot resonator filled with molecular media as well as the characteristics of a spatial light modulator (SLM) based on the nonlinearity induced by excited state absorption. In the present paper we present two practical configurations. First we analyze a cavity-less bistable element which removes some of the realization problems related to high finess cavity. In this configuration the nonlinear medium is located in one arm of an optical interferometer. The scheme provides the required amount of positive feedback by the bistable mechanism -- but without a cavity. We applied the nonlinear eikonal approximation, a method which takes care of the detailed propagation effects, and obtained conditions for bistability, as well as optimizing the design parameters such as the output mirror reflectivity, etc.
By applying a sufficiently intense beam of off-resonant light, simultaneously with a conventional excitation source beam, the efficiencies of one- and two-photon absorption processes may be significantly modified. The nonlinear mechanism that is responsible, known as laser modified absorption, is fully described by a quantum electrodynamical analysis. The origin of the process, which involves stimulated forward Rayleigh-scattering of the auxiliary beam, relates to higher order terms which are secured by a time-dependent perturbation treatment. These terms, usually inconsequential when a single beam of light is present, become prominent under the secondary optical stimulus – even with levels of intensity that are moderate by today’s standards. Distinctive kinds of behaviour may be observed for chromophores fixed in a static arrangement, or for solution- or gas-phase molecules whose response is tempered by a rotational average of orientations. In each case the results exhibit an interplay of factors involving the beam polarisations and the molecular electronic response. Special attention is given to interesting metastable states that are symmetry forbidden by one- or two-photon absorption. Such states may be accessible, and thus become populated, on input of the auxiliary beam. For example, in the one-photon absorption case, terms arise that are more usually associated with three-photon processes, corresponding to very different selection rules. Other kinds of metastable state also arise in the two-photon process, and measuring the effect of applying the stimulus beam to absorbances of such character adds a new dimension to the information content of the associated spectroscopy. Finally, based on these novel forms of optical nonlinearity, there may be new possibilities for quantum non-demolition measurements.
The main achievements in our research on the physical phenomena of the excited-state nonlinear absorption in a molecular system and its applications in photonic technology are described. In the first part of this paper, some energy-level models and rate-equations are used to explain various mechanisms of the excited-state nonlinear absorption under different conditions, such as reverse saturable absorption caused by the triplet and/or the singlet excited-state absorption; saturable absorption due to the first and/or the second singlet excited-state absorption; and the excited-state nonlinear absorption induced by two-photon absorption. The experimental results for metal-organic and C 60 materials irradiated by ps and ns laser pulses are consistent with the simulated curves of the transmittance versus fluences. In the second part, the applications of excited-state nonlinear absorption in photonic techniques including optical bistability, optical switching, optical limiting, optical modulation, optical logic and optical storage are introduced. The working principles of the photonic devices based on the excited-state nonlinear absorption are presented. The experimental characteristic curves are found in good agreement with the theoretical simulations for these devices.
It is shown that if two light beams intersect in a medium containing the appropriate molecule, one beam can modulate the other by making use of the differences in the absorption spectra of the ground and excited molecular states. This is possible even with the power of semiconductor lasers. From this, an opto–optical modulating device can be conceived which would have micrometer dimensions, potentially fast response time, and significant quantum gain. Such a device could find use in optical communications and optical computing.