The spatial redistribution of energy resulting from the interaction between a near-diffraction-limited nanosecond laser pulse and the nonlinear absorbing optical limiting dye silicon naphthalocyanine is described, for what is to our knowledge the first time, in an optical geometry that is likely to be found in practical applications. For input fluences above that required for nonlinear absorption but below that for bubble growth, a plane wave or Gaussian spatial input evolves unexpectedly to a sharp central spike and a well-defined outer ring. The observed energy redistribution is thought to rely on a combination of nonlinear processes, since a pure absorptive process alone cannot explain the profiles presented. A model involving nonlinear absorption and nonlinear refraction qualitatively reproduces the observed spatial profiles. It is clear from the results that the performance of optical limiting dyes in representative optical geometries, even at fluences well below that required for bubble growth, cannot be described solely by nonlinear absorption.

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The response of organic dyes to laser pulses is typically described solely by nonlinear absorption. Recently, spatial profiles of a nanosecond pulse exiting an organic nonlinear absorber have shown energy redistribution from a Gaussian input profile to a central spike and outer ring. It was suggested that the spike and ring resulted from both nonlinear absorption and nonlinear refraction. In this letter, the role of a thermal nonlinear refraction in beam shaping is demonstrated using single and time-delayed double picosecond pulses. It is concluded that the dynamics of nonlinear absorption and nonlinear refraction must be included to correctly describe the laser-material interaction.

Iron doped lithium niobate (Fe:LiNbO3) in a simple focal plane geometry has demonstrated efficient optical limiting through two-beam coupling. The performance is largely independent of the total Fe concentration and the oxidation state of the Fe ions, providing the linear optical transmission of uncoated crystals is between 30% and 60%. Fe has been found to be the best dopant for LiNbO3, giving the widest spectral coverage and the greatest optical limiting. Optical limiting in Fe:LiNbO3 has been shown to be very much greater than predicted by simple diffusion theory. The reason for this is a higher optical gain than expected. It is suggested that this may be due to an enhancement of the space-charge field arising from the photovoltaic effect. The standard two-beam coupling equations have been modified to include the effects of the dark conductivity. This has produced a theoretical intensity dependence on the ΔOD which closely follows the behaviour observed in the laboratory. A further modification to the theory has also shown that the focusing lens f-number greatly affects the optical limiting characteristics of Fe:LiNbO3. A lens f-number of approximately 20 gives the best results.

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