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International Conference on Luminescence - 1984

Nonlinear Optical Properties of Fluorescein in Glass

M. A. Kramer, Jerzy S. Krasiński, Robert W. Boyd

Published Jan 1, 1984• 0 citations
Publisher

Abstract

There is much interest in materials displaying a small saturation intensity for use in four-wave mixing and optical bistability. In this paper we report on one such material comprised of fluorescein dye molecules imbedded in a matrix of boric acid glass. This material shows a luminescence decay time of about 2 sec and hence an extremely small saturation intensity which we have measured to be about 10 mW/cm2. We have found that four-wave mixing can easily be observed at intensities of 10 mW/cm2.

DOI
10.1364/icol.1984.we21

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Applied Physics Letters•Mar 10, 2008•1 citation
There is much interest in materials displaying a small saturation intensity for use in four-wave mixing and optical bistability. In this paper we report on one such material comprised of fluorescein dye molecules imbedded in a matrix of boric acid glass. This material shows a luminescence decay time of about 2 sec and hence an extremely small saturation intensity which we have measured to be about 10 mW/cm2. We have found that four-wave mixing can easily be observed at intensities of 10 mW/cm2.
Optical bistability has been observed in highly concentrated substituted fluorescein dye solution and in thin (∼1 μm) doped polymeric films. For fluorescein, at concentrations larger than 10−5 mol/ℓ dye dimers are formed. The dimer–monomer equilibrium constant is 105 ℓ/mol so that most of the dye species are in the dimer form. At 480 nm the dimer absorption cross section is 10−18 cm2/molecule, while that for the dye monomer molecule is 7.6×10−17 cm2/molecule. Upon laser excitation dimers dissociate to form monomers thus providing a highly nonlinear laser induced absorption. The high nonlinear absorption coefficient can be utilized for optically bistable response of the dye system. Optical bistability was observed by placing dye solutions or dye thin films inside a Fabry–Perot resonator and exciting it with 480 nm dye laser pulses of 10 ns duration. The effect is more pronounced in 10−4 mol/ ℓ fluorescein than in 10−6 mol/ℓ fluorescein in which dimer formation is not that efficient. In disodium fluorescein, eosin Y and erythrosin B no significant dimer formation is observed even at 10−3 mol/ℓ dye concentration. The observed bistability both in solution and in thin films can be explained in terms of recent models for optical bistability in nonlinearly absorbing molecular system.
Optical bistability has been observed in highly concentrated fluorescein dye solutions and in thin (-1 pm) doped polymeric films. At concentrations larger than 10-5 mole/k dye dimers are formed. For fluorescein dye, the dimer-monomer equilibrium constant is 10 -5 mole/ℓ so that most of the dye species are in the dimer form. At 480 nm the dimer absorption cross section is 10-18 cm2/molecule, while that for the dye monomer molecule is 7.6 x 10-17 cm2/molecule. Upon laser excitation dimers dissociate to form monomers thus providing a highly nonlinear laser induced absorption. This high nonlinear absorption coefficient can be utilized for optically bistable response of the dye system. Optical bistability was observed by placing dye solutions or dye thin films inside a Fabry-Perot resonator and exciting it with 480 nm dye laser pulses of 10 ns duration. The effect is more pronounced in 10-4 mole/ℓ fluorescein than in 10-6 mole/k fluorescein in which dimer formation is not that efficient.
Rigidly held molecules display nonlinear optical properties which differ substantially from the properties of isotropic absorbers.1 In particular, the absorption of a collection of randomly oriented, rigidly held molecules saturates differently for different polarization states. We show that the polarization properties of degenerate four-wave mixing in such a medium are dramatically modified by this polarization-dependent saturation. We predict theoretically that for linearly polarized pump waves and for an input intensity near the saturation intensity, degenerate four-wave mixing in this material system can lead directly to vector phase conjugation; that is, to the simultaneous reversal of the optical wavefront and conjugation of the polarization state of the incident optical field.2 We confirm these theoretical predictions through phase conjugation experiments using fluorescein doped boric acid glass as the material system, and we find that degenerate four-wave mixing leads to nearly perfect vector phase conjugation when pumped by linearly polarized pump waves for field strengths near the saturation intensity.
Optical bistability has been observed in highly concentrated fluorescein dye solution and in thin (~1 μm) doped polymeric films. For fluorescein, at concentrations larger than 10-5 mole/1 dye dimers are formed. The dimer-monomer equilibrium constant is 1051/mole so that most of the dye species are in the dimer form. At 480 nm the dimer absorption cross section is 10-18cm2/molecule, while that for the dye monomer molecule is 7.6x10-17cm2/molecule. Upon laser excitation dimers dissociate to form monomers thus providing a highly nonlinear laser induced absorption. The high nonlinear absorption coefficient can be utilized for optically bistable response of the dye system. Optical bistability was observed by placing dye solutions or dye thin films inside a Fabry-Perot resonator and exciting it with 480 nm dye laser pulses of 10 ns duration. The effect is more pronounced in 10-4; mole/1 fluorescein than in 10-6mole/1 fluorescein in which dimer formation is not that efficient. In disodium fluorescein, eosin and erythrosin dye samples no significant dimer formation is observed even at 10-3 mole/1 dye concentration. The observed bistability in both solution and in thin films can be explained in terms of recent models for optical bistability in nonlinearly absorbing molecular systems.
The optical phase conjugation signal in nearly nondegenerate four wave mixing was studied using a rhodamine 110 doped boric acid glass saturable absorber nonlinear medium. We have demonstrated a narrow band optical filter (2.56±0.15Hz) using an optical phase conjugation signal in the frequency modulation of a weak probe beam in the presence of two strong counterpropagating pump beams in rhodamine 110 doped boric acid glass thin films (10−4m). Both the pump beams and the probe beam are at a wavelength of 488nm (continuous-wave Ar+ laser). The probe beam frequency was detuned with a ramp signal using a piezoelectric transducer mirror.