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New technique for degenerate two-photon absorption spectral measurements using femtosecond continuum generation

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Abstract

We present a new technique for direct measurements of degenerate two-photon absorption (TPA) spectra of two-photon absorbing materials including non-fluorescent samples. This technique is based on the use of an intense single continuum-generation beam as the coherent white-light source with specially flattened spectral distribution. The different spectral components of the continuum beam are spatially dispersed and then passed through the sample material along different pathways so that nondegenerate TPA processes among different input spectral components can be avoided. By comparing the input and transmitted continuum spectral distributions, the TPA spectrum for a given sample can be obtained. As an example, the continuous TPA spectrum (from 550 to 1000 nm) is measured for a novel two-photon-absorbing compound (AF-389) which exhibits an extremely high TPA cross-section value of ~1×10-20 cm4/GW, or ~249 GM, around ~800-nm spectral range in femtosecond regime.

©2002 Optical Society of America

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Figures (4)

Fig. 1.
Fig. 1. Experimental setup for white light continuum generation and degenerate TPA spectral measurement. ND: neutral density filters.
Fig. 2.
Fig. 2. Relative spectral curves of the continuum generation from heavy water: (a) at eight different input average power levels from 0.4 to 35 mW, (b) at 35-mW input level but after passing through a spatially selective silver-strip coating attenuator.
Fig. 3.
Fig. 3. Chemical structure of AF389, a strongly two-photon absorbing chromophore.
Fig. 4.
Fig. 4. (a) Relative spectral intensity distributions of the continuum after passing through a pure THF sample and an AF389/THF sample respectively, (b) Intensity-dependent transmissivity change due to AF389 chromophore, and (c) Relative TPA coefficient curve as a function of wavelength for AF389 in THF.

Equations (5)

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T ( λ ) = I AF ( λ ) I THF ( λ )
T ( λ ) = 1 1 + βzI THF ( λ ) .
β ( λ ) = 1 T ( λ ) I THF T ( λ ) z = 1 T ( λ ) I AF ( λ ) z .
σ 2 ( λ ) = β ( λ ) N A d 0 × 10 3 ( cm 4 GW ) ,
σ 2 ( λ ) = × σ 2 ( λ ) = × β ( λ ) N A d 0 × 10 3 ( cm 4 sec ) .
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