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Optics Express

Optics Express

  • Editor: Michael Duncan
  • Vol. 14, Iss. 18 — Sep. 4, 2006
  • pp: 8434–8447

Absolute measurement of molecular two-photon absorption cross-sections using a fluorescence saturation technique

Martin Kauert, Patrick C. Stoller, Martin Frenz, and Jaro Rička  »View Author Affiliations


Optics Express, Vol. 14, Issue 18, pp. 8434-8447 (2006)
http://dx.doi.org/10.1364/OE.14.008434


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Abstract

We have developed a fluorescence saturation technique for accurate measurements of the absolute molecular two-photon absorption (TPA) cross-section of fluorescent dyes. We determine the TPA cross-section both from measurements at excitation intensities well below saturation onset (in the square power-law regime) and from data obtained near the onset of saturation. The two estimates have different sensitivities to potential sources of errors. Using the square power-law regime requires calibration of the overall collection efficiency of the detection channel, including the quantum yield of the dye. In the saturation regime, the two key requirements are a good knowledge of the excitation profile and an adequate model of the two-photon excitation transition. To fulfill the former requirement, we developed diagnostic tools to characterize the tightly focussed excitation beam. To satisfy the latter requirement, we included the correct polarization dependent averaging over molecular orientations in our model. We measured the TPA cross-section of Rhodamine B (RhB) and Rhodamine 6g (Rh6g) in methanol at 798 nm for linear and circular polarization. For RhB we observed excellent agreement between the TPA cross-section estimate 〈σ2〉 obtained from the square power-law regime and that obtained from the saturation regime, 〈σ2 sat . For the case of linear polarization we found: 〈σ2〉 = 12 ± 2 GM and 〈σ2 sat = 10.5 ± 2 GM. For the case of circular polarization we obtained: 〈σ2〉 = 8.4 ± 2 GM and 〈σ2 sat = 7.5 ± 2 GM. The results obtained with linear polarization are in good agreement with previously published non-linear transmission data (δ = 2σ = 20.4 GM at 800nm). For Rh6g the difference between 〈σ2〉 and 〈σ2 sat is larger, but still considerably smaller than the variance of σ2 values found in the literature.

© 2006 Optical Society of America

OCIS Codes
(180.2520) Microscopy : Fluorescence microscopy
(190.4180) Nonlinear optics : Multiphoton processes
(300.2530) Spectroscopy : Fluorescence, laser-induced
(300.6410) Spectroscopy : Spectroscopy, multiphoton

ToC Category:
Spectroscopy

History
Original Manuscript: June 7, 2006
Revised Manuscript: August 18, 2006
Manuscript Accepted: August 23, 2006
Published: September 1, 2006

Virtual Issues
Vol. 1, Iss. 10 Virtual Journal for Biomedical Optics

Citation
Martin Kauert, Patrick C. Stoller, Martin Frenz, and Jaro Rička, "Absolute measurement of molecular two-photon absorption cross-sections using a fluorescence saturation technique," Opt. Express 14, 8434-8447 (2006)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-14-18-8434


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