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Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Editor: G. I. Stegeman
  • Vol. 23, Iss. 5 — May. 1, 2006
  • pp: 932–950

Spectroscopy of third-harmonic generation: evidence for resonances in model compounds and ligated hemoglobin

G. Omar Clay, Andrew C. Millard, Chris B. Schaffer, Juerg Aus-der-Au, Philbert S. Tsai, Jeffrey A. Squier, and David Kleinfeld  »View Author Affiliations

JOSA B, Vol. 23, Issue 5, pp. 932-950 (2006)

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We report on third-harmonic generation (THG) of biomolecular solutions at the fluid/glass interface as a means to probe resonant contributions to their nonlinear absorption spectra that could serve as contrast mechanisms for functional imaging. Our source was 100 fs laser pulses whose center wavelength varied from 760 to 1000 nm . We find evidence of a two-photon resonance in the ratio of third-order susceptibilities, χ sample ( 3 ) ( 3 ω ) χ glass ( 3 ) , for aqueous solutions of Rhodamine B, Fura-2, and hemoglobin and a three-photon resonance in χ sample ( 3 ) ( 3 ω ) χ glass ( 3 ) for solutions of bovine serum albumin. Consistent with past work, we find evidence of a one-photon resonance of χ sample ( 3 ) ( 3 ω ) χ glass ( 3 ) for water, while confirming a lack of resonant enhancement for benzene. At physiological concentrations, hemoglobin in different ligand-binding states could be distinguished on the basis of features of its THG spectrum.

© 2006 Optical Society of America

OCIS Codes
(120.6200) Instrumentation, measurement, and metrology : Spectrometers and spectroscopic instrumentation
(170.3880) Medical optics and biotechnology : Medical and biological imaging
(190.4160) Nonlinear optics : Multiharmonic generation
(190.4180) Nonlinear optics : Multiphoton processes
(190.4350) Nonlinear optics : Nonlinear optics at surfaces
(190.4710) Nonlinear optics : Optical nonlinearities in organic materials
(300.6420) Spectroscopy : Spectroscopy, nonlinear

ToC Category:

Original Manuscript: September 2, 2005
Revised Manuscript: November 17, 2005
Manuscript Accepted: November 18, 2005

Virtual Issues
Vol. 1, Iss. 6 Virtual Journal for Biomedical Optics

G. Omar Clay, Andrew C. Millard, Chris B. Schaffer, Juerg Aus-der-Au, Philbert S. Tsai, Jeffrey A. Squier, and David Kleinfeld, "Spectroscopy of third-harmonic generation: evidence for resonances in model compounds and ligated hemoglobin," J. Opt. Soc. Am. B 23, 932-950 (2006)

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