Abstract

The third-order nonlinear susceptibility (χ(3)) can be measured quantitatively using third-harmonic generation (THG) from two different interfaces. For the first time it is demonstrated both in experiments and theory that the magnitude of the THG signals from the two interfaces is not only determined by material properties (refractive index and χ(3)), but also by optical aberrations. It is found that this method of χ(3) determination can be applied without additional correction factors only for focusing conditions with a numerical aperture (NA) ≤ 0.35. The implications for general application of THG in three-dimensional microscopy are discussed.

© 2006 Optical Society of America

Full Article  |  PDF Article

References

  • View by:
  • |
  • |
  • |

  1. Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear Scanning Laser Microscopy by Third Harmonic Generation,” Appl. Phys. Lett. 70, 922–924 (1997).
    [Crossref]
  2. M. Müller, J. Squier, K. R. Wilson, and G. J. Brakenhoff, “3D Microscopy of transparent objects using third-harmonic generation,” J. Microsc. 191, 266–274 (1998).
    [Crossref] [PubMed]
  3. J. F. Ward and G. H. C. New, “Optical Third Harmonic Generation in Gases by a Focused Laser Beam,” Phys. Rev. 185, 57–72 (1969).
    [Crossref]
  4. R. W. Boyd, Nonlinear Optics (Academic Press, Inc., New York, 1992).
  5. M. Born and E. Wolf, Principles of Optics (Pergamon Press, Oxford, 1993).
  6. J. F. Reintjes, Nonlinear Optical Parametric Processes in Liquids and Gases (Academic Press, Inc., Orlando, 1984).
  7. J. A. Squier, M. Müller, G. J. Brakenhoff, and K. R. Wilson, “Third Harmonic Generation Microscopy,” Opt. Express 3, 315–324 (1998).
    [Crossref] [PubMed]
  8. J. A. Squier and M. Müller, “Third - Harmonic Generation Imaging of laser - induced breakdown in glass,” Appl. Opt. 38, 5789–5794 (1999).
    [Crossref]
  9. D. Yelin and Y. Silberberg, “Laser scanning third-harmonic-generation microscopy in biology,” Opt. Express 5, 169 – 175 (1999).
    [Crossref] [PubMed]
  10. C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
    [Crossref]
  11. L. Canioni, S. Rivet, L. Sarger, R. Barille, P. Vacher, and P. Voisin, “Imaging of Ca2+ intracellular dynamics with a third-harmonic generation microscope,” Opt. Lett. 26, 515–517 (2001).
    [Crossref]
  12. D. Oron, E. Tal, and Y. Silberberg, “Depth-resolved multiphoton polarisation microscopy by third-harmonic generation,” Opt. Lett. 28, 2315–2317 (2003).
    [Crossref] [PubMed]
  13. D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, “Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy,” Appl. Phys. Lett. 74, 3107–3109 (1999).
    [Crossref]
  14. D. Débarre, W. Supatto, E. Farge, B. Moulia, M-C. Schanne-Klein, and E. Beaurepaire, “Velocimetric third-harmonic generation microscopy: micrometer-scale quantification of morphogenetic movements in unstained embryos,” Opt. Lett. 29, 2881–2883 (2004).
    [Crossref]
  15. S.-W. Chu, Szu-Yu Chen, Tsung-Han Tsai, Tzu-Ming Liu, Cheng-Yung Lin, Huai-Jen Tsai, and Chi-Kuang Sun, “In vivo developmental biology study using noninvasive multi-harmonic generation microscopy,” Opt. Express 11, 3093 – 3099 (2003).
    [Crossref] [PubMed]
  16. W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
    [Crossref] [PubMed]
  17. S. Hell, G. Reiner, C. Cremer, and E.H.K. Stelzer, “Aberrations in confocal fluorescence microscopy induced by mismatches in refractive index,” J. Microsc. 169, 391–405 (1993).
    [Crossref]
  18. C. J. R. Sheppard and C.J. Cogswell., “Effects of aberrating layers and tube length on confocal imaging properties,” Optik 87, 34–38 (1991).
  19. R. Barille, L. Canioni, L. Sarger, and G. Rivoire, “Nonlinearity measurements of thin films by third-harmonic-generation microscopy,” Phys. Rev. E 66 (2002).
    [Crossref]
  20. V. Shcheslavskiy, G. Petrov, and V. V. Yakovlev, “Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface,” Appl. Phys. Lett. 82, 3982–3984 (2003).
    [Crossref]
  21. V. Shcheslavskiy, G. I. Petrov, S. Saltiel, and V. V. Yakovlev, “Quantitative characterization of aqueous solutions probed by the third-harmonic generation microscopy,” J. Struct. Biol. 147, 42–49 (2004).
    [Crossref] [PubMed]
  22. J. M. Schins, T. Schrama, J. Squier, G. J. Brakenhoff, and M. Müller, “Determination of material properties by use of third-harmonic generation microscopy,” J. Opt. Soc. Am. B 19, 1627–1634 (2002).
    [Crossref]
  23. J. X. Cheng and X. S. Xie, “Green’s function formulation for third-harmonic generation microscopy,” J. Opt. Soc. Am. B 19, 1604–1610 (2002).
    [Crossref]
  24. F. Kajzar and J. Messier, “Third-harmonic generation in liquids,” Phys. Rev. A 32, 2352–2363 (1985).
    [Crossref] [PubMed]
  25. I. Z. Kozma, P. Krok, and E. Riedle, “Direct measurement of the group-velocity mismatch and derivatiion of the refractive-index dispersion for a variety of solvents in the ultraviolet,” J. Opt. Soc. Am. B 22, 1479–1485 (2005).
    [Crossref]
  26. G. R. Meredith, B. Buchalter, and C. Hanzlik, “Third-order susceptibility determination by third harmonic generation. II,” J. Chem. Phys. 78, 1543–1551 (1983).
    [Crossref]

2005 (2)

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

I. Z. Kozma, P. Krok, and E. Riedle, “Direct measurement of the group-velocity mismatch and derivatiion of the refractive-index dispersion for a variety of solvents in the ultraviolet,” J. Opt. Soc. Am. B 22, 1479–1485 (2005).
[Crossref]

2004 (2)

V. Shcheslavskiy, G. I. Petrov, S. Saltiel, and V. V. Yakovlev, “Quantitative characterization of aqueous solutions probed by the third-harmonic generation microscopy,” J. Struct. Biol. 147, 42–49 (2004).
[Crossref] [PubMed]

D. Débarre, W. Supatto, E. Farge, B. Moulia, M-C. Schanne-Klein, and E. Beaurepaire, “Velocimetric third-harmonic generation microscopy: micrometer-scale quantification of morphogenetic movements in unstained embryos,” Opt. Lett. 29, 2881–2883 (2004).
[Crossref]

2003 (3)

2002 (3)

2001 (1)

2000 (1)

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

1999 (3)

1998 (2)

M. Müller, J. Squier, K. R. Wilson, and G. J. Brakenhoff, “3D Microscopy of transparent objects using third-harmonic generation,” J. Microsc. 191, 266–274 (1998).
[Crossref] [PubMed]

J. A. Squier, M. Müller, G. J. Brakenhoff, and K. R. Wilson, “Third Harmonic Generation Microscopy,” Opt. Express 3, 315–324 (1998).
[Crossref] [PubMed]

1997 (1)

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear Scanning Laser Microscopy by Third Harmonic Generation,” Appl. Phys. Lett. 70, 922–924 (1997).
[Crossref]

1993 (1)

S. Hell, G. Reiner, C. Cremer, and E.H.K. Stelzer, “Aberrations in confocal fluorescence microscopy induced by mismatches in refractive index,” J. Microsc. 169, 391–405 (1993).
[Crossref]

1991 (1)

C. J. R. Sheppard and C.J. Cogswell., “Effects of aberrating layers and tube length on confocal imaging properties,” Optik 87, 34–38 (1991).

1985 (1)

F. Kajzar and J. Messier, “Third-harmonic generation in liquids,” Phys. Rev. A 32, 2352–2363 (1985).
[Crossref] [PubMed]

1983 (1)

G. R. Meredith, B. Buchalter, and C. Hanzlik, “Third-order susceptibility determination by third harmonic generation. II,” J. Chem. Phys. 78, 1543–1551 (1983).
[Crossref]

1969 (1)

J. F. Ward and G. H. C. New, “Optical Third Harmonic Generation in Gases by a Focused Laser Beam,” Phys. Rev. 185, 57–72 (1969).
[Crossref]

Barad, Y.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, “Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy,” Appl. Phys. Lett. 74, 3107–3109 (1999).
[Crossref]

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear Scanning Laser Microscopy by Third Harmonic Generation,” Appl. Phys. Lett. 70, 922–924 (1997).
[Crossref]

Barille, R.

R. Barille, L. Canioni, L. Sarger, and G. Rivoire, “Nonlinearity measurements of thin films by third-harmonic-generation microscopy,” Phys. Rev. E 66 (2002).
[Crossref]

L. Canioni, S. Rivet, L. Sarger, R. Barille, P. Vacher, and P. Voisin, “Imaging of Ca2+ intracellular dynamics with a third-harmonic generation microscope,” Opt. Lett. 26, 515–517 (2001).
[Crossref]

Beaurepaire, E.

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

D. Débarre, W. Supatto, E. Farge, B. Moulia, M-C. Schanne-Klein, and E. Beaurepaire, “Velocimetric third-harmonic generation microscopy: micrometer-scale quantification of morphogenetic movements in unstained embryos,” Opt. Lett. 29, 2881–2883 (2004).
[Crossref]

Born, M.

M. Born and E. Wolf, Principles of Optics (Pergamon Press, Oxford, 1993).

Boyd, R. W.

R. W. Boyd, Nonlinear Optics (Academic Press, Inc., New York, 1992).

Brakenhoff, G. J.

Brouzés, E.

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

Buchalter, B.

G. R. Meredith, B. Buchalter, and C. Hanzlik, “Third-order susceptibility determination by third harmonic generation. II,” J. Chem. Phys. 78, 1543–1551 (1983).
[Crossref]

Canioni, L.

R. Barille, L. Canioni, L. Sarger, and G. Rivoire, “Nonlinearity measurements of thin films by third-harmonic-generation microscopy,” Phys. Rev. E 66 (2002).
[Crossref]

L. Canioni, S. Rivet, L. Sarger, R. Barille, P. Vacher, and P. Voisin, “Imaging of Ca2+ intracellular dynamics with a third-harmonic generation microscope,” Opt. Lett. 26, 515–517 (2001).
[Crossref]

Chen, Szu-Yu

Cheng, J. X.

Chu, S.-W.

S.-W. Chu, Szu-Yu Chen, Tsung-Han Tsai, Tzu-Ming Liu, Cheng-Yung Lin, Huai-Jen Tsai, and Chi-Kuang Sun, “In vivo developmental biology study using noninvasive multi-harmonic generation microscopy,” Opt. Express 11, 3093 – 3099 (2003).
[Crossref] [PubMed]

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

Cogswell, C.J.

C. J. R. Sheppard and C.J. Cogswell., “Effects of aberrating layers and tube length on confocal imaging properties,” Optik 87, 34–38 (1991).

Cremer, C.

S. Hell, G. Reiner, C. Cremer, and E.H.K. Stelzer, “Aberrations in confocal fluorescence microscopy induced by mismatches in refractive index,” J. Microsc. 169, 391–405 (1993).
[Crossref]

Débarre, D.

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

D. Débarre, W. Supatto, E. Farge, B. Moulia, M-C. Schanne-Klein, and E. Beaurepaire, “Velocimetric third-harmonic generation microscopy: micrometer-scale quantification of morphogenetic movements in unstained embryos,” Opt. Lett. 29, 2881–2883 (2004).
[Crossref]

DenBaars, S.P.

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

Eisenberg, H.

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear Scanning Laser Microscopy by Third Harmonic Generation,” Appl. Phys. Lett. 70, 922–924 (1997).
[Crossref]

Farge, E.

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

D. Débarre, W. Supatto, E. Farge, B. Moulia, M-C. Schanne-Klein, and E. Beaurepaire, “Velocimetric third-harmonic generation microscopy: micrometer-scale quantification of morphogenetic movements in unstained embryos,” Opt. Lett. 29, 2881–2883 (2004).
[Crossref]

Hanzlik, C.

G. R. Meredith, B. Buchalter, and C. Hanzlik, “Third-order susceptibility determination by third harmonic generation. II,” J. Chem. Phys. 78, 1543–1551 (1983).
[Crossref]

Hell, S.

S. Hell, G. Reiner, C. Cremer, and E.H.K. Stelzer, “Aberrations in confocal fluorescence microscopy induced by mismatches in refractive index,” J. Microsc. 169, 391–405 (1993).
[Crossref]

Horowitz, M.

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear Scanning Laser Microscopy by Third Harmonic Generation,” Appl. Phys. Lett. 70, 922–924 (1997).
[Crossref]

Kajzar, F.

F. Kajzar and J. Messier, “Third-harmonic generation in liquids,” Phys. Rev. A 32, 2352–2363 (1985).
[Crossref] [PubMed]

Keller, S.

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

Kozma, I. Z.

Krok, P.

Lin, Cheng-Yung

Liu, Tzu-Ming

Martin, J-L.

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

Meredith, G. R.

G. R. Meredith, B. Buchalter, and C. Hanzlik, “Third-order susceptibility determination by third harmonic generation. II,” J. Chem. Phys. 78, 1543–1551 (1983).
[Crossref]

Messier, J.

F. Kajzar and J. Messier, “Third-harmonic generation in liquids,” Phys. Rev. A 32, 2352–2363 (1985).
[Crossref] [PubMed]

Mishra, U.K.

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

Moulia, B.

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

D. Débarre, W. Supatto, E. Farge, B. Moulia, M-C. Schanne-Klein, and E. Beaurepaire, “Velocimetric third-harmonic generation microscopy: micrometer-scale quantification of morphogenetic movements in unstained embryos,” Opt. Lett. 29, 2881–2883 (2004).
[Crossref]

Müller, M.

New, G. H. C.

J. F. Ward and G. H. C. New, “Optical Third Harmonic Generation in Gases by a Focused Laser Beam,” Phys. Rev. 185, 57–72 (1969).
[Crossref]

Oron, D.

Patel, J. S.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, “Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy,” Appl. Phys. Lett. 74, 3107–3109 (1999).
[Crossref]

Petrov, G.

V. Shcheslavskiy, G. Petrov, and V. V. Yakovlev, “Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface,” Appl. Phys. Lett. 82, 3982–3984 (2003).
[Crossref]

Petrov, G. I.

V. Shcheslavskiy, G. I. Petrov, S. Saltiel, and V. V. Yakovlev, “Quantitative characterization of aqueous solutions probed by the third-harmonic generation microscopy,” J. Struct. Biol. 147, 42–49 (2004).
[Crossref] [PubMed]

Reiner, G.

S. Hell, G. Reiner, C. Cremer, and E.H.K. Stelzer, “Aberrations in confocal fluorescence microscopy induced by mismatches in refractive index,” J. Microsc. 169, 391–405 (1993).
[Crossref]

Reintjes, J. F.

J. F. Reintjes, Nonlinear Optical Parametric Processes in Liquids and Gases (Academic Press, Inc., Orlando, 1984).

Riedle, E.

Rivet, S.

Rivoire, G.

R. Barille, L. Canioni, L. Sarger, and G. Rivoire, “Nonlinearity measurements of thin films by third-harmonic-generation microscopy,” Phys. Rev. E 66 (2002).
[Crossref]

Saltiel, S.

V. Shcheslavskiy, G. I. Petrov, S. Saltiel, and V. V. Yakovlev, “Quantitative characterization of aqueous solutions probed by the third-harmonic generation microscopy,” J. Struct. Biol. 147, 42–49 (2004).
[Crossref] [PubMed]

Sarger, L.

R. Barille, L. Canioni, L. Sarger, and G. Rivoire, “Nonlinearity measurements of thin films by third-harmonic-generation microscopy,” Phys. Rev. E 66 (2002).
[Crossref]

L. Canioni, S. Rivet, L. Sarger, R. Barille, P. Vacher, and P. Voisin, “Imaging of Ca2+ intracellular dynamics with a third-harmonic generation microscope,” Opt. Lett. 26, 515–517 (2001).
[Crossref]

Schanne-Klein, M-C.

Schins, J. M.

Schrama, T.

Shcheslavskiy, V.

V. Shcheslavskiy, G. I. Petrov, S. Saltiel, and V. V. Yakovlev, “Quantitative characterization of aqueous solutions probed by the third-harmonic generation microscopy,” J. Struct. Biol. 147, 42–49 (2004).
[Crossref] [PubMed]

V. Shcheslavskiy, G. Petrov, and V. V. Yakovlev, “Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface,” Appl. Phys. Lett. 82, 3982–3984 (2003).
[Crossref]

Sheppard, C. J. R.

C. J. R. Sheppard and C.J. Cogswell., “Effects of aberrating layers and tube length on confocal imaging properties,” Optik 87, 34–38 (1991).

Silberberg, Y.

D. Oron, E. Tal, and Y. Silberberg, “Depth-resolved multiphoton polarisation microscopy by third-harmonic generation,” Opt. Lett. 28, 2315–2317 (2003).
[Crossref] [PubMed]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, “Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy,” Appl. Phys. Lett. 74, 3107–3109 (1999).
[Crossref]

D. Yelin and Y. Silberberg, “Laser scanning third-harmonic-generation microscopy in biology,” Opt. Express 5, 169 – 175 (1999).
[Crossref] [PubMed]

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear Scanning Laser Microscopy by Third Harmonic Generation,” Appl. Phys. Lett. 70, 922–924 (1997).
[Crossref]

Squier, J.

J. M. Schins, T. Schrama, J. Squier, G. J. Brakenhoff, and M. Müller, “Determination of material properties by use of third-harmonic generation microscopy,” J. Opt. Soc. Am. B 19, 1627–1634 (2002).
[Crossref]

M. Müller, J. Squier, K. R. Wilson, and G. J. Brakenhoff, “3D Microscopy of transparent objects using third-harmonic generation,” J. Microsc. 191, 266–274 (1998).
[Crossref] [PubMed]

Squier, J. A.

Stelzer, E.H.K.

S. Hell, G. Reiner, C. Cremer, and E.H.K. Stelzer, “Aberrations in confocal fluorescence microscopy induced by mismatches in refractive index,” J. Microsc. 169, 391–405 (1993).
[Crossref]

Sun, C.-K.

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

Sun, Chi-Kuang

Supatto, W.

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

D. Débarre, W. Supatto, E. Farge, B. Moulia, M-C. Schanne-Klein, and E. Beaurepaire, “Velocimetric third-harmonic generation microscopy: micrometer-scale quantification of morphogenetic movements in unstained embryos,” Opt. Lett. 29, 2881–2883 (2004).
[Crossref]

Tai, S.-P.

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

Tal, E.

Tsai, Huai-Jen

Tsai, Tsung-Han

Vacher, P.

Voisin, P.

Ward, J. F.

J. F. Ward and G. H. C. New, “Optical Third Harmonic Generation in Gases by a Focused Laser Beam,” Phys. Rev. 185, 57–72 (1969).
[Crossref]

Wilson, K. R.

M. Müller, J. Squier, K. R. Wilson, and G. J. Brakenhoff, “3D Microscopy of transparent objects using third-harmonic generation,” J. Microsc. 191, 266–274 (1998).
[Crossref] [PubMed]

J. A. Squier, M. Müller, G. J. Brakenhoff, and K. R. Wilson, “Third Harmonic Generation Microscopy,” Opt. Express 3, 315–324 (1998).
[Crossref] [PubMed]

Wolf, E.

M. Born and E. Wolf, Principles of Optics (Pergamon Press, Oxford, 1993).

Xie, X. S.

Yakovlev, V. V.

V. Shcheslavskiy, G. I. Petrov, S. Saltiel, and V. V. Yakovlev, “Quantitative characterization of aqueous solutions probed by the third-harmonic generation microscopy,” J. Struct. Biol. 147, 42–49 (2004).
[Crossref] [PubMed]

V. Shcheslavskiy, G. Petrov, and V. V. Yakovlev, “Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface,” Appl. Phys. Lett. 82, 3982–3984 (2003).
[Crossref]

Yelin, D.

D. Yelin and Y. Silberberg, “Laser scanning third-harmonic-generation microscopy in biology,” Opt. Express 5, 169 – 175 (1999).
[Crossref] [PubMed]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, “Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy,” Appl. Phys. Lett. 74, 3107–3109 (1999).
[Crossref]

Appl. Opt. (1)

Appl. Phys. Lett. (4)

C.-K. Sun, S.-W. Chu, S.-P. Tai, S. Keller, U.K. Mishra, and S.P. DenBaars, “Scanning second-harmonic/third-harmonic generation microscopy of gallium nitride,” Appl. Phys. Lett. 77, 2331–2333 (2000).
[Crossref]

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear Scanning Laser Microscopy by Third Harmonic Generation,” Appl. Phys. Lett. 70, 922–924 (1997).
[Crossref]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, “Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy,” Appl. Phys. Lett. 74, 3107–3109 (1999).
[Crossref]

V. Shcheslavskiy, G. Petrov, and V. V. Yakovlev, “Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface,” Appl. Phys. Lett. 82, 3982–3984 (2003).
[Crossref]

J. Chem. Phys. (1)

G. R. Meredith, B. Buchalter, and C. Hanzlik, “Third-order susceptibility determination by third harmonic generation. II,” J. Chem. Phys. 78, 1543–1551 (1983).
[Crossref]

J. Microsc. (2)

S. Hell, G. Reiner, C. Cremer, and E.H.K. Stelzer, “Aberrations in confocal fluorescence microscopy induced by mismatches in refractive index,” J. Microsc. 169, 391–405 (1993).
[Crossref]

M. Müller, J. Squier, K. R. Wilson, and G. J. Brakenhoff, “3D Microscopy of transparent objects using third-harmonic generation,” J. Microsc. 191, 266–274 (1998).
[Crossref] [PubMed]

J. Opt. Soc. Am. B (3)

J. Struct. Biol. (1)

V. Shcheslavskiy, G. I. Petrov, S. Saltiel, and V. V. Yakovlev, “Quantitative characterization of aqueous solutions probed by the third-harmonic generation microscopy,” J. Struct. Biol. 147, 42–49 (2004).
[Crossref] [PubMed]

Opt. Express (3)

Opt. Lett. (3)

Optik (1)

C. J. R. Sheppard and C.J. Cogswell., “Effects of aberrating layers and tube length on confocal imaging properties,” Optik 87, 34–38 (1991).

Phys. Rev. (1)

J. F. Ward and G. H. C. New, “Optical Third Harmonic Generation in Gases by a Focused Laser Beam,” Phys. Rev. 185, 57–72 (1969).
[Crossref]

Phys. Rev. A (1)

F. Kajzar and J. Messier, “Third-harmonic generation in liquids,” Phys. Rev. A 32, 2352–2363 (1985).
[Crossref] [PubMed]

Phys. Rev. E (1)

R. Barille, L. Canioni, L. Sarger, and G. Rivoire, “Nonlinearity measurements of thin films by third-harmonic-generation microscopy,” Phys. Rev. E 66 (2002).
[Crossref]

PNAS (1)

W. Supatto, D. Débarre, B. Moulia, E. Brouzés, J-L. Martin, E. Farge, and E. Beaurepaire, “In vivo modulation of morphogenetic movements in Drosophila emryos with femtosecond laser pulses,” PNAS 102, 1047–1052 (2005).
[Crossref] [PubMed]

Other (3)

R. W. Boyd, Nonlinear Optics (Academic Press, Inc., New York, 1992).

M. Born and E. Wolf, Principles of Optics (Pergamon Press, Oxford, 1993).

J. F. Reintjes, Nonlinear Optical Parametric Processes in Liquids and Gases (Academic Press, Inc., Orlando, 1984).

Cited By

OSA participates in Crossref's Cited-By Linking service. Citing articles from OSA journals and other participating publishers are listed here.

Alert me when this article is cited.


Figures (5)

Fig. 1.
Fig. 1.

Experimental configuration for (a) quantitative χ(3) measurements and (b) evaluation of the THG signal depth dependence in a refractive index mismatched sample. Regions AB and CD are cover glasses, region BC contains the sample of interest. (c) Schematic of the experimental set-up for the THG measurements. Symbols used: Ln: lens; v.a.: variable aperture; S: sample; O: microscope objective; C: collection lens; F: filter. L4 can be translated along the optical axis, as can the microscope objective (O), which is mounted on a piezo scanner.

Fig. 2.
Fig. 2.

FWHM of the THG z-response as a function of the L4 position. Error bars represent one standard deviation of error and the solid line is a guide to the eye. Representative z-responses -open circles and corresponding fits to the left- and right-hand side (red and blue curves respectively) - are shown for L4 = 11.5, 14 and 16.5.

Fig. 3.
Fig. 3.

(a) Measured ratio IB/IA as a function of NA for G1 (triangles), G2 (circles) and G3 (squares) in a air-glass-air configuration. The solid line represents a numerical calculation for G2. (b) Measured (open symbols) and calculated (solid line) THG z-responses at interfaces A (red) and B (blue) for G2. The measurement error is approximately ±2%.

Fig. 4.
Fig. 4.

Measured χ(3) values for methanol, ethanol and 2-propanol. Red and light blue bars represent direct evaluation of χ(3) based on IB/IA measurements with NA = 0.35 and NA = 0.65 respectively. Dark blue bars represent χ(3) value obtained from the NA = 0.65 measurement after correcting for the effect of aberration. Violet bars denote literature χ(3) values obtained at 1062 nm for methanol and ethanol and at 1910 nm for 2-propanol [24, 26]

Fig. 5.
Fig. 5.

Measured ratio IC/IB as a function of depth in a refractive index mismatched medium (water) for two different microscope objectives: 0.65 NA/40x air-spaced (blue circles) and 1.25 NA/63x oil immersion. Solid lines represent theoretical calculations for NA = 0.65 (blue) with a uniform profile and NA = 1.25 (red) with a Gaussian profile. All measurements and calculations are for G2 glass.

Tables (1)

Tables Icon

Table 1. Properties of glass types used.

Equations (4)

Equations on this page are rendered with MathJax. Learn more.

ϕ = kt [ n 2 ( 1 4 n 1 2 s 2 ( 1 s 2 ) n 2 2 ) 1 2 n 1 ( 1 2 s 2 ) ]
ϕ = k ( t 170 ) [ n 2 ( 1 4 n 1 2 s 2 ( 1 s 2 ) n 2 2 ) 1 2 n 1 ( 1 2 s 2 ) ]
χ mat ( 3 ) = χ glass ( 3 ) J glass ( 1 ± I B I A ) J mat
J = 0 exp ( i Δ kz ) ( 1 + 2 iz b ) 2 dz

Metrics