Abstract

Third harmonic generation microscopy is described in the frame work of the theory of harmonic generation with Gaussian focused beams inside a bulk material as well as at the vicinity of an interface. This model is then applied to characterize different types of materials in terms of electronic third-order susceptibility. Examples of bulk glasses, poled glasses, laser-induced modifications in glasses and nanoparticles in solution are given in order to give a survey of the broad application field of THG microscopy in material characterization.

© 2006 Optical Society of Korea

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  1. P. S. Banks, M. D. Feit, and M. D. Perry, "High intensity direct third harmonic generation in BBO," in Nonlinear Optics "98: Materials, Fundamentals, and Applications Topical Meeting, Kauai, USA, 1998, pp. 268-270
    [CrossRef]
  2. D. Taverner, P. Britton, P. G. R. Smith, D. J. Richardson, G. W. Ross, and D. C. Hanna, "Highly efficient second-harmonic and sum-frequency generation of nanosecond pulses in a cascading erbium-doped fiber: periodically poled lithium niobate source," Optics Letters, vol. 23, pp. 162-164 (1998)
    [CrossRef]
  3. B. Buchalter and G. R. Meredith, "Third-order optical susceptibility of glasses determined by third harmonic generation," Applied Optics, vol. 21, pp. 3221-3224 (1982)
    [CrossRef]
  4. H. Nasu, K. Kubodera, M. Kobayashi, M. Nakamura, and K. Kamiya, "Third-Harmonic Generation from Some Chalcogenide Glasses," Journal of the American Ceramic Society, vol. 73, pp. 1794-1796 (1990)
    [CrossRef]
  5. S. H. Kim, T. Yoko, and S. Sakka, "Nonlinear Optical Properties of <TEX>$TeO_2$</TEX>-Based Glasses: <TEX>${La}_2O_3-TeO_2$</TEX> Binary Glasses," Journal of the American Ceramic Society, vol. 76, pp. 865-869 (1992)
    [CrossRef]
  6. U. Gubler and C. Bosshard, "Optical third-harmonic generation of fused silica in gas atmosphere: Absolute value of the third-order nonlinear susceptibility <TEX>$x^{(3)}$</TEX>," Physical Review B, vol. 61, pp. 702-710 (2000)
    [CrossRef]
  7. T. Y. F. Tsang, "Optical third harmonic generation at interfaces," Physical Review A, vol. 52, pp. 4116-4126 (1995)
    [CrossRef]
  8. Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, "Nonlinear scanning laser microscopy by third harmonic generation," Applied Physics Letters, vol. 70, pp. 922-924 (1997)
    [CrossRef]
  9. L. Canioni, S. Rivet, L. Sarger, R. Barille, P. Vacher, and P. Voisin, "Imaging of <TEX>$Ca^{2+}$</TEX> intracellular dynamics with a third-harmonic generation microscope," Optics Letters, vol. 26, pp. 515-517 (2001)
    [CrossRef]
  10. D. Yelin and Y. Silberberg, "Laser scanning third-harmonic-generation-microscopy in biology," Optics Express, vol. 5, pp. 169-175 (1999)
    [CrossRef]
  11. J. A. Squier, M. Muller, G. J. Brakenhoff, and K. R. Wilson, "Third harmonic generation microscopy," Optics Express, vol. 3, pp. 315-324 (1998)
    [CrossRef]
  12. D. Debarre, W. Supatto, A. M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M. C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cell and tissues using third-harmonic generation microscopy," Nature Methods, vol. 3, pp. 47-53 (2006)
    [CrossRef]
  13. R. Barille, L. Canioni, L. Sarger, and G. Rivoire, "Nonlinearity measurements of thin films by third-harmonic-generation microscopy," Physical Review E, vol. 66, pp. 067602-067605 (2002)
    [CrossRef]
  14. J. M. Schins, T. Schrama, J. Squier, G. J. Brakenhoff, and M. Muller, "Determination of materials properties by use of third-harmonic generation microscopy," Journal of Optical Society of America B, vol. 19, pp. 1627-1634 (2002)
    [CrossRef]
  15. V. Shcheslavskiy, G. Petrov. and V. V. Yakovlev, "Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface," Applied Physics Letters, vol. 82, pp. 3982-3984 (2003)
    [CrossRef]
  16. P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics (Cambridge University Press, Cambridge, UK, 1990), p. 225 and appendix 10
  17. R. W. Boyd, Nonlinear Optics (Academic Press, New York, USA, 2003), pp. 90-99
  18. A. Brocas, Microscopies non-lin<TEX>$\"{e}$</TEX>aires: Analyses et Instrumentations (Thesis, University of Bordeaux 1, France, 2005)
  19. D. Oron, E. Tal, and Y. Silberberg, "Depth-resolved multiphoton polarization microscopy by third-harmonic generation," Optics Letters, vol. 28, pp. 2315-2317 (2003)
    [CrossRef]
  20. D. Oron, D. Yelin, E. Tal, S. Raz, R. Fachima, and Y. Silberberg, "Depth-resolved structural imaging by third-harmonic generation microscopy," Journal of Structural Biology, vol. 147, pp. 3-11 (2004)
    [CrossRef]
  21. T. Cardinal, E. Fargin, G. Le Flem, M. Couzi, L. Canioni, P. Segonds, L. Sarger, A. Ducasse, and F. Adamietz, "Nonlinear optical properties of some niobium (V) oxide glasses," European Journal of Solid State and Inorganic Chemistry, vol. 33, pp. 597-605 (1996)
  22. T. Cardinal, E. Fargin, G. Le Flem, and S. Leboiteux, "Correlations between structural properties of <TEX>$Nb_2O_5$</TEX>-<TEX>$NaPO_3$</TEX>-<TEX>${Na}_2B_4O_7$</TEX> glasses and non-linear optical activities," Journal of Non-Crystalline Solids, vol. 222, pp. 228-234 (1997)
    [CrossRef]
  23. A. Malakho, M. Dussauze, E. Fargin, B. Lazoryak, V. Rodriguez, and F. Adamietz, "Crystallization and second harmonic generation in thermally poled niobium borophosphate glasses," Journal of Solid State Chemistry, vol. 178, pp. 1888-1897 (2005)
    [CrossRef]
  24. A. Zoubir, M. Richardson, L. Canioni, A. Brocas, and L. Sarger, "Optical properties of infrared femtosecond laser-modified fused silica and application to waveguide fabrication", Journal of Optical Society of America B, vol. 22, pp. 2138-2143 (2005)
    [CrossRef]
  25. D. Blomer, A. Szameit, F. Dreisow, T. Schreiber, S. Nolte, and A. Tunnermann, "Nonlinear refractive-index of fs-laser-written waveguides in fused silica," Optics Express, vol. 14, pp. 2151-2157 (2006)
    [CrossRef]
  26. F. Rocco, A. K. Jain, M. Treguer, T. Cardinal, S. Yotte, P. Le Coustumer, C. Y. Lee, S. H. Park, and J. G. Ghoi, "Optical response of silver coatings on CdS colloids," Chemical Physics Letters, vol. 394, pp. 324-328 (2004)
    [CrossRef]
  27. N. Kalyaniwalla, J. W. Haus, R. Inguva, and M. H. Birnboim, "Intrinsic optical bistability for coated spheroidal particles," Physical Review A, vol. 42, pp. 5613-5621 (1990)
    [CrossRef]

2006 (2)

D. Debarre, W. Supatto, A. M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M. C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cell and tissues using third-harmonic generation microscopy," Nature Methods, vol. 3, pp. 47-53 (2006)
[CrossRef]

D. Blomer, A. Szameit, F. Dreisow, T. Schreiber, S. Nolte, and A. Tunnermann, "Nonlinear refractive-index of fs-laser-written waveguides in fused silica," Optics Express, vol. 14, pp. 2151-2157 (2006)
[CrossRef]

2005 (3)

A. Malakho, M. Dussauze, E. Fargin, B. Lazoryak, V. Rodriguez, and F. Adamietz, "Crystallization and second harmonic generation in thermally poled niobium borophosphate glasses," Journal of Solid State Chemistry, vol. 178, pp. 1888-1897 (2005)
[CrossRef]

A. Zoubir, M. Richardson, L. Canioni, A. Brocas, and L. Sarger, "Optical properties of infrared femtosecond laser-modified fused silica and application to waveguide fabrication", Journal of Optical Society of America B, vol. 22, pp. 2138-2143 (2005)
[CrossRef]

A. Brocas, Microscopies non-lin<TEX>$\"{e}$</TEX>aires: Analyses et Instrumentations (Thesis, University of Bordeaux 1, France, 2005)

2004 (2)

D. Oron, D. Yelin, E. Tal, S. Raz, R. Fachima, and Y. Silberberg, "Depth-resolved structural imaging by third-harmonic generation microscopy," Journal of Structural Biology, vol. 147, pp. 3-11 (2004)
[CrossRef]

F. Rocco, A. K. Jain, M. Treguer, T. Cardinal, S. Yotte, P. Le Coustumer, C. Y. Lee, S. H. Park, and J. G. Ghoi, "Optical response of silver coatings on CdS colloids," Chemical Physics Letters, vol. 394, pp. 324-328 (2004)
[CrossRef]

2003 (3)

D. Oron, E. Tal, and Y. Silberberg, "Depth-resolved multiphoton polarization microscopy by third-harmonic generation," Optics Letters, vol. 28, pp. 2315-2317 (2003)
[CrossRef]

R. W. Boyd, Nonlinear Optics (Academic Press, New York, USA, 2003), pp. 90-99

V. Shcheslavskiy, G. Petrov. and V. V. Yakovlev, "Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface," Applied Physics Letters, vol. 82, pp. 3982-3984 (2003)
[CrossRef]

2002 (2)

R. Barille, L. Canioni, L. Sarger, and G. Rivoire, "Nonlinearity measurements of thin films by third-harmonic-generation microscopy," Physical Review E, vol. 66, pp. 067602-067605 (2002)
[CrossRef]

J. M. Schins, T. Schrama, J. Squier, G. J. Brakenhoff, and M. Muller, "Determination of materials properties by use of third-harmonic generation microscopy," Journal of Optical Society of America B, vol. 19, pp. 1627-1634 (2002)
[CrossRef]

2001 (1)

L. Canioni, S. Rivet, L. Sarger, R. Barille, P. Vacher, and P. Voisin, "Imaging of <TEX>$Ca^{2+}$</TEX> intracellular dynamics with a third-harmonic generation microscope," Optics Letters, vol. 26, pp. 515-517 (2001)
[CrossRef]

2000 (1)

U. Gubler and C. Bosshard, "Optical third-harmonic generation of fused silica in gas atmosphere: Absolute value of the third-order nonlinear susceptibility <TEX>$x^{(3)}$</TEX>," Physical Review B, vol. 61, pp. 702-710 (2000)
[CrossRef]

1999 (1)

D. Yelin and Y. Silberberg, "Laser scanning third-harmonic-generation-microscopy in biology," Optics Express, vol. 5, pp. 169-175 (1999)
[CrossRef]

1998 (3)

J. A. Squier, M. Muller, G. J. Brakenhoff, and K. R. Wilson, "Third harmonic generation microscopy," Optics Express, vol. 3, pp. 315-324 (1998)
[CrossRef]

P. S. Banks, M. D. Feit, and M. D. Perry, "High intensity direct third harmonic generation in BBO," in Nonlinear Optics "98: Materials, Fundamentals, and Applications Topical Meeting, Kauai, USA, 1998, pp. 268-270
[CrossRef]

D. Taverner, P. Britton, P. G. R. Smith, D. J. Richardson, G. W. Ross, and D. C. Hanna, "Highly efficient second-harmonic and sum-frequency generation of nanosecond pulses in a cascading erbium-doped fiber: periodically poled lithium niobate source," Optics Letters, vol. 23, pp. 162-164 (1998)
[CrossRef]

1997 (2)

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, "Nonlinear scanning laser microscopy by third harmonic generation," Applied Physics Letters, vol. 70, pp. 922-924 (1997)
[CrossRef]

T. Cardinal, E. Fargin, G. Le Flem, and S. Leboiteux, "Correlations between structural properties of <TEX>$Nb_2O_5$</TEX>-<TEX>$NaPO_3$</TEX>-<TEX>${Na}_2B_4O_7$</TEX> glasses and non-linear optical activities," Journal of Non-Crystalline Solids, vol. 222, pp. 228-234 (1997)
[CrossRef]

1996 (1)

T. Cardinal, E. Fargin, G. Le Flem, M. Couzi, L. Canioni, P. Segonds, L. Sarger, A. Ducasse, and F. Adamietz, "Nonlinear optical properties of some niobium (V) oxide glasses," European Journal of Solid State and Inorganic Chemistry, vol. 33, pp. 597-605 (1996)

1995 (1)

T. Y. F. Tsang, "Optical third harmonic generation at interfaces," Physical Review A, vol. 52, pp. 4116-4126 (1995)
[CrossRef]

1992 (1)

S. H. Kim, T. Yoko, and S. Sakka, "Nonlinear Optical Properties of <TEX>$TeO_2$</TEX>-Based Glasses: <TEX>${La}_2O_3-TeO_2$</TEX> Binary Glasses," Journal of the American Ceramic Society, vol. 76, pp. 865-869 (1992)
[CrossRef]

1990 (3)

H. Nasu, K. Kubodera, M. Kobayashi, M. Nakamura, and K. Kamiya, "Third-Harmonic Generation from Some Chalcogenide Glasses," Journal of the American Ceramic Society, vol. 73, pp. 1794-1796 (1990)
[CrossRef]

P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics (Cambridge University Press, Cambridge, UK, 1990), p. 225 and appendix 10

N. Kalyaniwalla, J. W. Haus, R. Inguva, and M. H. Birnboim, "Intrinsic optical bistability for coated spheroidal particles," Physical Review A, vol. 42, pp. 5613-5621 (1990)
[CrossRef]

1982 (1)

B. Buchalter and G. R. Meredith, "Third-order optical susceptibility of glasses determined by third harmonic generation," Applied Optics, vol. 21, pp. 3221-3224 (1982)
[CrossRef]

Applied Optics (1)

B. Buchalter and G. R. Meredith, "Third-order optical susceptibility of glasses determined by third harmonic generation," Applied Optics, vol. 21, pp. 3221-3224 (1982)
[CrossRef]

Applied Physics Letters (2)

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, "Nonlinear scanning laser microscopy by third harmonic generation," Applied Physics Letters, vol. 70, pp. 922-924 (1997)
[CrossRef]

V. Shcheslavskiy, G. Petrov. and V. V. Yakovlev, "Nonlinear optical susceptibility measurements of solutions using third-harmonic generation on the interface," Applied Physics Letters, vol. 82, pp. 3982-3984 (2003)
[CrossRef]

Chemical Physics Letters (1)

F. Rocco, A. K. Jain, M. Treguer, T. Cardinal, S. Yotte, P. Le Coustumer, C. Y. Lee, S. H. Park, and J. G. Ghoi, "Optical response of silver coatings on CdS colloids," Chemical Physics Letters, vol. 394, pp. 324-328 (2004)
[CrossRef]

European Journal of Solid State and Inorganic Chemistry (1)

T. Cardinal, E. Fargin, G. Le Flem, M. Couzi, L. Canioni, P. Segonds, L. Sarger, A. Ducasse, and F. Adamietz, "Nonlinear optical properties of some niobium (V) oxide glasses," European Journal of Solid State and Inorganic Chemistry, vol. 33, pp. 597-605 (1996)

Journal of Non-Crystalline Solids (1)

T. Cardinal, E. Fargin, G. Le Flem, and S. Leboiteux, "Correlations between structural properties of <TEX>$Nb_2O_5$</TEX>-<TEX>$NaPO_3$</TEX>-<TEX>${Na}_2B_4O_7$</TEX> glasses and non-linear optical activities," Journal of Non-Crystalline Solids, vol. 222, pp. 228-234 (1997)
[CrossRef]

Journal of Solid State Chemistry (1)

A. Malakho, M. Dussauze, E. Fargin, B. Lazoryak, V. Rodriguez, and F. Adamietz, "Crystallization and second harmonic generation in thermally poled niobium borophosphate glasses," Journal of Solid State Chemistry, vol. 178, pp. 1888-1897 (2005)
[CrossRef]

Journal of Structural Biology (1)

D. Oron, D. Yelin, E. Tal, S. Raz, R. Fachima, and Y. Silberberg, "Depth-resolved structural imaging by third-harmonic generation microscopy," Journal of Structural Biology, vol. 147, pp. 3-11 (2004)
[CrossRef]

Journal of the American Ceramic Society (2)

H. Nasu, K. Kubodera, M. Kobayashi, M. Nakamura, and K. Kamiya, "Third-Harmonic Generation from Some Chalcogenide Glasses," Journal of the American Ceramic Society, vol. 73, pp. 1794-1796 (1990)
[CrossRef]

S. H. Kim, T. Yoko, and S. Sakka, "Nonlinear Optical Properties of <TEX>$TeO_2$</TEX>-Based Glasses: <TEX>${La}_2O_3-TeO_2$</TEX> Binary Glasses," Journal of the American Ceramic Society, vol. 76, pp. 865-869 (1992)
[CrossRef]

Journal of the Optical Society of America B (2)

J. M. Schins, T. Schrama, J. Squier, G. J. Brakenhoff, and M. Muller, "Determination of materials properties by use of third-harmonic generation microscopy," Journal of Optical Society of America B, vol. 19, pp. 1627-1634 (2002)
[CrossRef]

A. Zoubir, M. Richardson, L. Canioni, A. Brocas, and L. Sarger, "Optical properties of infrared femtosecond laser-modified fused silica and application to waveguide fabrication", Journal of Optical Society of America B, vol. 22, pp. 2138-2143 (2005)
[CrossRef]

Nature Methods (1)

D. Debarre, W. Supatto, A. M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M. C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cell and tissues using third-harmonic generation microscopy," Nature Methods, vol. 3, pp. 47-53 (2006)
[CrossRef]

Nonlinear Optics '98: Materials, Fundamentals and Applications Topical Meeting (1)

P. S. Banks, M. D. Feit, and M. D. Perry, "High intensity direct third harmonic generation in BBO," in Nonlinear Optics "98: Materials, Fundamentals, and Applications Topical Meeting, Kauai, USA, 1998, pp. 268-270
[CrossRef]

Optics Express (3)

D. Yelin and Y. Silberberg, "Laser scanning third-harmonic-generation-microscopy in biology," Optics Express, vol. 5, pp. 169-175 (1999)
[CrossRef]

J. A. Squier, M. Muller, G. J. Brakenhoff, and K. R. Wilson, "Third harmonic generation microscopy," Optics Express, vol. 3, pp. 315-324 (1998)
[CrossRef]

D. Blomer, A. Szameit, F. Dreisow, T. Schreiber, S. Nolte, and A. Tunnermann, "Nonlinear refractive-index of fs-laser-written waveguides in fused silica," Optics Express, vol. 14, pp. 2151-2157 (2006)
[CrossRef]

Optics Letters (3)

D. Oron, E. Tal, and Y. Silberberg, "Depth-resolved multiphoton polarization microscopy by third-harmonic generation," Optics Letters, vol. 28, pp. 2315-2317 (2003)
[CrossRef]

D. Taverner, P. Britton, P. G. R. Smith, D. J. Richardson, G. W. Ross, and D. C. Hanna, "Highly efficient second-harmonic and sum-frequency generation of nanosecond pulses in a cascading erbium-doped fiber: periodically poled lithium niobate source," Optics Letters, vol. 23, pp. 162-164 (1998)
[CrossRef]

L. Canioni, S. Rivet, L. Sarger, R. Barille, P. Vacher, and P. Voisin, "Imaging of <TEX>$Ca^{2+}$</TEX> intracellular dynamics with a third-harmonic generation microscope," Optics Letters, vol. 26, pp. 515-517 (2001)
[CrossRef]

Physical Review A (2)

T. Y. F. Tsang, "Optical third harmonic generation at interfaces," Physical Review A, vol. 52, pp. 4116-4126 (1995)
[CrossRef]

N. Kalyaniwalla, J. W. Haus, R. Inguva, and M. H. Birnboim, "Intrinsic optical bistability for coated spheroidal particles," Physical Review A, vol. 42, pp. 5613-5621 (1990)
[CrossRef]

Physical Review B (1)

U. Gubler and C. Bosshard, "Optical third-harmonic generation of fused silica in gas atmosphere: Absolute value of the third-order nonlinear susceptibility <TEX>$x^{(3)}$</TEX>," Physical Review B, vol. 61, pp. 702-710 (2000)
[CrossRef]

Physical Review E (1)

R. Barille, L. Canioni, L. Sarger, and G. Rivoire, "Nonlinearity measurements of thin films by third-harmonic-generation microscopy," Physical Review E, vol. 66, pp. 067602-067605 (2002)
[CrossRef]

Other (3)

P. N. Butcher and D. Cotter, The Elements of Nonlinear Optics (Cambridge University Press, Cambridge, UK, 1990), p. 225 and appendix 10

R. W. Boyd, Nonlinear Optics (Academic Press, New York, USA, 2003), pp. 90-99

A. Brocas, Microscopies non-lin<TEX>$\"{e}$</TEX>aires: Analyses et Instrumentations (Thesis, University of Bordeaux 1, France, 2005)

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