Abstract

The generation of nonlinear optical functional crystals in borate, niobate, and titanate glasses that have been irradiated by 800-nm femtosecond laser pulses was investigated by Raman spectroscopy. The effects of the length of irradiation time on the generation of crystals were measured. We show that the structure of the glass network was destroyed during irradiation by the femtosecond laser. (B3O6)3-, (NbO6)7-, and (TiO4)4- anion units as well as β-BaB2O4, LiNbO3, and Ba2TiO4 crystals were formed in the focal area of the irradiation. We suggest that femtosecond laser irradiation can be a useful approach to the fabrication of integrated optical devices.

© 2004 Optical Society of America

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  1. K. O. Hill, Y. Fujii, D. C. Johnson, and B. S. Kawasaki, “Photosensitivity in optical fiber waveguides: application to reflection filter fabrication,” Appl. Phys. Lett. 32, 647–649 (1978).
    [CrossRef]
  2. O. Osterberg and W. Margulis, “Dye laser pumped by Nd:YAG laser pulses frequency doubled in a glass optical fiber,” Opt. Lett. 11, 516–518 (1986).
    [CrossRef] [PubMed]
  3. J. H. Strikler and W. W. Webb, “Three-dimensional optical data storage in refractive media by two-photon point excitation,” Opt. Lett. 16, 1780–1782 (1991).
    [CrossRef]
  4. K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
    [CrossRef]
  5. M. Will, S. Molte, and A. Tuennermann, “Three-dimensional integrated optical device fabrication in glass by femtosecond laser processing,” in Conference on Lasers and Electro-Optics (CLEO), Vol. 73 of OSA Trends in Optics and Photonics Series (Optical Society of America, Washington, D.C., 2000), pp. 127–128.
  6. W. L. Konijnendijk and J. M. Stevels, “Structure of borate glasses,” J. Non-Cryst. Solids 18, 307–331 (1975).
    [CrossRef]
  7. E. I. Kamitsos, M. A. Karakassides, and A. P. Patsis, “Spectroscopic study of carbonate retention in high-basicity borate glasses,” J. Non-Cryst. Solids 111, 252–259 (1989).
    [CrossRef]
  8. Y. Roussignè, R. Farhi, and C. Dugautier, and J. Gardard, “A Raman study of both phases of barium metaborate (BBO),” Solid State Commun. 82, 287–293 (1992).
    [CrossRef]
  9. B. K. Yu, T. Y. Yu, G. C. Jiang, and J. L. You, “Phase transition and frequency doubling of β-BaB2O4 and K3Li12−xNb12−xO15+x crystals,” in Optical Devices and Diagnostics in Materials Science, D. L. Andrews, T. Asakura, S. Jutamulia, W. P. Kirk, M. G. Lagally, R. B. Lal, and J. D. Trolinger, eds., Proc. SPIE 4098, 210–213 (2000).
    [CrossRef]
  10. K. Fukumi and S. Sakka, “Structure of alkali or alkaline earth niobium gallate glasses,” J. Non-Cryst. Solids 110, 61–68 (1989).
    [CrossRef]
  11. H. X. Gao, Z. C. Wang, and S. Z. Wang, “Properties and structure of niobosilicate glasses,” J. Non-Cryst. Solids 112, 332–335 (1989).
    [CrossRef]
  12. R. F. Schaufele and M. J. Weber, “Raman scattering by lithium niobate,” Phys. Rev. 152, 705–708 (1966).
    [CrossRef]
  13. J. Wang, K. Yang, and C. Jin, “A study on the structure of the crystal LiNbO3:MgO,” Acta Phys. Sin. 48, 1103–1106 (1999).
  14. K. Kamiya and S. Sakka, “Thermal expansion of TiO2-SiO2 and TiO2-GeO2 glasses,” J. Non-Cryst. Solids 52, 357–363 (1982).
    [CrossRef]
  15. X. L. Song, Y. X. Qu, C. Chao, and M. H. Jiang, “A laser Raman spectra study on the structure of titanium borasilicate glasses,” Chin. J. Light Scatt. 10, 30–36 (1998).

2000 (1)

B. K. Yu, T. Y. Yu, G. C. Jiang, and J. L. You, “Phase transition and frequency doubling of β-BaB2O4 and K3Li12−xNb12−xO15+x crystals,” in Optical Devices and Diagnostics in Materials Science, D. L. Andrews, T. Asakura, S. Jutamulia, W. P. Kirk, M. G. Lagally, R. B. Lal, and J. D. Trolinger, eds., Proc. SPIE 4098, 210–213 (2000).
[CrossRef]

1999 (1)

J. Wang, K. Yang, and C. Jin, “A study on the structure of the crystal LiNbO3:MgO,” Acta Phys. Sin. 48, 1103–1106 (1999).

1998 (1)

X. L. Song, Y. X. Qu, C. Chao, and M. H. Jiang, “A laser Raman spectra study on the structure of titanium borasilicate glasses,” Chin. J. Light Scatt. 10, 30–36 (1998).

1997 (1)

K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
[CrossRef]

1992 (1)

Y. Roussignè, R. Farhi, and C. Dugautier, and J. Gardard, “A Raman study of both phases of barium metaborate (BBO),” Solid State Commun. 82, 287–293 (1992).
[CrossRef]

1991 (1)

1989 (3)

E. I. Kamitsos, M. A. Karakassides, and A. P. Patsis, “Spectroscopic study of carbonate retention in high-basicity borate glasses,” J. Non-Cryst. Solids 111, 252–259 (1989).
[CrossRef]

K. Fukumi and S. Sakka, “Structure of alkali or alkaline earth niobium gallate glasses,” J. Non-Cryst. Solids 110, 61–68 (1989).
[CrossRef]

H. X. Gao, Z. C. Wang, and S. Z. Wang, “Properties and structure of niobosilicate glasses,” J. Non-Cryst. Solids 112, 332–335 (1989).
[CrossRef]

1986 (1)

1982 (1)

K. Kamiya and S. Sakka, “Thermal expansion of TiO2-SiO2 and TiO2-GeO2 glasses,” J. Non-Cryst. Solids 52, 357–363 (1982).
[CrossRef]

1978 (1)

K. O. Hill, Y. Fujii, D. C. Johnson, and B. S. Kawasaki, “Photosensitivity in optical fiber waveguides: application to reflection filter fabrication,” Appl. Phys. Lett. 32, 647–649 (1978).
[CrossRef]

1975 (1)

W. L. Konijnendijk and J. M. Stevels, “Structure of borate glasses,” J. Non-Cryst. Solids 18, 307–331 (1975).
[CrossRef]

1966 (1)

R. F. Schaufele and M. J. Weber, “Raman scattering by lithium niobate,” Phys. Rev. 152, 705–708 (1966).
[CrossRef]

Chao, C.

X. L. Song, Y. X. Qu, C. Chao, and M. H. Jiang, “A laser Raman spectra study on the structure of titanium borasilicate glasses,” Chin. J. Light Scatt. 10, 30–36 (1998).

Dugautier, C.

Y. Roussignè, R. Farhi, and C. Dugautier, and J. Gardard, “A Raman study of both phases of barium metaborate (BBO),” Solid State Commun. 82, 287–293 (1992).
[CrossRef]

Farhi, R.

Y. Roussignè, R. Farhi, and C. Dugautier, and J. Gardard, “A Raman study of both phases of barium metaborate (BBO),” Solid State Commun. 82, 287–293 (1992).
[CrossRef]

Fujii, Y.

K. O. Hill, Y. Fujii, D. C. Johnson, and B. S. Kawasaki, “Photosensitivity in optical fiber waveguides: application to reflection filter fabrication,” Appl. Phys. Lett. 32, 647–649 (1978).
[CrossRef]

Fukumi, K.

K. Fukumi and S. Sakka, “Structure of alkali or alkaline earth niobium gallate glasses,” J. Non-Cryst. Solids 110, 61–68 (1989).
[CrossRef]

Gao, H. X.

H. X. Gao, Z. C. Wang, and S. Z. Wang, “Properties and structure of niobosilicate glasses,” J. Non-Cryst. Solids 112, 332–335 (1989).
[CrossRef]

Gardard, J.

Y. Roussignè, R. Farhi, and C. Dugautier, and J. Gardard, “A Raman study of both phases of barium metaborate (BBO),” Solid State Commun. 82, 287–293 (1992).
[CrossRef]

Hill, K. O.

K. O. Hill, Y. Fujii, D. C. Johnson, and B. S. Kawasaki, “Photosensitivity in optical fiber waveguides: application to reflection filter fabrication,” Appl. Phys. Lett. 32, 647–649 (1978).
[CrossRef]

Hirao, K.

K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
[CrossRef]

Inouye, H.

K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
[CrossRef]

Jiang, G. C.

B. K. Yu, T. Y. Yu, G. C. Jiang, and J. L. You, “Phase transition and frequency doubling of β-BaB2O4 and K3Li12−xNb12−xO15+x crystals,” in Optical Devices and Diagnostics in Materials Science, D. L. Andrews, T. Asakura, S. Jutamulia, W. P. Kirk, M. G. Lagally, R. B. Lal, and J. D. Trolinger, eds., Proc. SPIE 4098, 210–213 (2000).
[CrossRef]

Jiang, M. H.

X. L. Song, Y. X. Qu, C. Chao, and M. H. Jiang, “A laser Raman spectra study on the structure of titanium borasilicate glasses,” Chin. J. Light Scatt. 10, 30–36 (1998).

Jin, C.

J. Wang, K. Yang, and C. Jin, “A study on the structure of the crystal LiNbO3:MgO,” Acta Phys. Sin. 48, 1103–1106 (1999).

Johnson, D. C.

K. O. Hill, Y. Fujii, D. C. Johnson, and B. S. Kawasaki, “Photosensitivity in optical fiber waveguides: application to reflection filter fabrication,” Appl. Phys. Lett. 32, 647–649 (1978).
[CrossRef]

Kamitsos, E. I.

E. I. Kamitsos, M. A. Karakassides, and A. P. Patsis, “Spectroscopic study of carbonate retention in high-basicity borate glasses,” J. Non-Cryst. Solids 111, 252–259 (1989).
[CrossRef]

Kamiya, K.

K. Kamiya and S. Sakka, “Thermal expansion of TiO2-SiO2 and TiO2-GeO2 glasses,” J. Non-Cryst. Solids 52, 357–363 (1982).
[CrossRef]

Karakassides, M. A.

E. I. Kamitsos, M. A. Karakassides, and A. P. Patsis, “Spectroscopic study of carbonate retention in high-basicity borate glasses,” J. Non-Cryst. Solids 111, 252–259 (1989).
[CrossRef]

Kawasaki, B. S.

K. O. Hill, Y. Fujii, D. C. Johnson, and B. S. Kawasaki, “Photosensitivity in optical fiber waveguides: application to reflection filter fabrication,” Appl. Phys. Lett. 32, 647–649 (1978).
[CrossRef]

Konijnendijk, W. L.

W. L. Konijnendijk and J. M. Stevels, “Structure of borate glasses,” J. Non-Cryst. Solids 18, 307–331 (1975).
[CrossRef]

Margulis, W.

Mitsuyu, T.

K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
[CrossRef]

Miura, K.

K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
[CrossRef]

Osterberg, O.

Patsis, A. P.

E. I. Kamitsos, M. A. Karakassides, and A. P. Patsis, “Spectroscopic study of carbonate retention in high-basicity borate glasses,” J. Non-Cryst. Solids 111, 252–259 (1989).
[CrossRef]

Qiu, J.

K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
[CrossRef]

Qu, Y. X.

X. L. Song, Y. X. Qu, C. Chao, and M. H. Jiang, “A laser Raman spectra study on the structure of titanium borasilicate glasses,” Chin. J. Light Scatt. 10, 30–36 (1998).

Roussignè, Y.

Y. Roussignè, R. Farhi, and C. Dugautier, and J. Gardard, “A Raman study of both phases of barium metaborate (BBO),” Solid State Commun. 82, 287–293 (1992).
[CrossRef]

Sakka, S.

K. Fukumi and S. Sakka, “Structure of alkali or alkaline earth niobium gallate glasses,” J. Non-Cryst. Solids 110, 61–68 (1989).
[CrossRef]

K. Kamiya and S. Sakka, “Thermal expansion of TiO2-SiO2 and TiO2-GeO2 glasses,” J. Non-Cryst. Solids 52, 357–363 (1982).
[CrossRef]

Schaufele, R. F.

R. F. Schaufele and M. J. Weber, “Raman scattering by lithium niobate,” Phys. Rev. 152, 705–708 (1966).
[CrossRef]

Song, X. L.

X. L. Song, Y. X. Qu, C. Chao, and M. H. Jiang, “A laser Raman spectra study on the structure of titanium borasilicate glasses,” Chin. J. Light Scatt. 10, 30–36 (1998).

Stevels, J. M.

W. L. Konijnendijk and J. M. Stevels, “Structure of borate glasses,” J. Non-Cryst. Solids 18, 307–331 (1975).
[CrossRef]

Strikler, J. H.

Wang, J.

J. Wang, K. Yang, and C. Jin, “A study on the structure of the crystal LiNbO3:MgO,” Acta Phys. Sin. 48, 1103–1106 (1999).

Wang, S. Z.

H. X. Gao, Z. C. Wang, and S. Z. Wang, “Properties and structure of niobosilicate glasses,” J. Non-Cryst. Solids 112, 332–335 (1989).
[CrossRef]

Wang, Z. C.

H. X. Gao, Z. C. Wang, and S. Z. Wang, “Properties and structure of niobosilicate glasses,” J. Non-Cryst. Solids 112, 332–335 (1989).
[CrossRef]

Webb, W. W.

Weber, M. J.

R. F. Schaufele and M. J. Weber, “Raman scattering by lithium niobate,” Phys. Rev. 152, 705–708 (1966).
[CrossRef]

Yang, K.

J. Wang, K. Yang, and C. Jin, “A study on the structure of the crystal LiNbO3:MgO,” Acta Phys. Sin. 48, 1103–1106 (1999).

You, J. L.

B. K. Yu, T. Y. Yu, G. C. Jiang, and J. L. You, “Phase transition and frequency doubling of β-BaB2O4 and K3Li12−xNb12−xO15+x crystals,” in Optical Devices and Diagnostics in Materials Science, D. L. Andrews, T. Asakura, S. Jutamulia, W. P. Kirk, M. G. Lagally, R. B. Lal, and J. D. Trolinger, eds., Proc. SPIE 4098, 210–213 (2000).
[CrossRef]

Yu, B. K.

B. K. Yu, T. Y. Yu, G. C. Jiang, and J. L. You, “Phase transition and frequency doubling of β-BaB2O4 and K3Li12−xNb12−xO15+x crystals,” in Optical Devices and Diagnostics in Materials Science, D. L. Andrews, T. Asakura, S. Jutamulia, W. P. Kirk, M. G. Lagally, R. B. Lal, and J. D. Trolinger, eds., Proc. SPIE 4098, 210–213 (2000).
[CrossRef]

Yu, T. Y.

B. K. Yu, T. Y. Yu, G. C. Jiang, and J. L. You, “Phase transition and frequency doubling of β-BaB2O4 and K3Li12−xNb12−xO15+x crystals,” in Optical Devices and Diagnostics in Materials Science, D. L. Andrews, T. Asakura, S. Jutamulia, W. P. Kirk, M. G. Lagally, R. B. Lal, and J. D. Trolinger, eds., Proc. SPIE 4098, 210–213 (2000).
[CrossRef]

Acta Phys. Sin. (1)

J. Wang, K. Yang, and C. Jin, “A study on the structure of the crystal LiNbO3:MgO,” Acta Phys. Sin. 48, 1103–1106 (1999).

Appl. Phys. Lett. (2)

K. O. Hill, Y. Fujii, D. C. Johnson, and B. S. Kawasaki, “Photosensitivity in optical fiber waveguides: application to reflection filter fabrication,” Appl. Phys. Lett. 32, 647–649 (1978).
[CrossRef]

K. Miura, J. Qiu, H. Inouye, T. Mitsuyu, and K. Hirao, “Photo-written optical waveguides in various glasses with ultra short pulse laser,” Appl. Phys. Lett. 71, 3329–3331 (1997).
[CrossRef]

Chin. J. Light Scatt. (1)

X. L. Song, Y. X. Qu, C. Chao, and M. H. Jiang, “A laser Raman spectra study on the structure of titanium borasilicate glasses,” Chin. J. Light Scatt. 10, 30–36 (1998).

J. Non-Cryst. Solids (5)

K. Kamiya and S. Sakka, “Thermal expansion of TiO2-SiO2 and TiO2-GeO2 glasses,” J. Non-Cryst. Solids 52, 357–363 (1982).
[CrossRef]

W. L. Konijnendijk and J. M. Stevels, “Structure of borate glasses,” J. Non-Cryst. Solids 18, 307–331 (1975).
[CrossRef]

E. I. Kamitsos, M. A. Karakassides, and A. P. Patsis, “Spectroscopic study of carbonate retention in high-basicity borate glasses,” J. Non-Cryst. Solids 111, 252–259 (1989).
[CrossRef]

K. Fukumi and S. Sakka, “Structure of alkali or alkaline earth niobium gallate glasses,” J. Non-Cryst. Solids 110, 61–68 (1989).
[CrossRef]

H. X. Gao, Z. C. Wang, and S. Z. Wang, “Properties and structure of niobosilicate glasses,” J. Non-Cryst. Solids 112, 332–335 (1989).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. (1)

R. F. Schaufele and M. J. Weber, “Raman scattering by lithium niobate,” Phys. Rev. 152, 705–708 (1966).
[CrossRef]

Proc. SPIE (1)

B. K. Yu, T. Y. Yu, G. C. Jiang, and J. L. You, “Phase transition and frequency doubling of β-BaB2O4 and K3Li12−xNb12−xO15+x crystals,” in Optical Devices and Diagnostics in Materials Science, D. L. Andrews, T. Asakura, S. Jutamulia, W. P. Kirk, M. G. Lagally, R. B. Lal, and J. D. Trolinger, eds., Proc. SPIE 4098, 210–213 (2000).
[CrossRef]

Solid State Commun. (1)

Y. Roussignè, R. Farhi, and C. Dugautier, and J. Gardard, “A Raman study of both phases of barium metaborate (BBO),” Solid State Commun. 82, 287–293 (1992).
[CrossRef]

Other (1)

M. Will, S. Molte, and A. Tuennermann, “Three-dimensional integrated optical device fabrication in glass by femtosecond laser processing,” in Conference on Lasers and Electro-Optics (CLEO), Vol. 73 of OSA Trends in Optics and Photonics Series (Optical Society of America, Washington, D.C., 2000), pp. 127–128.

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Figures (7)

Fig. 1
Fig. 1

Femtosecond laser system: B. S., beam splitter.

Fig. 2
Fig. 2

Raman spectra of borate glass obtained by use of different irradiation times.

Fig. 3
Fig. 3

Micrographs of the microstructure after several irradiation times taken under (A) natural light and (B) cross-polarized light: S, second(s).

Fig. 4
Fig. 4

Raman spectra of borate glass obtained from three layers about the focal area irradiated for 15 min.

Fig. 5
Fig. 5

Raman spectra of niobate glass obtained at two irradiation times.

Fig. 6
Fig. 6

Raman spectra of titanate glass obtained at two irradiation times.

Fig. 7
Fig. 7

Comparison of spectrum unscrambling at 600–1000 cm-1 in Raman spectra of (A) unirradiated titanate glass and (B) glass irradiated for 20 min.

Tables (1)

Tables Icon

Table 1 Raman Spectra Assigned to the Vibrational Modes of the BBO Crystal

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