Abstract

The formation of color centers induced by irradiation with ArF excimer lasers in CaF2 crystals was found to depend strongly on the sodium impurity concentration. Sodium-related color centers were generated by two-photon absorption because the slope of the induced absorption coefficient just after irradiation started was proportional to the square of the laser fluence. The saturation absorption also depended on laser fluence, and a photobleaching induced absorption phenomenon was observed. We concluded that the saturation absorption level was determined by the equilibrium between two-photon excitation and one-photon reverse reaction.

© 2000 Optical Society of America

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References

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  1. D. R. Cope, “UV lasers require tough transmissive materials,” Laser Focus World 28(1), 107–111 (1992).
  2. T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
    [CrossRef]
  3. J. H. Schulman, W. D. Compton, Color Centers in Solids (Pergamon, Oxford, 1962), Chap. X.
  4. D. L. Staebler, S. E. Schnatterly, “Optical studies of a photochromic color center in rare-earth-doped CaF2,” Phys. Rev. B 3, 516–526 (1971).
    [CrossRef]
  5. J. R. O’Connor, J. H. Chen, “Color centers in alkaline earth fluorides,” Phys. Rev. 130, 1790–1901 (1963).
    [CrossRef]
  6. M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Generation of optical absorption bands in CaF2 single crystals by ArF excimer laser irradiation: effect of yttrium impurity,” J. Vac. Sci. Technol. A 16, 3052–3057 (1998).
    [CrossRef]
  7. M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Color center formation and time-resolved photoluminescence by ArF excimer laser irradiation in CaF2 single crystals,” in Inorganic Optical Materials, J. A. Marker, ed., Proc. SPIE3424, 60–70 (1998).
    [CrossRef]
  8. M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Time-resolved photoluminescence for diagnosis of resistance to ArF excimer laser damage to CaF2 single crystals,” J. Opt. Soc. Am. B 16, 1153–1159 (1999).
    [CrossRef]
  9. J. M. G. Tijero, F. Jaque, “Thermal and optical properties of the FA and (F2+)A centers in Na-doped CaF2 crystals,” Phys. Rev. B 41, 3832–3836 (1990).
    [CrossRef]
  10. J. M. G. Tijero, J. Casas-Gonzalez, “On the coloration of CaF2:Na,” J. Phys. Lett. 46, L861–L868 (1985).
    [CrossRef]
  11. J. L. Doualan, J. Margerie, F. Martin-Brunetiere, E. Rzepka, “Magnetic circular dichroism of color centers in CaF2:Na,” J. Phys. Lett. 44, L375–L385 (1985).
    [CrossRef]
  12. V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
    [CrossRef]
  13. E. D. Thoma, H. M. Yochum, P. A. Sheldon, R. T. Williams, “Subpicosecond absorption spectroscopy of band-gap excitation and defect formation in alkali halide crystals,” Nucl. Instrum. Methods Phys. Res. B 141, 552–554 (1998).
    [CrossRef]

1999 (2)

V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Time-resolved photoluminescence for diagnosis of resistance to ArF excimer laser damage to CaF2 single crystals,” J. Opt. Soc. Am. B 16, 1153–1159 (1999).
[CrossRef]

1998 (3)

E. D. Thoma, H. M. Yochum, P. A. Sheldon, R. T. Williams, “Subpicosecond absorption spectroscopy of band-gap excitation and defect formation in alkali halide crystals,” Nucl. Instrum. Methods Phys. Res. B 141, 552–554 (1998).
[CrossRef]

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Generation of optical absorption bands in CaF2 single crystals by ArF excimer laser irradiation: effect of yttrium impurity,” J. Vac. Sci. Technol. A 16, 3052–3057 (1998).
[CrossRef]

1992 (1)

D. R. Cope, “UV lasers require tough transmissive materials,” Laser Focus World 28(1), 107–111 (1992).

1990 (1)

J. M. G. Tijero, F. Jaque, “Thermal and optical properties of the FA and (F2+)A centers in Na-doped CaF2 crystals,” Phys. Rev. B 41, 3832–3836 (1990).
[CrossRef]

1985 (2)

J. M. G. Tijero, J. Casas-Gonzalez, “On the coloration of CaF2:Na,” J. Phys. Lett. 46, L861–L868 (1985).
[CrossRef]

J. L. Doualan, J. Margerie, F. Martin-Brunetiere, E. Rzepka, “Magnetic circular dichroism of color centers in CaF2:Na,” J. Phys. Lett. 44, L375–L385 (1985).
[CrossRef]

1971 (1)

D. L. Staebler, S. E. Schnatterly, “Optical studies of a photochromic color center in rare-earth-doped CaF2,” Phys. Rev. B 3, 516–526 (1971).
[CrossRef]

1963 (1)

J. R. O’Connor, J. H. Chen, “Color centers in alkaline earth fluorides,” Phys. Rev. 130, 1790–1901 (1963).
[CrossRef]

Bloomstein, T. M.

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

Casas-Gonzalez, J.

J. M. G. Tijero, J. Casas-Gonzalez, “On the coloration of CaF2:Na,” J. Phys. Lett. 46, L861–L868 (1985).
[CrossRef]

Chen, J. H.

J. R. O’Connor, J. H. Chen, “Color centers in alkaline earth fluorides,” Phys. Rev. 130, 1790–1901 (1963).
[CrossRef]

Compton, W. D.

J. H. Schulman, W. D. Compton, Color Centers in Solids (Pergamon, Oxford, 1962), Chap. X.

Cope, D. R.

D. R. Cope, “UV lasers require tough transmissive materials,” Laser Focus World 28(1), 107–111 (1992).

Doualan, J. L.

J. L. Doualan, J. Margerie, F. Martin-Brunetiere, E. Rzepka, “Magnetic circular dichroism of color centers in CaF2:Na,” J. Phys. Lett. 44, L375–L385 (1985).
[CrossRef]

Goodman, R. B.

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

Grenville, A.

V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
[CrossRef]

Hardy, D. E.

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

Hosono, H.

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Time-resolved photoluminescence for diagnosis of resistance to ArF excimer laser damage to CaF2 single crystals,” J. Opt. Soc. Am. B 16, 1153–1159 (1999).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Generation of optical absorption bands in CaF2 single crystals by ArF excimer laser irradiation: effect of yttrium impurity,” J. Vac. Sci. Technol. A 16, 3052–3057 (1998).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Color center formation and time-resolved photoluminescence by ArF excimer laser irradiation in CaF2 single crystals,” in Inorganic Optical Materials, J. A. Marker, ed., Proc. SPIE3424, 60–70 (1998).
[CrossRef]

Jaque, F.

J. M. G. Tijero, F. Jaque, “Thermal and optical properties of the FA and (F2+)A centers in Na-doped CaF2 crystals,” Phys. Rev. B 41, 3832–3836 (1990).
[CrossRef]

Kawazoe, H.

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Time-resolved photoluminescence for diagnosis of resistance to ArF excimer laser damage to CaF2 single crystals,” J. Opt. Soc. Am. B 16, 1153–1159 (1999).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Generation of optical absorption bands in CaF2 single crystals by ArF excimer laser irradiation: effect of yttrium impurity,” J. Vac. Sci. Technol. A 16, 3052–3057 (1998).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Color center formation and time-resolved photoluminescence by ArF excimer laser irradiation in CaF2 single crystals,” in Inorganic Optical Materials, J. A. Marker, ed., Proc. SPIE3424, 60–70 (1998).
[CrossRef]

Kunz, R. R.

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

Liberman, V.

V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
[CrossRef]

Margerie, J.

J. L. Doualan, J. Margerie, F. Martin-Brunetiere, E. Rzepka, “Magnetic circular dichroism of color centers in CaF2:Na,” J. Phys. Lett. 44, L375–L385 (1985).
[CrossRef]

Martin-Brunetiere, F.

J. L. Doualan, J. Margerie, F. Martin-Brunetiere, E. Rzepka, “Magnetic circular dichroism of color centers in CaF2:Na,” J. Phys. Lett. 44, L375–L385 (1985).
[CrossRef]

Mizuguchi, M.

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Time-resolved photoluminescence for diagnosis of resistance to ArF excimer laser damage to CaF2 single crystals,” J. Opt. Soc. Am. B 16, 1153–1159 (1999).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Generation of optical absorption bands in CaF2 single crystals by ArF excimer laser irradiation: effect of yttrium impurity,” J. Vac. Sci. Technol. A 16, 3052–3057 (1998).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Color center formation and time-resolved photoluminescence by ArF excimer laser irradiation in CaF2 single crystals,” in Inorganic Optical Materials, J. A. Marker, ed., Proc. SPIE3424, 60–70 (1998).
[CrossRef]

O’Connor, J. R.

J. R. O’Connor, J. H. Chen, “Color centers in alkaline earth fluorides,” Phys. Rev. 130, 1790–1901 (1963).
[CrossRef]

Ogawa, T.

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Time-resolved photoluminescence for diagnosis of resistance to ArF excimer laser damage to CaF2 single crystals,” J. Opt. Soc. Am. B 16, 1153–1159 (1999).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Generation of optical absorption bands in CaF2 single crystals by ArF excimer laser irradiation: effect of yttrium impurity,” J. Vac. Sci. Technol. A 16, 3052–3057 (1998).
[CrossRef]

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Color center formation and time-resolved photoluminescence by ArF excimer laser irradiation in CaF2 single crystals,” in Inorganic Optical Materials, J. A. Marker, ed., Proc. SPIE3424, 60–70 (1998).
[CrossRef]

Palmacci, S. T.

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

Rothschild, M.

V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
[CrossRef]

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

Rzepka, E.

J. L. Doualan, J. Margerie, F. Martin-Brunetiere, E. Rzepka, “Magnetic circular dichroism of color centers in CaF2:Na,” J. Phys. Lett. 44, L375–L385 (1985).
[CrossRef]

Schnatterly, S. E.

D. L. Staebler, S. E. Schnatterly, “Optical studies of a photochromic color center in rare-earth-doped CaF2,” Phys. Rev. B 3, 516–526 (1971).
[CrossRef]

Schulman, J. H.

J. H. Schulman, W. D. Compton, Color Centers in Solids (Pergamon, Oxford, 1962), Chap. X.

Sedlacek, J. H. C.

V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
[CrossRef]

Sheldon, P. A.

E. D. Thoma, H. M. Yochum, P. A. Sheldon, R. T. Williams, “Subpicosecond absorption spectroscopy of band-gap excitation and defect formation in alkali halide crystals,” Nucl. Instrum. Methods Phys. Res. B 141, 552–554 (1998).
[CrossRef]

Staebler, D. L.

D. L. Staebler, S. E. Schnatterly, “Optical studies of a photochromic color center in rare-earth-doped CaF2,” Phys. Rev. B 3, 516–526 (1971).
[CrossRef]

Thoma, E. D.

E. D. Thoma, H. M. Yochum, P. A. Sheldon, R. T. Williams, “Subpicosecond absorption spectroscopy of band-gap excitation and defect formation in alkali halide crystals,” Nucl. Instrum. Methods Phys. Res. B 141, 552–554 (1998).
[CrossRef]

Tijero, J. M. G.

J. M. G. Tijero, F. Jaque, “Thermal and optical properties of the FA and (F2+)A centers in Na-doped CaF2 crystals,” Phys. Rev. B 41, 3832–3836 (1990).
[CrossRef]

J. M. G. Tijero, J. Casas-Gonzalez, “On the coloration of CaF2:Na,” J. Phys. Lett. 46, L861–L868 (1985).
[CrossRef]

Uttaro, R. S.

V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
[CrossRef]

Williams, R. T.

E. D. Thoma, H. M. Yochum, P. A. Sheldon, R. T. Williams, “Subpicosecond absorption spectroscopy of band-gap excitation and defect formation in alkali halide crystals,” Nucl. Instrum. Methods Phys. Res. B 141, 552–554 (1998).
[CrossRef]

Yochum, H. M.

E. D. Thoma, H. M. Yochum, P. A. Sheldon, R. T. Williams, “Subpicosecond absorption spectroscopy of band-gap excitation and defect formation in alkali halide crystals,” Nucl. Instrum. Methods Phys. Res. B 141, 552–554 (1998).
[CrossRef]

J. Non-Cryst. Solids (1)

V. Liberman, M. Rothschild, J. H. C. Sedlacek, R. S. Uttaro, A. Grenville, “Excimer-laser-induced densification of fused silica: laser-fluence and material-grade effects on the scaling law,” J. Non-Cryst. Solids 244, 159–171 (1999).
[CrossRef]

J. Opt. Soc. Am. B (1)

J. Phys. Lett. (2)

J. M. G. Tijero, J. Casas-Gonzalez, “On the coloration of CaF2:Na,” J. Phys. Lett. 46, L861–L868 (1985).
[CrossRef]

J. L. Doualan, J. Margerie, F. Martin-Brunetiere, E. Rzepka, “Magnetic circular dichroism of color centers in CaF2:Na,” J. Phys. Lett. 44, L375–L385 (1985).
[CrossRef]

J. Vac. Sci. Technol. A (1)

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Generation of optical absorption bands in CaF2 single crystals by ArF excimer laser irradiation: effect of yttrium impurity,” J. Vac. Sci. Technol. A 16, 3052–3057 (1998).
[CrossRef]

J. Vac. Sci. Technol. B (1)

T. M. Bloomstein, M. Rothschild, R. R. Kunz, D. E. Hardy, R. B. Goodman, S. T. Palmacci, “Critical issues in 157 nm lithography,” J. Vac. Sci. Technol. B 16, 3154–3157 (1998).
[CrossRef]

Laser Focus World (1)

D. R. Cope, “UV lasers require tough transmissive materials,” Laser Focus World 28(1), 107–111 (1992).

Nucl. Instrum. Methods Phys. Res. B (1)

E. D. Thoma, H. M. Yochum, P. A. Sheldon, R. T. Williams, “Subpicosecond absorption spectroscopy of band-gap excitation and defect formation in alkali halide crystals,” Nucl. Instrum. Methods Phys. Res. B 141, 552–554 (1998).
[CrossRef]

Phys. Rev. (1)

J. R. O’Connor, J. H. Chen, “Color centers in alkaline earth fluorides,” Phys. Rev. 130, 1790–1901 (1963).
[CrossRef]

Phys. Rev. B (2)

J. M. G. Tijero, F. Jaque, “Thermal and optical properties of the FA and (F2+)A centers in Na-doped CaF2 crystals,” Phys. Rev. B 41, 3832–3836 (1990).
[CrossRef]

D. L. Staebler, S. E. Schnatterly, “Optical studies of a photochromic color center in rare-earth-doped CaF2,” Phys. Rev. B 3, 516–526 (1971).
[CrossRef]

Other (2)

J. H. Schulman, W. D. Compton, Color Centers in Solids (Pergamon, Oxford, 1962), Chap. X.

M. Mizuguchi, H. Hosono, H. Kawazoe, T. Ogawa, “Color center formation and time-resolved photoluminescence by ArF excimer laser irradiation in CaF2 single crystals,” in Inorganic Optical Materials, J. A. Marker, ed., Proc. SPIE3424, 60–70 (1998).
[CrossRef]

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Figures (6)

Fig. 1
Fig. 1

Experimental setup for in situ transmission measurements during ArF excimer-laser irradiation.

Fig. 2
Fig. 2

Dependence of the induced absorption coefficient after ArF excimer-laser irradiation on the concentration of sodium in pure CaF2 crystals. The induced absorption coefficient was completely saturated in all samples under the irradiation conditions shown.

Fig. 3
Fig. 3

Comparison of ArF-induced absorption spectra in the sodium-doped CaF2 crystal (Sample A) and in a typical pure-CaF2 crystal (Sample B): p, pulse. We show the results at different fluences to make clear the different fluence values needed for the absorption coefficients to appear roughly the same.

Fig. 4
Fig. 4

Behavior of in situ absorption induced by ArF irradiation at various fluences in Samples A and B: p, pulse. At all the fluences the ArF-induced absorption showed a monotonic increase from zero to plateau (saturation absorption). Solid curves, best fitting curves of a single exponential function defined as Eq. (1) with measured data.

Fig. 5
Fig. 5

Laser fluence dependence of (a) the slope of the induced absorption coefficient just after irradiation starts (αstart), (b) the saturation absorption coefficient (αsat), and (c) the time constant (T C ). The slopes of αstart were proportional to the square of the laser fluence, and the saturation absorption coefficients depended on the laser fluence for both Samples A and B. The value of T C for the YFC formation was ∼5 × 105 pulses at a laser fluence of 2 (mJ/cm2)/pulse (from Fig. 2 of Ref. 6) and larger by an order of magnitude than that (5 × 104 pulses) of sodium-related color-center formation.

Fig. 6
Fig. 6

Photobleaching of ArF excimer-laser-induced absorption in a sodium-doped CaF2 crystal: p, pulse. The large absorption induced by irradiation with a high fluence of 10 (mJ/cm2)/pulse decreased and returned to the level of saturation absorption at the low fluence of 0.8 (mJ/cm2)/pulse when the low-fluence irradiation impinged upon the sample at the same position as the high-fluence irradiation. The same phenomenon was observed in pure CaF2 crystals.

Equations (10)

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

α=-lntransmission after irradiation/theoretical transmissionsample thickness,
α193 nm=αsat1-exp-NTc,
dPdN=-k2P+k1F,
dFdN=+k2P-k1F,
P+F=P0=const.,
dFdN=k2P0-k2+k1F.
F=k2P0k2+k11-exp-k2+k1N.
α=k2α0k2+k11-exp-k2+k1N,
αstart=k2α0N.
αsat=k2k2+k1 α0.

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