Abstract

Several experiments on surface second-harmonic generation are presented to show how the contribution from a transparent substrate can interfere with that from an adsorbate monolayer. The interference depends on the relative phase of the two contributions, which varies with the molecular orientation, the laser frequency, the polarization, and the optical geometry.

© 1989 Optical Society of America

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References

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  1. Y. R. Shen, Ann. Rev. Mater. Sci. 16, 69 (1986); in New Laser and Optical Investigations of Chemistry and Structure of Interfaces, R. B. Hall and A. B. Ellis, eds. (Verlag Chemie, Weinheim, 1986), p. 151.
    [Crossref]
  2. G. L. Richmond, H. M. Rojhantalab, J. M. Robinson, and V. L. Shannon, J. Opt. Soc. Am. B 4, 228 (1987).
    [Crossref]
  3. J. M. Chen, J. R. Bower, C. S. Wang, and C. H. Lee, Opt. Commun. 9, 132 (1973).
    [Crossref]
  4. X. D. Zhu, Y. R. Shen, and R. Carr, Surf. Sci. 163, 114 (1985).
    [Crossref]
  5. T. F. Heinz, H. W. K. Tom, and Y. R. Shen, Phys. Rev. A 28, 1883 (1983).
    [Crossref]
  6. Th. Rasing, Y. R. Shen, M. W. Kim, and S. Grubb, Phys. Rev. Lett. 55, 2903 (1985).
    [Crossref] [PubMed]
  7. G. Berkovic, Th. Rasing, and Y. R. Shen, J. Chem. Phys. 85, 7374 (1986).
    [Crossref]
  8. I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
    [Crossref]
  9. G. Berkovic, Th. Rasing, and Y. R. Shen, J. Opt. Soc. Am. B 4, 945 (1987).
    [Crossref]
  10. O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).
  11. G. Marowsky, A. Gierulski, and B. Dick, Opt. Commun. 52, 339 (1985).
    [Crossref]
  12. Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 25.
  13. P. Guyot-Sionnest, W. Chen, and Y. R. Shen, Phys. Rev. B 33, 8254 (1986); P. Guyot-Sionnest and Y. R. Shen, Phys. Rev. B 35, 4420 (1987).
    [Crossref]
  14. H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
    [Crossref]
  15. R. K. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
    [Crossref]
  16. H. W. K. Tom, T. F. Heinz, and Y. R. Shen, Phys. Rev. Lett. 51, 1983 (1983).
    [Crossref]
  17. K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
    [Crossref]
  18. Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
    [Crossref]
  19. H. W. K. Tom, Ph.D. dissertation (University of California, Berkeley, Berkeley, Calif., 1985).
  20. P. Guyot-Sionnest, H. Hsuing, and Y. R. Shen, Phys. Rev. Lett. 57, 2963 (1986).
    [Crossref] [PubMed]
  21. T. F. Heinz, Ph.D. dissertation (University of California, Berkeley, Berkeley, Calif., 1983).

1987 (2)

1986 (7)

P. Guyot-Sionnest, W. Chen, and Y. R. Shen, Phys. Rev. B 33, 8254 (1986); P. Guyot-Sionnest and Y. R. Shen, Phys. Rev. B 35, 4420 (1987).
[Crossref]

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
[Crossref]

P. Guyot-Sionnest, H. Hsuing, and Y. R. Shen, Phys. Rev. Lett. 57, 2963 (1986).
[Crossref] [PubMed]

Y. R. Shen, Ann. Rev. Mater. Sci. 16, 69 (1986); in New Laser and Optical Investigations of Chemistry and Structure of Interfaces, R. B. Hall and A. B. Ellis, eds. (Verlag Chemie, Weinheim, 1986), p. 151.
[Crossref]

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Chem. Phys. 85, 7374 (1986).
[Crossref]

1985 (5)

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Th. Rasing, Y. R. Shen, M. W. Kim, and S. Grubb, Phys. Rev. Lett. 55, 2903 (1985).
[Crossref] [PubMed]

X. D. Zhu, Y. R. Shen, and R. Carr, Surf. Sci. 163, 114 (1985).
[Crossref]

O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).

G. Marowsky, A. Gierulski, and B. Dick, Opt. Commun. 52, 339 (1985).
[Crossref]

1983 (2)

H. W. K. Tom, T. F. Heinz, and Y. R. Shen, Phys. Rev. Lett. 51, 1983 (1983).
[Crossref]

T. F. Heinz, H. W. K. Tom, and Y. R. Shen, Phys. Rev. A 28, 1883 (1983).
[Crossref]

1973 (1)

J. M. Chen, J. R. Bower, C. S. Wang, and C. H. Lee, Opt. Commun. 9, 132 (1973).
[Crossref]

1965 (1)

R. K. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[Crossref]

Akhmediev, N. N.

O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).

Aktsipetrov, O. A.

O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).

Baranova, I. M.

O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).

Berkovic, G.

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Opt. Soc. Am. B 4, 945 (1987).
[Crossref]

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Chem. Phys. 85, 7374 (1986).
[Crossref]

Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
[Crossref]

Bhattacharyya, K.

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

Bloembergen, N.

R. K. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[Crossref]

Bower, J. R.

J. M. Chen, J. R. Bower, C. S. Wang, and C. H. Lee, Opt. Commun. 9, 132 (1973).
[Crossref]

Cade, N. A.

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Carr, R.

X. D. Zhu, Y. R. Shen, and R. Carr, Surf. Sci. 163, 114 (1985).
[Crossref]

Chang, R. K.

R. K. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[Crossref]

Chen, J. M.

J. M. Chen, J. R. Bower, C. S. Wang, and C. H. Lee, Opt. Commun. 9, 132 (1973).
[Crossref]

Chen, W.

P. Guyot-Sionnest, W. Chen, and Y. R. Shen, Phys. Rev. B 33, 8254 (1986); P. Guyot-Sionnest and Y. R. Shen, Phys. Rev. B 35, 4420 (1987).
[Crossref]

Cross, G. H.

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Crowell, J. E.

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

Dick, B.

G. Marowsky, A. Gierulski, and B. Dick, Opt. Commun. 52, 339 (1985).
[Crossref]

Ducuing, J.

R. K. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[Crossref]

Earls, J. D.

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Eisenthal, K. B.

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

Gierulski, A.

G. Marowsky, A. Gierulski, and B. Dick, Opt. Commun. 52, 339 (1985).
[Crossref]

Girling, I. R.

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Grubb, S.

Th. Rasing, Y. R. Shen, M. W. Kim, and S. Grubb, Phys. Rev. Lett. 55, 2903 (1985).
[Crossref] [PubMed]

Grubb, S. G.

Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
[Crossref]

Guyot-Sionnest, P.

P. Guyot-Sionnest, H. Hsuing, and Y. R. Shen, Phys. Rev. Lett. 57, 2963 (1986).
[Crossref] [PubMed]

P. Guyot-Sionnest, W. Chen, and Y. R. Shen, Phys. Rev. B 33, 8254 (1986); P. Guyot-Sionnest and Y. R. Shen, Phys. Rev. B 35, 4420 (1987).
[Crossref]

Heinz, T. F.

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

H. W. K. Tom, T. F. Heinz, and Y. R. Shen, Phys. Rev. Lett. 51, 1983 (1983).
[Crossref]

T. F. Heinz, H. W. K. Tom, and Y. R. Shen, Phys. Rev. A 28, 1883 (1983).
[Crossref]

T. F. Heinz, Ph.D. dissertation (University of California, Berkeley, Berkeley, Calif., 1983).

Hicks, J. M.

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

Hsuing, H.

P. Guyot-Sionnest, H. Hsuing, and Y. R. Shen, Phys. Rev. Lett. 57, 2963 (1986).
[Crossref] [PubMed]

Kemnitz, K.

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

Kim, M. W.

Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
[Crossref]

Th. Rasing, Y. R. Shen, M. W. Kim, and S. Grubb, Phys. Rev. Lett. 55, 2903 (1985).
[Crossref] [PubMed]

Kolinsky, P. V.

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Lee, C. H.

J. M. Chen, J. R. Bower, C. S. Wang, and C. H. Lee, Opt. Commun. 9, 132 (1973).
[Crossref]

Marowsky, G.

G. Marowsky, A. Gierulski, and B. Dick, Opt. Commun. 52, 339 (1985).
[Crossref]

Mate, C. M.

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

Mishina, E. D.

O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).

Novak, V. R.

O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).

Peterson, I. R.

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Pinto, G. R.

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

Rasing, Th.

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Opt. Soc. Am. B 4, 945 (1987).
[Crossref]

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Chem. Phys. 85, 7374 (1986).
[Crossref]

Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
[Crossref]

Th. Rasing, Y. R. Shen, M. W. Kim, and S. Grubb, Phys. Rev. Lett. 55, 2903 (1985).
[Crossref] [PubMed]

Richmond, G. L.

Robinson, J. M.

Rojhantalab, H. M.

Shannon, V. L.

Shen, Y. R.

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Opt. Soc. Am. B 4, 945 (1987).
[Crossref]

Y. R. Shen, Ann. Rev. Mater. Sci. 16, 69 (1986); in New Laser and Optical Investigations of Chemistry and Structure of Interfaces, R. B. Hall and A. B. Ellis, eds. (Verlag Chemie, Weinheim, 1986), p. 151.
[Crossref]

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Chem. Phys. 85, 7374 (1986).
[Crossref]

Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
[Crossref]

P. Guyot-Sionnest, H. Hsuing, and Y. R. Shen, Phys. Rev. Lett. 57, 2963 (1986).
[Crossref] [PubMed]

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

P. Guyot-Sionnest, W. Chen, and Y. R. Shen, Phys. Rev. B 33, 8254 (1986); P. Guyot-Sionnest and Y. R. Shen, Phys. Rev. B 35, 4420 (1987).
[Crossref]

Th. Rasing, Y. R. Shen, M. W. Kim, and S. Grubb, Phys. Rev. Lett. 55, 2903 (1985).
[Crossref] [PubMed]

X. D. Zhu, Y. R. Shen, and R. Carr, Surf. Sci. 163, 114 (1985).
[Crossref]

T. F. Heinz, H. W. K. Tom, and Y. R. Shen, Phys. Rev. A 28, 1883 (1983).
[Crossref]

H. W. K. Tom, T. F. Heinz, and Y. R. Shen, Phys. Rev. Lett. 51, 1983 (1983).
[Crossref]

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 25.

Somorjai, G. A.

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

Tom, H. W. K.

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

H. W. K. Tom, T. F. Heinz, and Y. R. Shen, Phys. Rev. Lett. 51, 1983 (1983).
[Crossref]

T. F. Heinz, H. W. K. Tom, and Y. R. Shen, Phys. Rev. A 28, 1883 (1983).
[Crossref]

H. W. K. Tom, Ph.D. dissertation (University of California, Berkeley, Berkeley, Calif., 1985).

Wang, C. S.

J. M. Chen, J. R. Bower, C. S. Wang, and C. H. Lee, Opt. Commun. 9, 132 (1973).
[Crossref]

Zhu, X. D.

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

X. D. Zhu, Y. R. Shen, and R. Carr, Surf. Sci. 163, 114 (1985).
[Crossref]

Ann. Rev. Mater. Sci. (1)

Y. R. Shen, Ann. Rev. Mater. Sci. 16, 69 (1986); in New Laser and Optical Investigations of Chemistry and Structure of Interfaces, R. B. Hall and A. B. Ellis, eds. (Verlag Chemie, Weinheim, 1986), p. 151.
[Crossref]

Chem. Phys. Lett. (2)

K. Kemnitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, and T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
[Crossref]

Th. Rasing, G. Berkovic, Y. R. Shen, S. G. Grubb, and M. W. Kim, Chem. Phys. Lett. 130, 1 (1986).
[Crossref]

J. Chem. Phys. (1)

G. Berkovic, Th. Rasing, and Y. R. Shen, J. Chem. Phys. 85, 7374 (1986).
[Crossref]

J. Opt. Soc. Am. B (2)

Opt. Commun. (2)

G. Marowsky, A. Gierulski, and B. Dick, Opt. Commun. 52, 339 (1985).
[Crossref]

J. M. Chen, J. R. Bower, C. S. Wang, and C. H. Lee, Opt. Commun. 9, 132 (1973).
[Crossref]

Phys. Rev. A (1)

T. F. Heinz, H. W. K. Tom, and Y. R. Shen, Phys. Rev. A 28, 1883 (1983).
[Crossref]

Phys. Rev. B (1)

P. Guyot-Sionnest, W. Chen, and Y. R. Shen, Phys. Rev. B 33, 8254 (1986); P. Guyot-Sionnest and Y. R. Shen, Phys. Rev. B 35, 4420 (1987).
[Crossref]

Phys. Rev. Lett. (4)

R. K. Chang, J. Ducuing, and N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
[Crossref]

H. W. K. Tom, T. F. Heinz, and Y. R. Shen, Phys. Rev. Lett. 51, 1983 (1983).
[Crossref]

Th. Rasing, Y. R. Shen, M. W. Kim, and S. Grubb, Phys. Rev. Lett. 55, 2903 (1985).
[Crossref] [PubMed]

P. Guyot-Sionnest, H. Hsuing, and Y. R. Shen, Phys. Rev. Lett. 57, 2963 (1986).
[Crossref] [PubMed]

Sov. Phys. JETP (1)

O. A. Aktsipetrov, N. N. Akhmediev, I. M. Baranova, E. D. Mishina, and V. R. Novak, Sov. Phys. JETP 62, 524 (1985).

Surf. Sci. (2)

H. W. K. Tom, C. M. Mate, X. D. Zhu, J. E. Crowell, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 172, 466 (1986); H. W. K. Tom, X. D. Zhu, Y. R. Shen, and G. A. Somorjai, Surf. Sci. 167, 167 (1986).
[Crossref]

X. D. Zhu, Y. R. Shen, and R. Carr, Surf. Sci. 163, 114 (1985).
[Crossref]

Thin Solid Films (1)

I. R. Girling, N. A. Cade, P. V. Kolinsky, J. D. Earls, G. H. Cross, and I. R. Peterson, Thin Solid Films 132, 101 (1985).
[Crossref]

Other (3)

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984), Chap. 25.

T. F. Heinz, Ph.D. dissertation (University of California, Berkeley, Berkeley, Calif., 1983).

H. W. K. Tom, Ph.D. dissertation (University of California, Berkeley, Berkeley, Calif., 1985).

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Figures (6)

Fig. 1
Fig. 1

SHG from an adsorbate-covered substrate in (a) simple reflection and (b) TIR geometries at air–glass interfaces. Wave-vector conservation causes the fundamental and second-harmonic beams to emerge collinearly in the simple reflection geometry but not in the TIR geometry.

Fig. 2
Fig. 2

SHG intensities from two selected adsorbate-covered substrates as a function of concentration of adsorbate dipping solution used. The curves are least-squares fits to Eq. (4). (a) 8CB on glass, in simple reflection, with s-polarized 750-nm fundamental and p-polarized SHG output. (b) DAP on fused silica, in TIR geometry, with s-polarized 720-nm fundamental and p-polarized SHG output.

Fig. 3
Fig. 3

Comparison of interferences obtained when a second harmonic is generated from both the sample (glass and 8CB-coated glass) and a crystalline quartz plate mounted onto a translation stage. The fundamental (700 nm) was s polarized, and the second harmonic was p polarized in simple reflection. The dashed curves are fits to the theoretical interference band shape y = [A + B sin (2πx/Lc)]2, where Lc = 3.6 ± 0.1 cm, as given by Eq. (3).

Fig. 4
Fig. 4

Vectorial relations between χ ads ( 2 ) , χ sub ( 2 ) , χ sub ( 2 ) and relative phases.

Fig. 5
Fig. 5

The relative phase, Δϕads, for Rhodamine 110 on glass is shown at various wavelengths. The effect of the second-harmonic frequency’s entering into resonance with the S0S2 absorption is shown by comparison with the absorption spectrum (measured in isopropyl alcohol solution) of Rhodamine 110. The absorption beginning at ≈400 nm is the edge of the S0S1 transition.

Fig. 6
Fig. 6

SHG intensity from Rhodamine 110-covered silica substrate in TIR geometry with p-polarized fundamental input at 720 nm and p-polarized SHG output. The curve is the best fit to expression (4).

Equations (5)

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

P s ( 2 ) ( 2 ω ) = χ s ( 2 ) : E ( ω ) E ( ω ) .
χ s ( 2 ) = χ sub ( 2 ) + χ ads ( 2 ) ,
L c = λ / [ 2 ( n 2 ω - n ω ) ] ,
SH signal χ s ( 2 ) 2 = χ sub ( 2 ) - N β 2 ,
[ F 1 χ x z x ( 2 ) + F 2 χ z z z ( 2 ) + F 3 χ z x x ( 2 ) ] sub + [ F 1 χ x z x ( 2 ) + F 2 χ z z z ( 2 ) + F 3 χ z x x ( 2 ) ] ads .

Metrics