Abstract

We present what are to our knowledge the first measurements of the phase of the infrared–visible sum-frequency generation signal. We introduce two techniques and apply the measurements to the determination of the polar orientation of a selected group of atoms within an adsorbed molecule.

© 1990 Optical Society of America

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References

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  1. Y. R. Shen, The Principles of Nonlinear Optics (Wiley, New York, 1984).
  2. Y. R. Shen, Ann. Rev. Phys. Chem. 40, 327 (1989).
    [CrossRef]
  3. Y. R. Shen, Nature (London) 337, 519 (1989).
    [CrossRef]
  4. X. D. Zhu, H. Suhr, Y. R. Shen, Phys. Rev. B 35, 3047 (1987).
    [CrossRef]
  5. J. H. Hunt, P. Guyot-Sionnest, Y. R. Shen, Chem. Phys. Lett. 133, 189 (1987).
    [CrossRef]
  6. P. Guyot-Sionnest, J. H. Hunt, Y. R. Shen, Phys. Rev. Lett. 59, 1597 (1987).
    [CrossRef] [PubMed]
  7. A. L. Harris, C. E. D. Chidsey, N. J. Levinos, D. N. Loiacono, Chem. Phys. Lett. 141, 350 (1987).
    [CrossRef]
  8. R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
    [CrossRef]
  9. P. Guyot-Sionnest, R. Superfine, J. H. Hunt, Y. R. Shen, Chem. Phys. Lett. 144, 1 (1988).
    [CrossRef]
  10. R. K. Chang, J. Ducuing, N. Bloembergen, Phys. Rev. Lett. 15, 6 (1965).
  11. H. W. K. Tom, T. F. Heinz, Y. R. Shen, Phys. Rev. Lett. 51, 1983 (1983).
    [CrossRef]
  12. K. Keminitz, K. Bhattacharyya, J. M. Hicks, G. R. Pinto, K. B. Eisenthal, T. F. Heinz, Chem. Phys. Lett. 131, 285 (1986).
    [CrossRef]
  13. G. Berkovic, Y. R. Shen, G. Marowsky, R. Steinhoff, J. Opt. Soc. Am. B 6, 205 (1989).
    [CrossRef]
  14. H. W. K. Tom, Ph.D. thesis (University of California, Berkeley, California, 1985).
  15. R. Superfine, J. Y. Huang, Y. R. Shen, “Experimental determination of the sign of molecular dipole moment derivatives; an infrared-visible sum-frequency generation absolute phase measurement study,” Chem. Phys. Lett. (to be published).

1989 (3)

Y. R. Shen, Ann. Rev. Phys. Chem. 40, 327 (1989).
[CrossRef]

Y. R. Shen, Nature (London) 337, 519 (1989).
[CrossRef]

G. Berkovic, Y. R. Shen, G. Marowsky, R. Steinhoff, J. Opt. Soc. Am. B 6, 205 (1989).
[CrossRef]

1988 (2)

R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
[CrossRef]

P. Guyot-Sionnest, R. Superfine, J. H. Hunt, Y. R. Shen, Chem. Phys. Lett. 144, 1 (1988).
[CrossRef]

1987 (4)

X. D. Zhu, H. Suhr, Y. R. Shen, Phys. Rev. B 35, 3047 (1987).
[CrossRef]

J. H. Hunt, P. Guyot-Sionnest, Y. R. Shen, Chem. Phys. Lett. 133, 189 (1987).
[CrossRef]

P. Guyot-Sionnest, J. H. Hunt, Y. R. Shen, Phys. Rev. Lett. 59, 1597 (1987).
[CrossRef] [PubMed]

A. L. Harris, C. E. D. Chidsey, N. J. Levinos, D. N. Loiacono, Chem. Phys. Lett. 141, 350 (1987).
[CrossRef]

1986 (1)

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

1983 (1)

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

1965 (1)

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

Berkovic, G.

Bhattacharyya, K.

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

Bloembergen, N.

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

Chang, R. K.

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

Chidsey, C. E. D.

A. L. Harris, C. E. D. Chidsey, N. J. Levinos, D. N. Loiacono, Chem. Phys. Lett. 141, 350 (1987).
[CrossRef]

Ducuing, J.

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

Eisenthal, K. B.

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

Guyot-Sionnest, P.

P. Guyot-Sionnest, R. Superfine, J. H. Hunt, Y. R. Shen, Chem. Phys. Lett. 144, 1 (1988).
[CrossRef]

R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
[CrossRef]

J. H. Hunt, P. Guyot-Sionnest, Y. R. Shen, Chem. Phys. Lett. 133, 189 (1987).
[CrossRef]

P. Guyot-Sionnest, J. H. Hunt, Y. R. Shen, Phys. Rev. Lett. 59, 1597 (1987).
[CrossRef] [PubMed]

Harris, A. L.

A. L. Harris, C. E. D. Chidsey, N. J. Levinos, D. N. Loiacono, Chem. Phys. Lett. 141, 350 (1987).
[CrossRef]

Heinz, T. F.

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

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

Hicks, J. M.

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

Huang, J. Y.

R. Superfine, J. Y. Huang, Y. R. Shen, “Experimental determination of the sign of molecular dipole moment derivatives; an infrared-visible sum-frequency generation absolute phase measurement study,” Chem. Phys. Lett. (to be published).

Hunt, J. H.

P. Guyot-Sionnest, R. Superfine, J. H. Hunt, Y. R. Shen, Chem. Phys. Lett. 144, 1 (1988).
[CrossRef]

R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
[CrossRef]

J. H. Hunt, P. Guyot-Sionnest, Y. R. Shen, Chem. Phys. Lett. 133, 189 (1987).
[CrossRef]

P. Guyot-Sionnest, J. H. Hunt, Y. R. Shen, Phys. Rev. Lett. 59, 1597 (1987).
[CrossRef] [PubMed]

Kao, C. T.

R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
[CrossRef]

Keminitz, K.

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

Levinos, N. J.

A. L. Harris, C. E. D. Chidsey, N. J. Levinos, D. N. Loiacono, Chem. Phys. Lett. 141, 350 (1987).
[CrossRef]

Loiacono, D. N.

A. L. Harris, C. E. D. Chidsey, N. J. Levinos, D. N. Loiacono, Chem. Phys. Lett. 141, 350 (1987).
[CrossRef]

Marowsky, G.

Pinto, G. R.

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

Shen, Y. R.

Y. R. Shen, Ann. Rev. Phys. Chem. 40, 327 (1989).
[CrossRef]

Y. R. Shen, Nature (London) 337, 519 (1989).
[CrossRef]

G. Berkovic, Y. R. Shen, G. Marowsky, R. Steinhoff, J. Opt. Soc. Am. B 6, 205 (1989).
[CrossRef]

R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
[CrossRef]

P. Guyot-Sionnest, R. Superfine, J. H. Hunt, Y. R. Shen, Chem. Phys. Lett. 144, 1 (1988).
[CrossRef]

P. Guyot-Sionnest, J. H. Hunt, Y. R. Shen, Phys. Rev. Lett. 59, 1597 (1987).
[CrossRef] [PubMed]

X. D. Zhu, H. Suhr, Y. R. Shen, Phys. Rev. B 35, 3047 (1987).
[CrossRef]

J. H. Hunt, P. Guyot-Sionnest, Y. R. Shen, Chem. Phys. Lett. 133, 189 (1987).
[CrossRef]

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

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

R. Superfine, J. Y. Huang, Y. R. Shen, “Experimental determination of the sign of molecular dipole moment derivatives; an infrared-visible sum-frequency generation absolute phase measurement study,” Chem. Phys. Lett. (to be published).

Steinhoff, R.

Suhr, H.

X. D. Zhu, H. Suhr, Y. R. Shen, Phys. Rev. B 35, 3047 (1987).
[CrossRef]

Superfine, R.

R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
[CrossRef]

P. Guyot-Sionnest, R. Superfine, J. H. Hunt, Y. R. Shen, Chem. Phys. Lett. 144, 1 (1988).
[CrossRef]

R. Superfine, J. Y. Huang, Y. R. Shen, “Experimental determination of the sign of molecular dipole moment derivatives; an infrared-visible sum-frequency generation absolute phase measurement study,” Chem. Phys. Lett. (to be published).

Tom, H. W. K.

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

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

Zhu, X. D.

X. D. Zhu, H. Suhr, Y. R. Shen, Phys. Rev. B 35, 3047 (1987).
[CrossRef]

Ann. Rev. Phys. Chem. (1)

Y. R. Shen, Ann. Rev. Phys. Chem. 40, 327 (1989).
[CrossRef]

Chem. Phys. Lett. (4)

J. H. Hunt, P. Guyot-Sionnest, Y. R. Shen, Chem. Phys. Lett. 133, 189 (1987).
[CrossRef]

A. L. Harris, C. E. D. Chidsey, N. J. Levinos, D. N. Loiacono, Chem. Phys. Lett. 141, 350 (1987).
[CrossRef]

P. Guyot-Sionnest, R. Superfine, J. H. Hunt, Y. R. Shen, Chem. Phys. Lett. 144, 1 (1988).
[CrossRef]

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

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

Nature (London) (1)

Y. R. Shen, Nature (London) 337, 519 (1989).
[CrossRef]

Phys. Rev. B (1)

X. D. Zhu, H. Suhr, Y. R. Shen, Phys. Rev. B 35, 3047 (1987).
[CrossRef]

Phys. Rev. Lett. (3)

P. Guyot-Sionnest, J. H. Hunt, Y. R. Shen, Phys. Rev. Lett. 59, 1597 (1987).
[CrossRef] [PubMed]

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

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

Surf. Sci. (1)

R. Superfine, P. Guyot-Sionnest, J. H. Hunt, C. T. Kao, Y. R. Shen, Surf. Sci. 200, L445 (1988).
[CrossRef]

Other (3)

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

R. Superfine, J. Y. Huang, Y. R. Shen, “Experimental determination of the sign of molecular dipole moment derivatives; an infrared-visible sum-frequency generation absolute phase measurement study,” Chem. Phys. Lett. (to be published).

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

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Figures (2)

Fig. 1
Fig. 1

(a) SFG spectrum (circles) of the CH3 symmetric stretch of the PDA monolayer on the water surface. The solid curve is obtained from a fit from Eqs. (3) and (4); the dashed curve is the phase of χNL obtained from the fit to the intensity, while the data points from the interference measurement are represented by bars, (b) Comparison of the interference patterns from quartz (squares) and the PDA monolayer (circles) obtained at ωir = 2859 cm−1 (top curves), 2876 cm−1 (middle curves), and 2889 cm−1 (bottom curves). The data have been normalized and shifted vertically for comparison.

Fig. 2
Fig. 2

Rotational dependence of SFG intensity for crystalline quartz off resonance (triangles), at CH3 symmetric stretch resonance for PDA deposited monolayer (circles), and on 4′-(n-octyl)-4-cyanobiphenyl monolayer (squares). The curves are fits of data from Eqs. (2) and (3).

Equations (7)

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P ( 2 ) ( ω s ) = χ NL ( ω S = ω 1 + ω 2 ) : E 1 ( ω υ ) E 2 ( ω ir ) ,
χ NL = χ S + χ B ,
χ S = N α ( 2 ) ,
α ( 2 ) = α NR + α R , α R = A Q / ( ξ q ω ir i Γ q ) ,
χ B = i L c χ ,
χ yyz B = i L c χ XXX sin 2 α cos α ,
S ( ω S ) | E I ( ω s ) + A P ( 2 ) ( ω s ) | 2 | 1 + | B | ( χ S + C χ B ) exp ( i Φ ) | 2 ,

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