Abstract

A hyper-Rayleigh scattering (HRS) system based on an optical parametric power oscillator is described. The first hyperpolarizability, β, of Crystal Violet dye was measured at 1450 and 1500 nm. The resonance-free β value, β(0), for this octupole was found to be comparable with that of the dipolar dye Disperse Red 1 but with the nonlinearity–transparency trade-off worse for the octupole. The discrepancy in β(0) with that reported previously is explained in terms of resonance and the adequacy of the octupolar three-state model. The possibility of dye aggregation by solvent-dependent HRS is investigated.

© 1996 Optical Society of America

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  1. S. R. Marder, J. W. Perry, W. P. SchaefferScience 245, 626 (1989).
    [CrossRef] [PubMed]
  2. W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
    [CrossRef]
  3. I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
    [CrossRef]
  4. L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
    [CrossRef]
  5. K. Clays, A. PersoonsPhys. Rev. Lett. 66, 2980 (1991).
    [CrossRef] [PubMed]
  6. S. R. Marder, J. W. PerryScience 263, 1706 (1994).
    [CrossRef] [PubMed]
  7. R. G. DenningJ. Mater. Chem. 5, 365 (1995).
    [CrossRef]
  8. M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
    [CrossRef]
  9. M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
    [CrossRef]
  10. T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
    [CrossRef]
  11. J. L. OudarJ. Chem. Phys. 67, 446 (1977).
    [CrossRef]
  12. J. Zyss, T. Chauvan, C. Dhenaut, I. LedouxChem. Phys. 177, 281 (1993).
    [CrossRef]
  13. K. Clays, A. PersoonsRev. Sci. Instrum. 65, 2190 (1994).
    [CrossRef]
  14. G. N. Lewis, T. T. Magel, D. LipkinJ. Am. Chem. Soc. 64, 1774 (1942).
    [CrossRef]

1995 (2)

R. G. DenningJ. Mater. Chem. 5, 365 (1995).
[CrossRef]

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

1994 (4)

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

K. Clays, A. PersoonsRev. Sci. Instrum. 65, 2190 (1994).
[CrossRef]

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

S. R. Marder, J. W. PerryScience 263, 1706 (1994).
[CrossRef] [PubMed]

1993 (2)

W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
[CrossRef]

J. Zyss, T. Chauvan, C. Dhenaut, I. LedouxChem. Phys. 177, 281 (1993).
[CrossRef]

1991 (2)

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

K. Clays, A. PersoonsPhys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

1990 (1)

I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
[CrossRef]

1989 (1)

S. R. Marder, J. W. Perry, W. P. SchaefferScience 245, 626 (1989).
[CrossRef] [PubMed]

1977 (1)

J. L. OudarJ. Chem. Phys. 67, 446 (1977).
[CrossRef]

1942 (1)

G. N. Lewis, T. T. Magel, D. LipkinJ. Am. Chem. Soc. 64, 1774 (1942).
[CrossRef]

Branger, C.

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

Brienne, J.

I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
[CrossRef]

Chauchard, E.

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
[CrossRef]

Chauvan, T.

J. Zyss, T. Chauvan, C. Dhenaut, I. LedouxChem. Phys. 177, 281 (1993).
[CrossRef]

Cheng, L.-T.

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

Clays, K.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

K. Clays, A. PersoonsRev. Sci. Instrum. 65, 2190 (1994).
[CrossRef]

K. Clays, A. PersoonsPhys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

De Jonge, R.

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Denning, R. G.

R. G. DenningJ. Mater. Chem. 5, 365 (1995).
[CrossRef]

W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
[CrossRef]

Dhenaut, C.

J. Zyss, T. Chauvan, C. Dhenaut, I. LedouxChem. Phys. 177, 281 (1993).
[CrossRef]

Flipse, M. C.

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Jenneskens, L. W.

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Laidlaw, W. M.

W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
[CrossRef]

Ledoux, I.

J. Zyss, T. Chauvan, C. Dhenaut, I. LedouxChem. Phys. 177, 281 (1993).
[CrossRef]

I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
[CrossRef]

Lehn, J.-M.

I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
[CrossRef]

Lequan, M.

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

Lewis, G. N.

G. N. Lewis, T. T. Magel, D. LipkinJ. Am. Chem. Soc. 64, 1774 (1942).
[CrossRef]

Lipkin, D.

G. N. Lewis, T. T. Magel, D. LipkinJ. Am. Chem. Soc. 64, 1774 (1942).
[CrossRef]

Magel, T. T.

G. N. Lewis, T. T. Magel, D. LipkinJ. Am. Chem. Soc. 64, 1774 (1942).
[CrossRef]

Marder, S. R.

S. R. Marder, J. W. PerryScience 263, 1706 (1994).
[CrossRef] [PubMed]

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

S. R. Marder, J. W. Perry, W. P. SchaefferScience 245, 626 (1989).
[CrossRef] [PubMed]

Marsman, A. W.

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Meredith, G. R.

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

Oudar, J. L.

J. L. OudarJ. Chem. Phys. 67, 446 (1977).
[CrossRef]

Perry, J. W.

S. R. Marder, J. W. PerryScience 263, 1706 (1994).
[CrossRef] [PubMed]

S. R. Marder, J. W. Perry, W. P. SchaefferScience 245, 626 (1989).
[CrossRef] [PubMed]

Persoons, A.

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

K. Clays, A. PersoonsRev. Sci. Instrum. 65, 2190 (1994).
[CrossRef]

W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
[CrossRef]

K. Clays, A. PersoonsPhys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

Reinhoudt, D.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

Rikken, G.

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

Samyn, C.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

Schaeffer, W. P.

S. R. Marder, J. W. Perry, W. P. SchaefferScience 245, 626 (1989).
[CrossRef] [PubMed]

Siegel, J. S.

I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
[CrossRef]

Simon, J.

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

Stevenson, S. H.

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

Tam, W.

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

Thami, T.

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

Van Walree, C. A.

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Verbiest, T.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
[CrossRef]

Wolff, J.

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

Woudenberg, R. H.

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

Zyss, J.

J. Zyss, T. Chauvan, C. Dhenaut, I. LedouxChem. Phys. 177, 281 (1993).
[CrossRef]

I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
[CrossRef]

Chem. Phys. (1)

J. Zyss, T. Chauvan, C. Dhenaut, I. LedouxChem. Phys. 177, 281 (1993).
[CrossRef]

Chem. Phys. Lett. (3)

I. Ledoux, J. Zyss, J. S. Siegel, J. Brienne, J.-M. LehnChem. Phys. Lett. 172, 440 (1990).
[CrossRef]

M. Lequan, C. Branger, J. Simon, T. Thami, E. Chauchard, A. PersoonsChem. Phys. Lett. 229, 101 (1994).
[CrossRef]

M. C. Flipse, R. De Jonge, R. H. Woudenberg, A. W. Marsman, C. A. Van Walree, L. W. JenneskensChem. Phys. Lett. 245, 297 (1995).
[CrossRef]

J. Am. Chem. Soc. (2)

T. Verbiest, K. Clays, C. Samyn, J. Wolff, D. Reinhoudt, A. PersoonsJ. Am. Chem. Soc. 116, 9320 (1994).
[CrossRef]

G. N. Lewis, T. T. Magel, D. LipkinJ. Am. Chem. Soc. 64, 1774 (1942).
[CrossRef]

J. Chem. Phys. (1)

J. L. OudarJ. Chem. Phys. 67, 446 (1977).
[CrossRef]

J. Mater. Chem. (1)

R. G. DenningJ. Mater. Chem. 5, 365 (1995).
[CrossRef]

J. Phys. Chem. (1)

L.-T. Cheng, W. Tam, S. H. Stevenson, G. R. Meredith, G. Rikken, S. R. MarderJ. Phys. Chem. 95, 10631 (1991).
[CrossRef]

Nature (1)

W. M. Laidlaw, R. G. Denning, T. Verbiest, E. Chauchard, A. PersoonsNature (London) 363, 58 (1993).
[CrossRef]

Phys. Rev. Lett. (1)

K. Clays, A. PersoonsPhys. Rev. Lett. 66, 2980 (1991).
[CrossRef] [PubMed]

Rev. Sci. Instrum. (1)

K. Clays, A. PersoonsRev. Sci. Instrum. 65, 2190 (1994).
[CrossRef]

Science (2)

S. R. Marder, J. W. Perry, W. P. SchaefferScience 245, 626 (1989).
[CrossRef] [PubMed]

S. R. Marder, J. W. PerryScience 263, 1706 (1994).
[CrossRef] [PubMed]

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Figures (3)

Fig. 1
Fig. 1

HRS experimental setup using the 355-nm output of an Infinity Nd:YAG laser: WP, half-wave plate for the OPPO (OPO) idler wave; BD, beam dump; LP’s, long-pass filters; M’s, mirrors; L1 (L2), 250- (50-) mm focal-length lens; HP (VP), horizontal (vertical) polarizer; LTB, light-tight box; PMT, photomultiplier tube; A/D, analog-to-digital converter.

Fig. 2
Fig. 2

A, I(2ω) against half-wave-plate angle for various concentrations (2.87 × 1018, 5.07 × 1018, 8.45 × 1018, 10.37 × 1018 molecules/cm3) of CV in CHCl3 at 1500 nm. The curves are best fits of experimental data to Eq. (1). B, as for A but for 5.00 × 1018, 9.99 × 1018, 15.14 × 1018 molecules/cm3 of CV in CH3CN at 1450 nm. A pure solvent curve is included, showing that I(2ω) was below detection threshold.

Fig. 3
Fig. 3

A, maximum SH intensity versus solute number density for CV and DR1 in chloroform at 1500 nm. B, as for A but for CV and DPD in acetonitrile at 1450 nm.

Equations (3)

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I ( 2 ω ) = A [ sin ( 2 ϕ + α ) ] 4 + b ,
I ( 2 ω ) = G [ N 1 β 1 2 + N 2 β 2 2 ] I ( ω ) 2 ,
A ( s ) A ( r ) = [ N 1 β 1 2 + N 2 β 2 2 ] s [ N 1 β 1 2 + N 2 β 2 2 ] r .

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