Abstract

A sharp resonant amplification of the third-order susceptibility of a diluted β-carotene solution in dodecane is observed by means of the time-resolved optical Kerr effect when the wavelength of the probe is tuned in the range of 490–570 nm. The resonance is well in the red with respect to the 0–0 first electronic transition; some evidence is given of the possible role of higher excited states and of two-photon resonance.

© 1992 Optical Society of America

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References

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  1. C. Kalpouzos, D. McMorrow, W. T. Lotshaw, G. A. Kenney-Wallace, Chem. Phys. Lett. 150, 138 (1988).
    [CrossRef]
  2. P. Foggi, V. F. Kamalov, R. Righini, R. Torre, “Molecular dynamics of β-carotene in solution measured by subpicosecond transient optical Kerr effect,” Chem. Phys. Lett. (to be published).
  3. R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
    [CrossRef]
  4. A. R. Mantini, M. P. Marzocchi, G. Smulevich, J. Chem. Phys. 91, 85 (1989).
    [CrossRef]
  5. N. Bloembergen, H. Lotem, R. T. Lynch, Indian J. Pure Appl. Phys. 16, 151 (1978).
  6. C. Ferrante, A. Speghini, A. Feis, R. Bozio, “Multiresonance FWM as a probe of spectral broadening mechanisms: influence of excited state dynamics on resonance CARS processes,” J. Lumin. (to be published).
  7. F. Inagaki, M. Tasumi, T. Miyozawa, J. Mol. Spectrosc. 50, 286 (1974).
    [CrossRef]
  8. H. Lotem, R. T. Lynch, N. Bloembergen, Phys. Rev. A 14, 1748 (1976).
    [CrossRef]
  9. S. D. Kramers, N. Bloembergen, Phys. Rev. B 9, 1853 (1974); S. D. Kramers, N. Bloembergen, Phys. Rev. B, 14, 4654 (1976); .
    [CrossRef]
  10. P. Foggi, P. R. Salvi, R. Bini, E. Castellucci, J. Mol. Struct. 175, 147 (1988).
    [CrossRef]
  11. F. C. Spano, S. Mukamel, Phys. Rev. A 40, 5783 (1989).
    [CrossRef] [PubMed]

1989 (2)

A. R. Mantini, M. P. Marzocchi, G. Smulevich, J. Chem. Phys. 91, 85 (1989).
[CrossRef]

F. C. Spano, S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

1988 (2)

P. Foggi, P. R. Salvi, R. Bini, E. Castellucci, J. Mol. Struct. 175, 147 (1988).
[CrossRef]

C. Kalpouzos, D. McMorrow, W. T. Lotshaw, G. A. Kenney-Wallace, Chem. Phys. Lett. 150, 138 (1988).
[CrossRef]

1978 (1)

N. Bloembergen, H. Lotem, R. T. Lynch, Indian J. Pure Appl. Phys. 16, 151 (1978).

1977 (1)

R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
[CrossRef]

1976 (1)

H. Lotem, R. T. Lynch, N. Bloembergen, Phys. Rev. A 14, 1748 (1976).
[CrossRef]

1974 (2)

S. D. Kramers, N. Bloembergen, Phys. Rev. B 9, 1853 (1974); S. D. Kramers, N. Bloembergen, Phys. Rev. B, 14, 4654 (1976); .
[CrossRef]

F. Inagaki, M. Tasumi, T. Miyozawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

Bini, R.

P. Foggi, P. R. Salvi, R. Bini, E. Castellucci, J. Mol. Struct. 175, 147 (1988).
[CrossRef]

Bloembergen, N.

N. Bloembergen, H. Lotem, R. T. Lynch, Indian J. Pure Appl. Phys. 16, 151 (1978).

H. Lotem, R. T. Lynch, N. Bloembergen, Phys. Rev. A 14, 1748 (1976).
[CrossRef]

S. D. Kramers, N. Bloembergen, Phys. Rev. B 9, 1853 (1974); S. D. Kramers, N. Bloembergen, Phys. Rev. B, 14, 4654 (1976); .
[CrossRef]

Bozio, R.

C. Ferrante, A. Speghini, A. Feis, R. Bozio, “Multiresonance FWM as a probe of spectral broadening mechanisms: influence of excited state dynamics on resonance CARS processes,” J. Lumin. (to be published).

Castellucci, E.

P. Foggi, P. R. Salvi, R. Bini, E. Castellucci, J. Mol. Struct. 175, 147 (1988).
[CrossRef]

Feis, A.

C. Ferrante, A. Speghini, A. Feis, R. Bozio, “Multiresonance FWM as a probe of spectral broadening mechanisms: influence of excited state dynamics on resonance CARS processes,” J. Lumin. (to be published).

Ferrante, C.

C. Ferrante, A. Speghini, A. Feis, R. Bozio, “Multiresonance FWM as a probe of spectral broadening mechanisms: influence of excited state dynamics on resonance CARS processes,” J. Lumin. (to be published).

Foggi, P.

P. Foggi, P. R. Salvi, R. Bini, E. Castellucci, J. Mol. Struct. 175, 147 (1988).
[CrossRef]

P. Foggi, V. F. Kamalov, R. Righini, R. Torre, “Molecular dynamics of β-carotene in solution measured by subpicosecond transient optical Kerr effect,” Chem. Phys. Lett. (to be published).

Hellwarth, R. W.

R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
[CrossRef]

Inagaki, F.

F. Inagaki, M. Tasumi, T. Miyozawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

Kalpouzos, C.

C. Kalpouzos, D. McMorrow, W. T. Lotshaw, G. A. Kenney-Wallace, Chem. Phys. Lett. 150, 138 (1988).
[CrossRef]

Kamalov, V. F.

P. Foggi, V. F. Kamalov, R. Righini, R. Torre, “Molecular dynamics of β-carotene in solution measured by subpicosecond transient optical Kerr effect,” Chem. Phys. Lett. (to be published).

Kenney-Wallace, G. A.

C. Kalpouzos, D. McMorrow, W. T. Lotshaw, G. A. Kenney-Wallace, Chem. Phys. Lett. 150, 138 (1988).
[CrossRef]

Kramers, S. D.

S. D. Kramers, N. Bloembergen, Phys. Rev. B 9, 1853 (1974); S. D. Kramers, N. Bloembergen, Phys. Rev. B, 14, 4654 (1976); .
[CrossRef]

Lotem, H.

N. Bloembergen, H. Lotem, R. T. Lynch, Indian J. Pure Appl. Phys. 16, 151 (1978).

H. Lotem, R. T. Lynch, N. Bloembergen, Phys. Rev. A 14, 1748 (1976).
[CrossRef]

Lotshaw, W. T.

C. Kalpouzos, D. McMorrow, W. T. Lotshaw, G. A. Kenney-Wallace, Chem. Phys. Lett. 150, 138 (1988).
[CrossRef]

Lynch, R. T.

N. Bloembergen, H. Lotem, R. T. Lynch, Indian J. Pure Appl. Phys. 16, 151 (1978).

H. Lotem, R. T. Lynch, N. Bloembergen, Phys. Rev. A 14, 1748 (1976).
[CrossRef]

Mantini, A. R.

A. R. Mantini, M. P. Marzocchi, G. Smulevich, J. Chem. Phys. 91, 85 (1989).
[CrossRef]

Marzocchi, M. P.

A. R. Mantini, M. P. Marzocchi, G. Smulevich, J. Chem. Phys. 91, 85 (1989).
[CrossRef]

McMorrow, D.

C. Kalpouzos, D. McMorrow, W. T. Lotshaw, G. A. Kenney-Wallace, Chem. Phys. Lett. 150, 138 (1988).
[CrossRef]

Miyozawa, T.

F. Inagaki, M. Tasumi, T. Miyozawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

Mukamel, S.

F. C. Spano, S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

Righini, R.

P. Foggi, V. F. Kamalov, R. Righini, R. Torre, “Molecular dynamics of β-carotene in solution measured by subpicosecond transient optical Kerr effect,” Chem. Phys. Lett. (to be published).

Salvi, P. R.

P. Foggi, P. R. Salvi, R. Bini, E. Castellucci, J. Mol. Struct. 175, 147 (1988).
[CrossRef]

Smulevich, G.

A. R. Mantini, M. P. Marzocchi, G. Smulevich, J. Chem. Phys. 91, 85 (1989).
[CrossRef]

Spano, F. C.

F. C. Spano, S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

Speghini, A.

C. Ferrante, A. Speghini, A. Feis, R. Bozio, “Multiresonance FWM as a probe of spectral broadening mechanisms: influence of excited state dynamics on resonance CARS processes,” J. Lumin. (to be published).

Tasumi, M.

F. Inagaki, M. Tasumi, T. Miyozawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

Torre, R.

P. Foggi, V. F. Kamalov, R. Righini, R. Torre, “Molecular dynamics of β-carotene in solution measured by subpicosecond transient optical Kerr effect,” Chem. Phys. Lett. (to be published).

Chem. Phys. Lett. (1)

C. Kalpouzos, D. McMorrow, W. T. Lotshaw, G. A. Kenney-Wallace, Chem. Phys. Lett. 150, 138 (1988).
[CrossRef]

Indian J. Pure Appl. Phys. (1)

N. Bloembergen, H. Lotem, R. T. Lynch, Indian J. Pure Appl. Phys. 16, 151 (1978).

J. Chem. Phys. (1)

A. R. Mantini, M. P. Marzocchi, G. Smulevich, J. Chem. Phys. 91, 85 (1989).
[CrossRef]

J. Mol. Spectrosc. (1)

F. Inagaki, M. Tasumi, T. Miyozawa, J. Mol. Spectrosc. 50, 286 (1974).
[CrossRef]

J. Mol. Struct. (1)

P. Foggi, P. R. Salvi, R. Bini, E. Castellucci, J. Mol. Struct. 175, 147 (1988).
[CrossRef]

Phys. Rev. A (2)

F. C. Spano, S. Mukamel, Phys. Rev. A 40, 5783 (1989).
[CrossRef] [PubMed]

H. Lotem, R. T. Lynch, N. Bloembergen, Phys. Rev. A 14, 1748 (1976).
[CrossRef]

Phys. Rev. B (1)

S. D. Kramers, N. Bloembergen, Phys. Rev. B 9, 1853 (1974); S. D. Kramers, N. Bloembergen, Phys. Rev. B, 14, 4654 (1976); .
[CrossRef]

Prog. Quantum Electron. (1)

R. W. Hellwarth, Prog. Quantum Electron. 5, 1 (1977).
[CrossRef]

Other (2)

P. Foggi, V. F. Kamalov, R. Righini, R. Torre, “Molecular dynamics of β-carotene in solution measured by subpicosecond transient optical Kerr effect,” Chem. Phys. Lett. (to be published).

C. Ferrante, A. Speghini, A. Feis, R. Bozio, “Multiresonance FWM as a probe of spectral broadening mechanisms: influence of excited state dynamics on resonance CARS processes,” J. Lumin. (to be published).

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Figures (3)

Fig. 1
Fig. 1

Time-resolved OKE signal of β-carotene solution in dodecane (5 × 10−4 M, T = 298 K) measured at different probe wavelengths. λpump = 604 nm, λprobe = 490–507 nm.

Fig. 2
Fig. 2

Absorption spectrum of β-carotene in dodecane. The wavelengths of the pump and probe beams are marked; also shown is the position λ00 of the purely electronic resonance for β-carotene in hexane at T = 298 K.4 The hatched area shows the spectral range of ωpump + ωprobe. The inset shows a scheme of the electronic levels of β-carotene.

Fig. 3
Fig. 3

Ratio of instantaneous to orientational contributions to the OKE signal of β-carotene in dodecane versus the probe wavelength (λpump = 604 nm). The dotted curve is the red tail of the absorption spectrum of β-carotene. The solid curve is merely a guide to the eye.

Equations (1)

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P i ( 3 ) = χ i j k l ( 3 ) el E j ( t ) E k ( t ) E l ( t ) + E j ( t ) - t d t χ i j k l ( 3 ) n ( t - t ) E k * ( t ) E l ( t ) .

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