Abstract

Diffractive optics are applied to six-wave mixing processes to provide a single optic approach to attaining the required, relatively complex, phase-matching geometry to discriminate against lower-order nonlinear responses. The diffractive optics were designed specifically for broad-bandwidth operation and passive phase locking of the appropriate pulse pairs for use in femtosecond two-dimensional Raman studies of the dynamic structure of liquids. The fifth-order signal was studied in liquid CS2; two different colors were used for the excitation and the probe to reduce background scatter, as were two different phase-matching geometries with different degrees of suppression of cascaded third-order processes.

© 2000 Optical Society of America

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References

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  1. J. A. Rogers and K. A. Nelson, Phys. B 219&220, 562 (1996).
    [CrossRef]
  2. G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
    [CrossRef]
  3. G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. B 103, 603 (1999).
  4. G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. A 103, 10,630 (1999).
  5. A. A. Maznev, K. A. Nelson, and J. A. Rogers, Opt. Lett. 23, 1319 (1998); A. A. Maznev, T. F. Crimmins, and K. A. Nelson, Opt. Lett. 23, 1378 (1998).
    [CrossRef]
  6. G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
    [CrossRef]
  7. Y. Tanimura and S. Mukamel, J. Chem. Phys. 99, 9496 (1993).
  8. K. Tominaga and K. Yoshihara, Phys. Rev. Lett. 76, 987 (1996).
    [CrossRef] [PubMed]
  9. T. Steffen and K. Duppen, Phys. Rev. Lett. 76, 1224 (1996).
    [CrossRef] [PubMed]
  10. A. Tokmakoff and G. R. Fleming, J. Chem. Phys. 106, 2569 (1997).
  11. D. J. Ulness, J. C. Kirkwood, and A. C. Albrecht, J. Chem. Phys. 108, 3897 (1998).
  12. D. A. Blank, L. J. Kaufman, and G. R. Fleming, J. Chem. Phys. 111, 3105 (1999).
  13. M. W. Farn and W. B. Veldkamp, in Handbook of Optics, M. Bass, ed. (McGraw-Hill, New York, 1995), Vol. II, p. 8.11.
  14. R. L. Murry and J. T. Fourkas, J. Chem. Phys. 107, 9726 (1997).
  15. S. Saito and I. Ohmine, J. Chem. Phys. 108, 240 (1998).

1999 (3)

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. B 103, 603 (1999).

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. A 103, 10,630 (1999).

D. A. Blank, L. J. Kaufman, and G. R. Fleming, J. Chem. Phys. 111, 3105 (1999).

1998 (5)

D. J. Ulness, J. C. Kirkwood, and A. C. Albrecht, J. Chem. Phys. 108, 3897 (1998).

S. Saito and I. Ohmine, J. Chem. Phys. 108, 240 (1998).

A. A. Maznev, K. A. Nelson, and J. A. Rogers, Opt. Lett. 23, 1319 (1998); A. A. Maznev, T. F. Crimmins, and K. A. Nelson, Opt. Lett. 23, 1378 (1998).
[CrossRef]

G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
[CrossRef]

G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
[CrossRef]

1997 (2)

A. Tokmakoff and G. R. Fleming, J. Chem. Phys. 106, 2569 (1997).

R. L. Murry and J. T. Fourkas, J. Chem. Phys. 107, 9726 (1997).

1996 (3)

J. A. Rogers and K. A. Nelson, Phys. B 219&220, 562 (1996).
[CrossRef]

K. Tominaga and K. Yoshihara, Phys. Rev. Lett. 76, 987 (1996).
[CrossRef] [PubMed]

T. Steffen and K. Duppen, Phys. Rev. Lett. 76, 1224 (1996).
[CrossRef] [PubMed]

1993 (1)

Y. Tanimura and S. Mukamel, J. Chem. Phys. 99, 9496 (1993).

Albrecht, A. C.

D. J. Ulness, J. C. Kirkwood, and A. C. Albrecht, J. Chem. Phys. 108, 3897 (1998).

Astinov, V.

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. B 103, 603 (1999).

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. A 103, 10,630 (1999).

Blank, D. A.

D. A. Blank, L. J. Kaufman, and G. R. Fleming, J. Chem. Phys. 111, 3105 (1999).

Chiu, H.-L.

G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
[CrossRef]

Dadusc, G.

G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
[CrossRef]

G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
[CrossRef]

Duppen, K.

T. Steffen and K. Duppen, Phys. Rev. Lett. 76, 1224 (1996).
[CrossRef] [PubMed]

Farn, M. W.

M. W. Farn and W. B. Veldkamp, in Handbook of Optics, M. Bass, ed. (McGraw-Hill, New York, 1995), Vol. II, p. 8.11.

Fleming, G. R.

D. A. Blank, L. J. Kaufman, and G. R. Fleming, J. Chem. Phys. 111, 3105 (1999).

A. Tokmakoff and G. R. Fleming, J. Chem. Phys. 106, 2569 (1997).

Fourkas, J. T.

R. L. Murry and J. T. Fourkas, J. Chem. Phys. 107, 9726 (1997).

Goodno, G. D.

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. A 103, 10,630 (1999).

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. B 103, 603 (1999).

G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
[CrossRef]

G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
[CrossRef]

Kaufman, L. J.

D. A. Blank, L. J. Kaufman, and G. R. Fleming, J. Chem. Phys. 111, 3105 (1999).

Kirkwood, J. C.

D. J. Ulness, J. C. Kirkwood, and A. C. Albrecht, J. Chem. Phys. 108, 3897 (1998).

Maznev, A. A.

Miller, R. J. D.

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. A 103, 10,630 (1999).

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. B 103, 603 (1999).

G. D. Goodno, G. Dadusc, and R. J. D. Miller, J. Opt. Soc. Am. B 15, 1791 (1998).
[CrossRef]

G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
[CrossRef]

Mukamel, S.

Y. Tanimura and S. Mukamel, J. Chem. Phys. 99, 9496 (1993).

Murry, R. L.

R. L. Murry and J. T. Fourkas, J. Chem. Phys. 107, 9726 (1997).

Nelson, K. A.

Ogilvie, J.

G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
[CrossRef]

Ohmine, I.

S. Saito and I. Ohmine, J. Chem. Phys. 108, 240 (1998).

Rogers, J. A.

Saito, S.

S. Saito and I. Ohmine, J. Chem. Phys. 108, 240 (1998).

Steffen, T.

T. Steffen and K. Duppen, Phys. Rev. Lett. 76, 1224 (1996).
[CrossRef] [PubMed]

Tanimura, Y.

Y. Tanimura and S. Mukamel, J. Chem. Phys. 99, 9496 (1993).

Tokmakoff, A.

A. Tokmakoff and G. R. Fleming, J. Chem. Phys. 106, 2569 (1997).

Tominaga, K.

K. Tominaga and K. Yoshihara, Phys. Rev. Lett. 76, 987 (1996).
[CrossRef] [PubMed]

Ulness, D. J.

D. J. Ulness, J. C. Kirkwood, and A. C. Albrecht, J. Chem. Phys. 108, 3897 (1998).

Veldkamp, W. B.

M. W. Farn and W. B. Veldkamp, in Handbook of Optics, M. Bass, ed. (McGraw-Hill, New York, 1995), Vol. II, p. 8.11.

Yoshihara, K.

K. Tominaga and K. Yoshihara, Phys. Rev. Lett. 76, 987 (1996).
[CrossRef] [PubMed]

Isr. J. Chem. (1)

G. Dadusc, G. D. Goodno, H.-L. Chiu, J. Ogilvie, and R. J. D. Miller, Isr. J. Chem. 38, 191 (1998).
[CrossRef]

J. Chem. Phys. (6)

Y. Tanimura and S. Mukamel, J. Chem. Phys. 99, 9496 (1993).

A. Tokmakoff and G. R. Fleming, J. Chem. Phys. 106, 2569 (1997).

D. J. Ulness, J. C. Kirkwood, and A. C. Albrecht, J. Chem. Phys. 108, 3897 (1998).

D. A. Blank, L. J. Kaufman, and G. R. Fleming, J. Chem. Phys. 111, 3105 (1999).

R. L. Murry and J. T. Fourkas, J. Chem. Phys. 107, 9726 (1997).

S. Saito and I. Ohmine, J. Chem. Phys. 108, 240 (1998).

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

J. Phys. Chem. A (1)

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. A 103, 10,630 (1999).

J. Phys. Chem. B (1)

G. D. Goodno, V. Astinov, and R. J. D. Miller, J. Phys. Chem. B 103, 603 (1999).

Opt. Lett. (1)

Phys. B (1)

J. A. Rogers and K. A. Nelson, Phys. B 219&220, 562 (1996).
[CrossRef]

Phys. Rev. Lett. (2)

K. Tominaga and K. Yoshihara, Phys. Rev. Lett. 76, 987 (1996).
[CrossRef] [PubMed]

T. Steffen and K. Duppen, Phys. Rev. Lett. 76, 1224 (1996).
[CrossRef] [PubMed]

Other (1)

M. W. Farn and W. B. Veldkamp, in Handbook of Optics, M. Bass, ed. (McGraw-Hill, New York, 1995), Vol. II, p. 8.11.

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Figures (3)

Fig. 1
Fig. 1

Ladder diagram for the nonlinear six-wave mixing process (top left) and phase-matching beam pattern (top right). Bottom, calculated diffraction efficiency as a function of wavelength for beams 1 and 4 for the target beam pattern.

Fig. 2
Fig. 2

Experimental setup: S, sample; M1, M2, mirrors; D1, D2, pinholes, G, glass window; C1, C2, tilt plates; H, λ/2 plate; P, polarizer; PD, photodiode.

Fig. 3
Fig. 3

(a) Scattered light intensity in the χ5 phase-matched direction in the geometry of Fig. 1. The signal at τ2200 fs is due to cascaded χ3. (b) Scattered light intensity along the χ5 phase-matched direction with crossed excitation beam geometry for further suppression of cascaded χ3. Insets, beam geometries.

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