Abstract

Optical control of elementary molecular motion through impulsive stimulated Raman scattering is enhanced by means of timed sequences of femtosecond pulses that are produced by pulse-shaping techniques. In particular, terahertz-rate trains of femtosecond pulses are used for repetitive impulsive excitation of individual phonon modes in an α-perylene molecular crystal. When the pulse repetition rate is matched to the desired phonon frequency, mode-selective vibrational amplification is achieved. A comparison of data acquired with the transient-grating and the pump–probe experimental geometries reveals the timing dynamics of the induced phonon oscillations with respect to the driving femtosecond pulse sequence.

© 1991 Optical Society of America

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  1. R. A. Mathies, C. H. Brito Cruz, W. T. Pollard, and C. V. Shank, Science 240, 777 (1988).
    [CrossRef] [PubMed]
  2. Y.-X. Yan, L.-T. Cheng, and K. A. Nelson, in Advances in Nonlinear Spectroscopy, R. J. H. Clark and R. E. Hester, eds., Vol. 16 of Advances in Spectroscopy Series (Wiley, Chichester, UK, 1988), pp. 299–355; S. Ruhman, A. G. Joly, B. Kohler, L. R. Williams, and K. A. Nelson, Rev. Phys. Appl. 22, 1717 (1987).
    [CrossRef]
  3. J. Chesnoy and A. Mokhtari, Phys. Rev. A 38, 3566 (1988).
    [CrossRef] [PubMed]
  4. F. W. Wise, M. J. Rosker, and C. L. Tang, J. Chem. Phys. 86, 2827 (1986).
    [CrossRef]
  5. M. Dantus, M. J. Rosker, and A. H. Zewail, J. Chem. Phys. 89, 6128 (1988); N. F. Scherer, C. Sipes, R. B. Bernstein, and A. H. Zewail, J. Chem. Phys. 92, 5239 (1990).
    [CrossRef]
  6. H. L. Fragnito, J.-Y. Bigot, P. C. Becker, and C. V. Shank, Chem. Phys. Lett. 160, 101 (1989).
    [CrossRef]
  7. D. Tannor, R. Kosloff, and S. A. Rice, J. Chem. Phys. 85, 5805 (1986); S. Shi, A. Woody, and H. Rabitz, J. Chem. Phys. 88, 6870 (1988).
    [CrossRef]
  8. Y.-X. Yan, E. B. Gamble, and K. A. Nelson, J. Chem. Phys. 83, 5391 (1985).
    [CrossRef]
  9. A. M. Weiner, J. P. Heritage, and E. M. Kirschner, J. Opt. Soc. Am. B 5, 1563 (1988).
    [CrossRef]
  10. A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, Opt. Lett. 15, 326 (1990).
    [CrossRef]
  11. M. Haner and W. S. Warren, Appl. Phys. Lett. 52, 1458 (1988); W. S. Warren, Science 242, 878 (1988).
    [CrossRef] [PubMed]
  12. A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, Science 247, 1327 (1990).
    [CrossRef]
  13. J. Tanaka, T. Kishi, and M. Tanaka, Bull. Chem. Soc. Jpn. 47, 2376 (1974).
    [CrossRef]
  14. T. J. Kosic, C. L. Schosser, and D. D. Dlott, Chem. Phys. Lett. 96, 57 (1983).
    [CrossRef]
  15. S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
    [CrossRef]
  16. R. L. Fork, B. I. Greene, and C. V. Shank, Appl. Phys. Lett. 38, 671 (1981); J. A. Valdmanis, R. L. Fork, and J. P. Gordon, Opt. Lett. 10, 131 (1985).
    [CrossRef] [PubMed]
  17. W. H. Knox, M. C. Downer, R. L. Fork, and C. V. Shank, Opt. Lett. 9, 552 (1984).
    [CrossRef] [PubMed]
  18. A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
    [CrossRef] [PubMed]
  19. A. M. Weiner and D. E. Leaird, Opt. Lett. 15, 51 (1990).
    [CrossRef] [PubMed]
  20. Y.-X. Yan and K. A. Nelson, J. Chem. Phys. 87, 6240, 6257 (1987).
    [CrossRef]
  21. Y. J. Yan and S. Mukamel, J. Chem. Phys. 94, 997 (1991).
    [CrossRef]
  22. J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
    [CrossRef]
  23. A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, M. J. Banet, and K. A. Nelson, in Picosecond and Femtosecond Spectroscopy from Laboratory to Real World, K. A. Nelson, ed., Proc. Soc. Photo-Opt. Instrum. Eng.1209, 185 (1990).
    [CrossRef]

1991 (1)

Y. J. Yan and S. Mukamel, J. Chem. Phys. 94, 997 (1991).
[CrossRef]

1990 (3)

1989 (1)

H. L. Fragnito, J.-Y. Bigot, P. C. Becker, and C. V. Shank, Chem. Phys. Lett. 160, 101 (1989).
[CrossRef]

1988 (6)

R. A. Mathies, C. H. Brito Cruz, W. T. Pollard, and C. V. Shank, Science 240, 777 (1988).
[CrossRef] [PubMed]

J. Chesnoy and A. Mokhtari, Phys. Rev. A 38, 3566 (1988).
[CrossRef] [PubMed]

M. Haner and W. S. Warren, Appl. Phys. Lett. 52, 1458 (1988); W. S. Warren, Science 242, 878 (1988).
[CrossRef] [PubMed]

M. Dantus, M. J. Rosker, and A. H. Zewail, J. Chem. Phys. 89, 6128 (1988); N. F. Scherer, C. Sipes, R. B. Bernstein, and A. H. Zewail, J. Chem. Phys. 92, 5239 (1990).
[CrossRef]

A. M. Weiner, J. P. Heritage, and E. M. Kirschner, J. Opt. Soc. Am. B 5, 1563 (1988).
[CrossRef]

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

1987 (1)

Y.-X. Yan and K. A. Nelson, J. Chem. Phys. 87, 6240, 6257 (1987).
[CrossRef]

1986 (2)

F. W. Wise, M. J. Rosker, and C. L. Tang, J. Chem. Phys. 86, 2827 (1986).
[CrossRef]

D. Tannor, R. Kosloff, and S. A. Rice, J. Chem. Phys. 85, 5805 (1986); S. Shi, A. Woody, and H. Rabitz, J. Chem. Phys. 88, 6870 (1988).
[CrossRef]

1985 (3)

Y.-X. Yan, E. B. Gamble, and K. A. Nelson, J. Chem. Phys. 83, 5391 (1985).
[CrossRef]

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
[CrossRef]

1984 (1)

1983 (1)

T. J. Kosic, C. L. Schosser, and D. D. Dlott, Chem. Phys. Lett. 96, 57 (1983).
[CrossRef]

1981 (1)

R. L. Fork, B. I. Greene, and C. V. Shank, Appl. Phys. Lett. 38, 671 (1981); J. A. Valdmanis, R. L. Fork, and J. P. Gordon, Opt. Lett. 10, 131 (1985).
[CrossRef] [PubMed]

1974 (1)

J. Tanaka, T. Kishi, and M. Tanaka, Bull. Chem. Soc. Jpn. 47, 2376 (1974).
[CrossRef]

Banet, M. J.

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, M. J. Banet, and K. A. Nelson, in Picosecond and Femtosecond Spectroscopy from Laboratory to Real World, K. A. Nelson, ed., Proc. Soc. Photo-Opt. Instrum. Eng.1209, 185 (1990).
[CrossRef]

Becker, P. C.

H. L. Fragnito, J.-Y. Bigot, P. C. Becker, and C. V. Shank, Chem. Phys. Lett. 160, 101 (1989).
[CrossRef]

Bigot, J.-Y.

H. L. Fragnito, J.-Y. Bigot, P. C. Becker, and C. V. Shank, Chem. Phys. Lett. 160, 101 (1989).
[CrossRef]

Brito Cruz, C. H.

R. A. Mathies, C. H. Brito Cruz, W. T. Pollard, and C. V. Shank, Science 240, 777 (1988).
[CrossRef] [PubMed]

Cheng, L.-T.

Y.-X. Yan, L.-T. Cheng, and K. A. Nelson, in Advances in Nonlinear Spectroscopy, R. J. H. Clark and R. E. Hester, eds., Vol. 16 of Advances in Spectroscopy Series (Wiley, Chichester, UK, 1988), pp. 299–355; S. Ruhman, A. G. Joly, B. Kohler, L. R. Williams, and K. A. Nelson, Rev. Phys. Appl. 22, 1717 (1987).
[CrossRef]

Chesnoy, J.

J. Chesnoy and A. Mokhtari, Phys. Rev. A 38, 3566 (1988).
[CrossRef] [PubMed]

Dantus, M.

M. Dantus, M. J. Rosker, and A. H. Zewail, J. Chem. Phys. 89, 6128 (1988); N. F. Scherer, C. Sipes, R. B. Bernstein, and A. H. Zewail, J. Chem. Phys. 92, 5239 (1990).
[CrossRef]

De Silvestri, S.

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

Dlott, D. D.

T. J. Kosic, C. L. Schosser, and D. D. Dlott, Chem. Phys. Lett. 96, 57 (1983).
[CrossRef]

Downer, M. C.

Fork, R. L.

W. H. Knox, M. C. Downer, R. L. Fork, and C. V. Shank, Opt. Lett. 9, 552 (1984).
[CrossRef] [PubMed]

R. L. Fork, B. I. Greene, and C. V. Shank, Appl. Phys. Lett. 38, 671 (1981); J. A. Valdmanis, R. L. Fork, and J. P. Gordon, Opt. Lett. 10, 131 (1985).
[CrossRef] [PubMed]

Fragnito, H. L.

H. L. Fragnito, J.-Y. Bigot, P. C. Becker, and C. V. Shank, Chem. Phys. Lett. 160, 101 (1989).
[CrossRef]

Fujimoto, J. G.

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

Gamble, E. B.

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

Y.-X. Yan, E. B. Gamble, and K. A. Nelson, J. Chem. Phys. 83, 5391 (1985).
[CrossRef]

Greene, B. I.

R. L. Fork, B. I. Greene, and C. V. Shank, Appl. Phys. Lett. 38, 671 (1981); J. A. Valdmanis, R. L. Fork, and J. P. Gordon, Opt. Lett. 10, 131 (1985).
[CrossRef] [PubMed]

Haner, M.

M. Haner and W. S. Warren, Appl. Phys. Lett. 52, 1458 (1988); W. S. Warren, Science 242, 878 (1988).
[CrossRef] [PubMed]

Hawkins, R. J.

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

Heritage, J. P.

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

A. M. Weiner, J. P. Heritage, and E. M. Kirschner, J. Opt. Soc. Am. B 5, 1563 (1988).
[CrossRef]

J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
[CrossRef]

Ippen, E. P.

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

Kirschner, E. M.

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

A. M. Weiner, J. P. Heritage, and E. M. Kirschner, J. Opt. Soc. Am. B 5, 1563 (1988).
[CrossRef]

Kishi, T.

J. Tanaka, T. Kishi, and M. Tanaka, Bull. Chem. Soc. Jpn. 47, 2376 (1974).
[CrossRef]

Knox, W. H.

Kosic, T. J.

T. J. Kosic, C. L. Schosser, and D. D. Dlott, Chem. Phys. Lett. 96, 57 (1983).
[CrossRef]

Kosloff, R.

D. Tannor, R. Kosloff, and S. A. Rice, J. Chem. Phys. 85, 5805 (1986); S. Shi, A. Woody, and H. Rabitz, J. Chem. Phys. 88, 6870 (1988).
[CrossRef]

Leaird, D. E.

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, Opt. Lett. 15, 326 (1990).
[CrossRef]

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, Science 247, 1327 (1990).
[CrossRef]

A. M. Weiner and D. E. Leaird, Opt. Lett. 15, 51 (1990).
[CrossRef] [PubMed]

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, M. J. Banet, and K. A. Nelson, in Picosecond and Femtosecond Spectroscopy from Laboratory to Real World, K. A. Nelson, ed., Proc. Soc. Photo-Opt. Instrum. Eng.1209, 185 (1990).
[CrossRef]

Mathies, R. A.

R. A. Mathies, C. H. Brito Cruz, W. T. Pollard, and C. V. Shank, Science 240, 777 (1988).
[CrossRef] [PubMed]

Mokhtari, A.

J. Chesnoy and A. Mokhtari, Phys. Rev. A 38, 3566 (1988).
[CrossRef] [PubMed]

Mukamel, S.

Y. J. Yan and S. Mukamel, J. Chem. Phys. 94, 997 (1991).
[CrossRef]

Nelson, K. A.

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, Science 247, 1327 (1990).
[CrossRef]

Y.-X. Yan and K. A. Nelson, J. Chem. Phys. 87, 6240, 6257 (1987).
[CrossRef]

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

Y.-X. Yan, E. B. Gamble, and K. A. Nelson, J. Chem. Phys. 83, 5391 (1985).
[CrossRef]

Y.-X. Yan, L.-T. Cheng, and K. A. Nelson, in Advances in Nonlinear Spectroscopy, R. J. H. Clark and R. E. Hester, eds., Vol. 16 of Advances in Spectroscopy Series (Wiley, Chichester, UK, 1988), pp. 299–355; S. Ruhman, A. G. Joly, B. Kohler, L. R. Williams, and K. A. Nelson, Rev. Phys. Appl. 22, 1717 (1987).
[CrossRef]

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, M. J. Banet, and K. A. Nelson, in Picosecond and Femtosecond Spectroscopy from Laboratory to Real World, K. A. Nelson, ed., Proc. Soc. Photo-Opt. Instrum. Eng.1209, 185 (1990).
[CrossRef]

Patel, J. S.

Pollard, W. T.

R. A. Mathies, C. H. Brito Cruz, W. T. Pollard, and C. V. Shank, Science 240, 777 (1988).
[CrossRef] [PubMed]

Rice, S. A.

D. Tannor, R. Kosloff, and S. A. Rice, J. Chem. Phys. 85, 5805 (1986); S. Shi, A. Woody, and H. Rabitz, J. Chem. Phys. 88, 6870 (1988).
[CrossRef]

Rosker, M. J.

M. Dantus, M. J. Rosker, and A. H. Zewail, J. Chem. Phys. 89, 6128 (1988); N. F. Scherer, C. Sipes, R. B. Bernstein, and A. H. Zewail, J. Chem. Phys. 92, 5239 (1990).
[CrossRef]

F. W. Wise, M. J. Rosker, and C. L. Tang, J. Chem. Phys. 86, 2827 (1986).
[CrossRef]

Schosser, C. L.

T. J. Kosic, C. L. Schosser, and D. D. Dlott, Chem. Phys. Lett. 96, 57 (1983).
[CrossRef]

Shank, C. V.

H. L. Fragnito, J.-Y. Bigot, P. C. Becker, and C. V. Shank, Chem. Phys. Lett. 160, 101 (1989).
[CrossRef]

R. A. Mathies, C. H. Brito Cruz, W. T. Pollard, and C. V. Shank, Science 240, 777 (1988).
[CrossRef] [PubMed]

W. H. Knox, M. C. Downer, R. L. Fork, and C. V. Shank, Opt. Lett. 9, 552 (1984).
[CrossRef] [PubMed]

R. L. Fork, B. I. Greene, and C. V. Shank, Appl. Phys. Lett. 38, 671 (1981); J. A. Valdmanis, R. L. Fork, and J. P. Gordon, Opt. Lett. 10, 131 (1985).
[CrossRef] [PubMed]

Stolen, R. H.

J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
[CrossRef]

Tanaka, J.

J. Tanaka, T. Kishi, and M. Tanaka, Bull. Chem. Soc. Jpn. 47, 2376 (1974).
[CrossRef]

Tanaka, M.

J. Tanaka, T. Kishi, and M. Tanaka, Bull. Chem. Soc. Jpn. 47, 2376 (1974).
[CrossRef]

Tang, C. L.

F. W. Wise, M. J. Rosker, and C. L. Tang, J. Chem. Phys. 86, 2827 (1986).
[CrossRef]

Tannor, D.

D. Tannor, R. Kosloff, and S. A. Rice, J. Chem. Phys. 85, 5805 (1986); S. Shi, A. Woody, and H. Rabitz, J. Chem. Phys. 88, 6870 (1988).
[CrossRef]

Thurston, R. N.

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
[CrossRef]

Tomlinson, W. J.

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
[CrossRef]

Warren, W. S.

M. Haner and W. S. Warren, Appl. Phys. Lett. 52, 1458 (1988); W. S. Warren, Science 242, 878 (1988).
[CrossRef] [PubMed]

Weiner, A. M.

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, Science 247, 1327 (1990).
[CrossRef]

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, Opt. Lett. 15, 326 (1990).
[CrossRef]

A. M. Weiner and D. E. Leaird, Opt. Lett. 15, 51 (1990).
[CrossRef] [PubMed]

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

A. M. Weiner, J. P. Heritage, and E. M. Kirschner, J. Opt. Soc. Am. B 5, 1563 (1988).
[CrossRef]

J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
[CrossRef]

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, M. J. Banet, and K. A. Nelson, in Picosecond and Femtosecond Spectroscopy from Laboratory to Real World, K. A. Nelson, ed., Proc. Soc. Photo-Opt. Instrum. Eng.1209, 185 (1990).
[CrossRef]

Wiederrecht, G. P.

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, Science 247, 1327 (1990).
[CrossRef]

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, M. J. Banet, and K. A. Nelson, in Picosecond and Femtosecond Spectroscopy from Laboratory to Real World, K. A. Nelson, ed., Proc. Soc. Photo-Opt. Instrum. Eng.1209, 185 (1990).
[CrossRef]

Williams, L. R.

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

Wise, F. W.

F. W. Wise, M. J. Rosker, and C. L. Tang, J. Chem. Phys. 86, 2827 (1986).
[CrossRef]

Wullert, J. R.

Yan, Y. J.

Y. J. Yan and S. Mukamel, J. Chem. Phys. 94, 997 (1991).
[CrossRef]

Yan, Y.-X.

Y.-X. Yan and K. A. Nelson, J. Chem. Phys. 87, 6240, 6257 (1987).
[CrossRef]

Y.-X. Yan, E. B. Gamble, and K. A. Nelson, J. Chem. Phys. 83, 5391 (1985).
[CrossRef]

Y.-X. Yan, L.-T. Cheng, and K. A. Nelson, in Advances in Nonlinear Spectroscopy, R. J. H. Clark and R. E. Hester, eds., Vol. 16 of Advances in Spectroscopy Series (Wiley, Chichester, UK, 1988), pp. 299–355; S. Ruhman, A. G. Joly, B. Kohler, L. R. Williams, and K. A. Nelson, Rev. Phys. Appl. 22, 1717 (1987).
[CrossRef]

Zewail, A. H.

M. Dantus, M. J. Rosker, and A. H. Zewail, J. Chem. Phys. 89, 6128 (1988); N. F. Scherer, C. Sipes, R. B. Bernstein, and A. H. Zewail, J. Chem. Phys. 92, 5239 (1990).
[CrossRef]

Appl. Phys. Lett. (3)

M. Haner and W. S. Warren, Appl. Phys. Lett. 52, 1458 (1988); W. S. Warren, Science 242, 878 (1988).
[CrossRef] [PubMed]

R. L. Fork, B. I. Greene, and C. V. Shank, Appl. Phys. Lett. 38, 671 (1981); J. A. Valdmanis, R. L. Fork, and J. P. Gordon, Opt. Lett. 10, 131 (1985).
[CrossRef] [PubMed]

J. P. Heritage, R. N. Thurston, W. J. Tomlinson, A. M. Weiner, and R. H. Stolen, Appl. Phys. Lett. 47, 87 (1985).
[CrossRef]

Bull. Chem. Soc. Jpn. (1)

J. Tanaka, T. Kishi, and M. Tanaka, Bull. Chem. Soc. Jpn. 47, 2376 (1974).
[CrossRef]

Chem. Phys. Lett. (3)

T. J. Kosic, C. L. Schosser, and D. D. Dlott, Chem. Phys. Lett. 96, 57 (1983).
[CrossRef]

S. De Silvestri, J. G. Fujimoto, E. P. Ippen, E. B. Gamble, L. R. Williams, and K. A. Nelson, Chem. Phys. Lett. 116, 146 (1985).
[CrossRef]

H. L. Fragnito, J.-Y. Bigot, P. C. Becker, and C. V. Shank, Chem. Phys. Lett. 160, 101 (1989).
[CrossRef]

J. Chem. Phys. (6)

D. Tannor, R. Kosloff, and S. A. Rice, J. Chem. Phys. 85, 5805 (1986); S. Shi, A. Woody, and H. Rabitz, J. Chem. Phys. 88, 6870 (1988).
[CrossRef]

Y.-X. Yan, E. B. Gamble, and K. A. Nelson, J. Chem. Phys. 83, 5391 (1985).
[CrossRef]

F. W. Wise, M. J. Rosker, and C. L. Tang, J. Chem. Phys. 86, 2827 (1986).
[CrossRef]

M. Dantus, M. J. Rosker, and A. H. Zewail, J. Chem. Phys. 89, 6128 (1988); N. F. Scherer, C. Sipes, R. B. Bernstein, and A. H. Zewail, J. Chem. Phys. 92, 5239 (1990).
[CrossRef]

Y.-X. Yan and K. A. Nelson, J. Chem. Phys. 87, 6240, 6257 (1987).
[CrossRef]

Y. J. Yan and S. Mukamel, J. Chem. Phys. 94, 997 (1991).
[CrossRef]

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

Opt. Lett. (3)

Phys. Rev. A (1)

J. Chesnoy and A. Mokhtari, Phys. Rev. A 38, 3566 (1988).
[CrossRef] [PubMed]

Phys. Rev. Lett. (1)

A. M. Weiner, J. P. Heritage, R. J. Hawkins, R. N. Thurston, E. M. Kirschner, D. E. Leaird, and W. J. Tomlinson, Phys. Rev. Lett. 61, 2445 (1988).
[CrossRef] [PubMed]

Science (2)

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, Science 247, 1327 (1990).
[CrossRef]

R. A. Mathies, C. H. Brito Cruz, W. T. Pollard, and C. V. Shank, Science 240, 777 (1988).
[CrossRef] [PubMed]

Other (2)

Y.-X. Yan, L.-T. Cheng, and K. A. Nelson, in Advances in Nonlinear Spectroscopy, R. J. H. Clark and R. E. Hester, eds., Vol. 16 of Advances in Spectroscopy Series (Wiley, Chichester, UK, 1988), pp. 299–355; S. Ruhman, A. G. Joly, B. Kohler, L. R. Williams, and K. A. Nelson, Rev. Phys. Appl. 22, 1717 (1987).
[CrossRef]

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, M. J. Banet, and K. A. Nelson, in Picosecond and Femtosecond Spectroscopy from Laboratory to Real World, K. A. Nelson, ed., Proc. Soc. Photo-Opt. Instrum. Eng.1209, 185 (1990).
[CrossRef]

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Figures (12)

Fig. 1
Fig. 1

Experimental arrangement for multiple-pulse ISRS. (A) Sketch of the transient-grating scattering geometry. (B) Block diagram of the optical setup. CPM

Fig. 2
Fig. 2

Layout of a phase mask, designed to produce pulse trains with repetition rates ranging from 340 to 460 fs. Each individual pattern (from left to right) corresponds to a particular repetition rate. The repetition period is 340 fs at the top and increases by 5 fs per pattern toward the bottom. The shaded regions in the figure correspond to areas that are etched during the fabrication process (to a depth corresponding to a phase change of approximately π). The unshaded regions are not etched during fabrication.

Fig. 3
Fig. 3

Single-pulse ISRS data recorded from α-perylene with T < 10 K and with all pulses linearly polarized parallel to the b crystallographic axis. The femtosecond excitation pulses drive several phonon modes whose combined response yields a characteristic beating pattern. The spike at t = 0 is a purely electronic response of the crystal to the excitation pulses.

Fig. 4
Fig. 4

Solid curve: Fourier transform of the scattering data shown in Fig. 3. The electronic scattering peak at t = 0 in the time-domain data was suppressed before the Fourier transform was performed. Dashed curve: Fourier transform of the electronic scattering peak, representing the instrumental response function.

Fig. 5
Fig. 5

Multiple-pulse ISRS data recorded from α-perylene with T < 10 K and with all pulses linearly polarized parallel to the b crystallographic axis. (A) Intensity cross-correlation measurement of 2.39-THz (79.6-cm−1) pulse train used for resonant excitation of the α-perylene’s 80-cm−1 librational mode. ISRS data (B) for 79.6-cm−1 excitation, (C) for 77.8-cm−1 excitation, (D) for 88.7-cm−1 excitation.

Fig. 6
Fig. 6

Fourier transform of ISRS data, corresponding to resonant excitation of the 80-cm−1 Vibrational mode, as in Fig. 5(B).

Fig. 7
Fig. 7

Multiple-pulse ISRS data, showing decay of the 80-cm−1 at various temperatures. Note that a shorter time scale is used for plots (D) and (E). (A) T = 10 K, (B) T = 20 K, (C) T = 50 K, (D) T = 100 K, (E) T = 295 K.

Fig. 8
Fig. 8

ISRS data for resonant multiple-pulse excitation of the 104-cm−1 vibrational mode in α-perylene. The temperature is T = 10 K. (A) All pulses polarized along the a crystallographic axis. (B) Polarization along the b axis.

Fig. 9
Fig. 9

Simulation results for multiple-pulse excitation of the 80-cm−1 mode in α-perylene. (A) On resonance, 2.39-THz (79.6-cm−1) pulse repetition rate. (B) Detuned from resonance, 2.33-THz (77.8-cm−1) pulse repetition rate.

Fig. 10
Fig. 10

Experimental arrangement for forward (or pump–probe) ISRS experiments with multiple-pulse excitation.

Fig. 11
Fig. 11

Pump–probe ISRS measurements of α-perylene at T = 10 K, in conjunction with resonant multiple-pulse excitation of the 80-cm−1 librational mode. (A) Shortest-wavelength portion of the probe detected. (B) Longest-wavelength portion detected. (C) Entire probe spectrum detected. (D) Sum of (A) and (B). (E) Difference of (A) and (B).

Fig. 12
Fig. 12

Comparison of (A) transient-grating ISRS data and (B) pump–probe ISRS data, both corresponding to resonant excitation of the 80-cm−1 librational mode at T = 10 K. The extrema in the pump–probe data correspond to minima in the diffraction data, and the maxima in the diffraction data correspond to zero crossings of the pump–probe data.

Equations (5)

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I ( x , t ) = n I o exp [ - ( t - n T ) 2 t p 2 - n 2 N p 2 ] cos 2 k x .
G i ( t ) = C i exp ( - γ i t ) sin ω i t ,
Q i ( x , t ) = - t d t I ( t ) G i ( t - t ) .
δ ( x , t ) = i Q i Q i + 2 n 0 γ I ( x , t ) ,
Ψ ( t ) = n = 0 A n n ,

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