Abstract

A simple probing method for obtaining broadband multichannel infrared spectra with picosecond or higher time resolution is described. Spectrally broad infrared pulses are produced by difference frequency mixing in LiIO3 between the second harmonic of a Nd+3: YAG laser and the broadband output of a synchronously pumped dye laser. After sample absorption the infrared pulse is upconverted by a second LiIO3 crystal, which yields a visible pulse that is dispersed on a multichannel vidicon detector to obtain transient spectra of 4-cm−1 FWHM resolution.

© 1989 Optical Society of America

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  1. B. I. Greene, R. M. Hochstrasser, R. B. Weisman, J. Chem. Phys. 70, 1247 (1979).
    [Crossref]
  2. C. V. Shank, R. L. Fork, C. H. Brito Cruz, W. Knox, in Ultrafast Phenomena V, G. R. Fleming, A. E. Siegman, eds. (Springer-Verlag, New York, 1986), pp. 179–181.
  3. H. Graener, R. Dohlus, T. Q. Yeh, A. Laubereau, J. Chem. Phys. 90, 3413 (1989);Chem. Phys. Lett. 140, 306 (1987).
    [Crossref]
  4. J. N. Moore, P. A. Hansen, R. M. Hochstrasser, Chem. Phys. Lett. 138, 110 (1987).
    [Crossref]
  5. D. S. Bethune, A. J. Schell-Sorokin, J. R. Lankard, M. M. T. Loy, P. P. Sorokin, in Advances in Laser Spectroscopy, B. A. Garetz, J. R. Lombardi, eds. (Wiley, New York, 1983), Vol. 2, p. 1.
  6. J. H. Glownia, J. Misewich, P. P. Sorokin, Opt. Lett. 12, 19 (1987);Chem. Phys. Lett. 139, 491 (1987);M. Berg, A. L. Harris, J. K. Brown, C. B. Harris, Opt. Lett. 9, 50 (1984).
    [Crossref] [PubMed]
  7. E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, Chem. Phys. Lett. 134, 181 (1987);J. Phys. Chem. 92, 6099 (1988);J. Chem. Phys. 89, 5342 (1988).
    [Crossref]
  8. C. A. Moore, L. S. Goldberg, Opt. Commun. 16, 21 (1976).
    [Crossref]
  9. L. S. Goldberg, Appl. Opt. 14, 653 (1975).
    [Crossref] [PubMed]
  10. T. J. Jedju, L. Rothberg, Appl. Opt. 26, 2877 (1987).
    [Crossref] [PubMed]
  11. H. J. Hartman, A. Laubereau, Appl. Opt. 20, 4259 (1981).
    [Crossref]
  12. K.-J. Choi, B. P. Bozcar, M. R. Topp, Chem. Phys. 57, 415 (1981).
    [Crossref]
  13. R. Moore, F. E. Doany, E. J. Heilweil, R. M. Hochstrasser, J. Phys. Chem. 88, 876 (1984).
    [Crossref]
  14. E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, J. Chem. Phys. 89, 230 (1988).
    [Crossref]
  15. T. M. Jedju, L. Rothberg, A. Labrie, Opt. Lett. 13, 961 (1988).
    [Crossref] [PubMed]

1989 (1)

H. Graener, R. Dohlus, T. Q. Yeh, A. Laubereau, J. Chem. Phys. 90, 3413 (1989);Chem. Phys. Lett. 140, 306 (1987).
[Crossref]

1988 (2)

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, J. Chem. Phys. 89, 230 (1988).
[Crossref]

T. M. Jedju, L. Rothberg, A. Labrie, Opt. Lett. 13, 961 (1988).
[Crossref] [PubMed]

1987 (4)

J. N. Moore, P. A. Hansen, R. M. Hochstrasser, Chem. Phys. Lett. 138, 110 (1987).
[Crossref]

J. H. Glownia, J. Misewich, P. P. Sorokin, Opt. Lett. 12, 19 (1987);Chem. Phys. Lett. 139, 491 (1987);M. Berg, A. L. Harris, J. K. Brown, C. B. Harris, Opt. Lett. 9, 50 (1984).
[Crossref] [PubMed]

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, Chem. Phys. Lett. 134, 181 (1987);J. Phys. Chem. 92, 6099 (1988);J. Chem. Phys. 89, 5342 (1988).
[Crossref]

T. J. Jedju, L. Rothberg, Appl. Opt. 26, 2877 (1987).
[Crossref] [PubMed]

1984 (1)

R. Moore, F. E. Doany, E. J. Heilweil, R. M. Hochstrasser, J. Phys. Chem. 88, 876 (1984).
[Crossref]

1981 (2)

H. J. Hartman, A. Laubereau, Appl. Opt. 20, 4259 (1981).
[Crossref]

K.-J. Choi, B. P. Bozcar, M. R. Topp, Chem. Phys. 57, 415 (1981).
[Crossref]

1979 (1)

B. I. Greene, R. M. Hochstrasser, R. B. Weisman, J. Chem. Phys. 70, 1247 (1979).
[Crossref]

1976 (1)

C. A. Moore, L. S. Goldberg, Opt. Commun. 16, 21 (1976).
[Crossref]

1975 (1)

Bethune, D. S.

D. S. Bethune, A. J. Schell-Sorokin, J. R. Lankard, M. M. T. Loy, P. P. Sorokin, in Advances in Laser Spectroscopy, B. A. Garetz, J. R. Lombardi, eds. (Wiley, New York, 1983), Vol. 2, p. 1.

Bozcar, B. P.

K.-J. Choi, B. P. Bozcar, M. R. Topp, Chem. Phys. 57, 415 (1981).
[Crossref]

Brito Cruz, C. H.

C. V. Shank, R. L. Fork, C. H. Brito Cruz, W. Knox, in Ultrafast Phenomena V, G. R. Fleming, A. E. Siegman, eds. (Springer-Verlag, New York, 1986), pp. 179–181.

Cavanagh, R. R.

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, J. Chem. Phys. 89, 230 (1988).
[Crossref]

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, Chem. Phys. Lett. 134, 181 (1987);J. Phys. Chem. 92, 6099 (1988);J. Chem. Phys. 89, 5342 (1988).
[Crossref]

Choi, K.-J.

K.-J. Choi, B. P. Bozcar, M. R. Topp, Chem. Phys. 57, 415 (1981).
[Crossref]

Doany, F. E.

R. Moore, F. E. Doany, E. J. Heilweil, R. M. Hochstrasser, J. Phys. Chem. 88, 876 (1984).
[Crossref]

Dohlus, R.

H. Graener, R. Dohlus, T. Q. Yeh, A. Laubereau, J. Chem. Phys. 90, 3413 (1989);Chem. Phys. Lett. 140, 306 (1987).
[Crossref]

Fork, R. L.

C. V. Shank, R. L. Fork, C. H. Brito Cruz, W. Knox, in Ultrafast Phenomena V, G. R. Fleming, A. E. Siegman, eds. (Springer-Verlag, New York, 1986), pp. 179–181.

Glownia, J. H.

Goldberg, L. S.

C. A. Moore, L. S. Goldberg, Opt. Commun. 16, 21 (1976).
[Crossref]

L. S. Goldberg, Appl. Opt. 14, 653 (1975).
[Crossref] [PubMed]

Graener, H.

H. Graener, R. Dohlus, T. Q. Yeh, A. Laubereau, J. Chem. Phys. 90, 3413 (1989);Chem. Phys. Lett. 140, 306 (1987).
[Crossref]

Greene, B. I.

B. I. Greene, R. M. Hochstrasser, R. B. Weisman, J. Chem. Phys. 70, 1247 (1979).
[Crossref]

Hansen, P. A.

J. N. Moore, P. A. Hansen, R. M. Hochstrasser, Chem. Phys. Lett. 138, 110 (1987).
[Crossref]

Hartman, H. J.

Heilweil, E. J.

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, J. Chem. Phys. 89, 230 (1988).
[Crossref]

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, Chem. Phys. Lett. 134, 181 (1987);J. Phys. Chem. 92, 6099 (1988);J. Chem. Phys. 89, 5342 (1988).
[Crossref]

R. Moore, F. E. Doany, E. J. Heilweil, R. M. Hochstrasser, J. Phys. Chem. 88, 876 (1984).
[Crossref]

Hochstrasser, R. M.

J. N. Moore, P. A. Hansen, R. M. Hochstrasser, Chem. Phys. Lett. 138, 110 (1987).
[Crossref]

R. Moore, F. E. Doany, E. J. Heilweil, R. M. Hochstrasser, J. Phys. Chem. 88, 876 (1984).
[Crossref]

B. I. Greene, R. M. Hochstrasser, R. B. Weisman, J. Chem. Phys. 70, 1247 (1979).
[Crossref]

Jedju, T. J.

Jedju, T. M.

Knox, W.

C. V. Shank, R. L. Fork, C. H. Brito Cruz, W. Knox, in Ultrafast Phenomena V, G. R. Fleming, A. E. Siegman, eds. (Springer-Verlag, New York, 1986), pp. 179–181.

Labrie, A.

Lankard, J. R.

D. S. Bethune, A. J. Schell-Sorokin, J. R. Lankard, M. M. T. Loy, P. P. Sorokin, in Advances in Laser Spectroscopy, B. A. Garetz, J. R. Lombardi, eds. (Wiley, New York, 1983), Vol. 2, p. 1.

Laubereau, A.

H. Graener, R. Dohlus, T. Q. Yeh, A. Laubereau, J. Chem. Phys. 90, 3413 (1989);Chem. Phys. Lett. 140, 306 (1987).
[Crossref]

H. J. Hartman, A. Laubereau, Appl. Opt. 20, 4259 (1981).
[Crossref]

Loy, M. M. T.

D. S. Bethune, A. J. Schell-Sorokin, J. R. Lankard, M. M. T. Loy, P. P. Sorokin, in Advances in Laser Spectroscopy, B. A. Garetz, J. R. Lombardi, eds. (Wiley, New York, 1983), Vol. 2, p. 1.

Misewich, J.

Moore, C. A.

C. A. Moore, L. S. Goldberg, Opt. Commun. 16, 21 (1976).
[Crossref]

Moore, J. N.

J. N. Moore, P. A. Hansen, R. M. Hochstrasser, Chem. Phys. Lett. 138, 110 (1987).
[Crossref]

Moore, R.

R. Moore, F. E. Doany, E. J. Heilweil, R. M. Hochstrasser, J. Phys. Chem. 88, 876 (1984).
[Crossref]

Rothberg, L.

Schell-Sorokin, A. J.

D. S. Bethune, A. J. Schell-Sorokin, J. R. Lankard, M. M. T. Loy, P. P. Sorokin, in Advances in Laser Spectroscopy, B. A. Garetz, J. R. Lombardi, eds. (Wiley, New York, 1983), Vol. 2, p. 1.

Shank, C. V.

C. V. Shank, R. L. Fork, C. H. Brito Cruz, W. Knox, in Ultrafast Phenomena V, G. R. Fleming, A. E. Siegman, eds. (Springer-Verlag, New York, 1986), pp. 179–181.

Sorokin, P. P.

J. H. Glownia, J. Misewich, P. P. Sorokin, Opt. Lett. 12, 19 (1987);Chem. Phys. Lett. 139, 491 (1987);M. Berg, A. L. Harris, J. K. Brown, C. B. Harris, Opt. Lett. 9, 50 (1984).
[Crossref] [PubMed]

D. S. Bethune, A. J. Schell-Sorokin, J. R. Lankard, M. M. T. Loy, P. P. Sorokin, in Advances in Laser Spectroscopy, B. A. Garetz, J. R. Lombardi, eds. (Wiley, New York, 1983), Vol. 2, p. 1.

Stephenson, J. C.

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, J. Chem. Phys. 89, 230 (1988).
[Crossref]

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, Chem. Phys. Lett. 134, 181 (1987);J. Phys. Chem. 92, 6099 (1988);J. Chem. Phys. 89, 5342 (1988).
[Crossref]

Topp, M. R.

K.-J. Choi, B. P. Bozcar, M. R. Topp, Chem. Phys. 57, 415 (1981).
[Crossref]

Weisman, R. B.

B. I. Greene, R. M. Hochstrasser, R. B. Weisman, J. Chem. Phys. 70, 1247 (1979).
[Crossref]

Yeh, T. Q.

H. Graener, R. Dohlus, T. Q. Yeh, A. Laubereau, J. Chem. Phys. 90, 3413 (1989);Chem. Phys. Lett. 140, 306 (1987).
[Crossref]

Appl. Opt. (3)

Chem. Phys. (1)

K.-J. Choi, B. P. Bozcar, M. R. Topp, Chem. Phys. 57, 415 (1981).
[Crossref]

Chem. Phys. Lett. (2)

J. N. Moore, P. A. Hansen, R. M. Hochstrasser, Chem. Phys. Lett. 138, 110 (1987).
[Crossref]

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, Chem. Phys. Lett. 134, 181 (1987);J. Phys. Chem. 92, 6099 (1988);J. Chem. Phys. 89, 5342 (1988).
[Crossref]

J. Chem. Phys. (3)

H. Graener, R. Dohlus, T. Q. Yeh, A. Laubereau, J. Chem. Phys. 90, 3413 (1989);Chem. Phys. Lett. 140, 306 (1987).
[Crossref]

B. I. Greene, R. M. Hochstrasser, R. B. Weisman, J. Chem. Phys. 70, 1247 (1979).
[Crossref]

E. J. Heilweil, R. R. Cavanagh, J. C. Stephenson, J. Chem. Phys. 89, 230 (1988).
[Crossref]

J. Phys. Chem. (1)

R. Moore, F. E. Doany, E. J. Heilweil, R. M. Hochstrasser, J. Phys. Chem. 88, 876 (1984).
[Crossref]

Opt. Commun. (1)

C. A. Moore, L. S. Goldberg, Opt. Commun. 16, 21 (1976).
[Crossref]

Opt. Lett. (2)

Other (2)

C. V. Shank, R. L. Fork, C. H. Brito Cruz, W. Knox, in Ultrafast Phenomena V, G. R. Fleming, A. E. Siegman, eds. (Springer-Verlag, New York, 1986), pp. 179–181.

D. S. Bethune, A. J. Schell-Sorokin, J. R. Lankard, M. M. T. Loy, P. P. Sorokin, in Advances in Laser Spectroscopy, B. A. Garetz, J. R. Lombardi, eds. (Wiley, New York, 1983), Vol. 2, p. 1.

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Figures (4)

Fig. 1
Fig. 1

Optical arrangement for broadband IR pulse generation by difference frequency generation in the LiIO3(1) crystal and sum-frequency upconversion back to the visible in LiIO3(2) after sample absorption. Single-shot IR spectra are obtained by dispersing the upconverted blue pulse with spectrograph/OMA detection.

Fig. 2
Fig. 2

Broadband IR pulse spectrum obtained by scanning an IR monochromator (0.5-cm−1 resolution) with a HgCdTe detector at the exit slit and boxcar averager.

Fig. 3
Fig. 3

(a) Upconverted spectrum of the broadband IR pulses after averaging 600 total laser shots (1-min collection time). The single-track spectrum shows upconverted light spanning approximately 40 OMA channels (50 cm−1). (b) Difference spectrum obtained by subtracting two spectra that are similar to that shown in (a).

Fig. 4
Fig. 4

Curve (a): Picosecond broadband IR upconverted spectrum of Co4(CO)12 in n-hexane obtained under the conditions of Fig. 3. The detected wavelengths and corresponding IR frequencies are deduced from the peak absorption frequencies. Curve (b): Fourier-transform IR spectrum of the sample taken at 4-cm−1 resolution (three channels per resolution element). The similarity to curve (a) indicates that the broadband upconversion transient spectral resolution is ∼4 cm−1 and that absolute transmission levels are accurate to within a few percent.

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