Abstract

Rotationally resolved infrared–ultraviolet double-resonance effects have been observed in D2CO vapor by using pulsed radiation from a The infrared laser pumps CO2 laser and a tunable dye laser. D2CO molecules in the ν4 rovibrational band, and subsequent excitation by the dye laser in the 365-nm 410 vibronic band is detected by fluorescence at 420 nm. The results consolidate assignments from high-resolution absorption spectra and yield estimates of rotational-relaxation rates.

© 1980 Optical Society of America

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  1. J. I. Steinfeld, P. L. Houston, “Double-resonance spectroscopy,” in Laser and Coherence Spectroscopy, J. I. Steinfeld, ed. (Plenum, New York, 1978), pp. 1–123.
    [CrossRef]
  2. A. Yogev, Y Haas, Chem. Phys. Lett. 21, 544 (1973).
    [CrossRef]
  3. B. J. Orr, Chem. Phys. Lett. 43, 446 (1976).
    [CrossRef]
  4. I. Burak, T. J. Quelly, J. I. Steinfeld, J. Chem. Phys. 70, 334 (1979).
    [CrossRef]
  5. D. Coffey, C. Yamada, E. Hirota, J. Mol. Spectrosc. 64, 98 (1977).
    [CrossRef]
  6. T. Nakagawa, University of Tokyo, Tokyo, Japan, personal communication (1976).
  7. B. J. Orr, J. W. C. Johns, unpublished infrared absorption spectrum of D2CO vapor, recorded with a resolution of ~0.05 cm−1 in the 9–11-μm spectral region.
  8. B. J. Orr, Spectrochim. Acta 30A, 1275 (1975).
  9. J. C. D. Brand, J. Chem. Soc. 858 (1956).
  10. E. S. Yeung, C. B. Moore, J. Chem. Phys. 58, 3988 (1973).
    [CrossRef]
  11. R. G. Miller, E. K. C. Lee, Chem. Phys. Lett. 41, 52 (1976); J. Chem. Phys. 68, 4448 (1978).
    [CrossRef]
  12. D. Dangoisse, A. Deldalle, J. P. Splingard, J. Bellet, IEEE J. Quantum Electron. Q-E 13, 730 (1977).
    [CrossRef]
  13. E. S. Yeung, C. B. Moore, Appl. Phys. Lett. 21, 109 (1972); R. V. Ambartsumyan, V. M. Apatin, V. S. Letokhov, V. I. Mishin, Sov. J. Quantum Electron. 5, 191 (1975); J. Marling, J. Chem. Phys. 66, 4200 (1977).
    [CrossRef]
  14. G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
    [CrossRef]
  15. We use the notation JKaKc for the rotational levels of a near-prolate asymmetric rotor.
  16. T. Oka, J. Chem. Phys. 47, 13 (1967); Adv. At. Mol. Phys. 9, 127 (1973).
    [CrossRef]
  17. M. Takami, K. Shimoda, Jpn. J. Appl. Phys. 11, 1648 (1972).
    [CrossRef]
  18. V. Prakash, J. E. Boggs, J. Chem. Phys. 57, 2599 (1972).
    [CrossRef]

1979

I. Burak, T. J. Quelly, J. I. Steinfeld, J. Chem. Phys. 70, 334 (1979).
[CrossRef]

1977

D. Coffey, C. Yamada, E. Hirota, J. Mol. Spectrosc. 64, 98 (1977).
[CrossRef]

D. Dangoisse, A. Deldalle, J. P. Splingard, J. Bellet, IEEE J. Quantum Electron. Q-E 13, 730 (1977).
[CrossRef]

1976

G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
[CrossRef]

B. J. Orr, Chem. Phys. Lett. 43, 446 (1976).
[CrossRef]

R. G. Miller, E. K. C. Lee, Chem. Phys. Lett. 41, 52 (1976); J. Chem. Phys. 68, 4448 (1978).
[CrossRef]

1975

B. J. Orr, Spectrochim. Acta 30A, 1275 (1975).

1973

E. S. Yeung, C. B. Moore, J. Chem. Phys. 58, 3988 (1973).
[CrossRef]

A. Yogev, Y Haas, Chem. Phys. Lett. 21, 544 (1973).
[CrossRef]

1972

E. S. Yeung, C. B. Moore, Appl. Phys. Lett. 21, 109 (1972); R. V. Ambartsumyan, V. M. Apatin, V. S. Letokhov, V. I. Mishin, Sov. J. Quantum Electron. 5, 191 (1975); J. Marling, J. Chem. Phys. 66, 4200 (1977).
[CrossRef]

M. Takami, K. Shimoda, Jpn. J. Appl. Phys. 11, 1648 (1972).
[CrossRef]

V. Prakash, J. E. Boggs, J. Chem. Phys. 57, 2599 (1972).
[CrossRef]

1967

T. Oka, J. Chem. Phys. 47, 13 (1967); Adv. At. Mol. Phys. 9, 127 (1973).
[CrossRef]

1956

J. C. D. Brand, J. Chem. Soc. 858 (1956).

Bellet, J.

D. Dangoisse, A. Deldalle, J. P. Splingard, J. Bellet, IEEE J. Quantum Electron. Q-E 13, 730 (1977).
[CrossRef]

Boggs, J. E.

V. Prakash, J. E. Boggs, J. Chem. Phys. 57, 2599 (1972).
[CrossRef]

Brand, J. C. D.

J. C. D. Brand, J. Chem. Soc. 858 (1956).

Burak, I.

I. Burak, T. J. Quelly, J. I. Steinfeld, J. Chem. Phys. 70, 334 (1979).
[CrossRef]

Coffey, D.

D. Coffey, C. Yamada, E. Hirota, J. Mol. Spectrosc. 64, 98 (1977).
[CrossRef]

Dangoisse, D.

D. Dangoisse, A. Deldalle, J. P. Splingard, J. Bellet, IEEE J. Quantum Electron. Q-E 13, 730 (1977).
[CrossRef]

Deldalle, A.

D. Dangoisse, A. Deldalle, J. P. Splingard, J. Bellet, IEEE J. Quantum Electron. Q-E 13, 730 (1977).
[CrossRef]

Haas, Y

A. Yogev, Y Haas, Chem. Phys. Lett. 21, 544 (1973).
[CrossRef]

Hirota, E.

D. Coffey, C. Yamada, E. Hirota, J. Mol. Spectrosc. 64, 98 (1977).
[CrossRef]

Houston, P. L.

J. I. Steinfeld, P. L. Houston, “Double-resonance spectroscopy,” in Laser and Coherence Spectroscopy, J. I. Steinfeld, ed. (Plenum, New York, 1978), pp. 1–123.
[CrossRef]

Johns, J. W. C.

B. J. Orr, J. W. C. Johns, unpublished infrared absorption spectrum of D2CO vapor, recorded with a resolution of ~0.05 cm−1 in the 9–11-μm spectral region.

Koren, G.

G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
[CrossRef]

Lee, E. K. C.

R. G. Miller, E. K. C. Lee, Chem. Phys. Lett. 41, 52 (1976); J. Chem. Phys. 68, 4448 (1978).
[CrossRef]

Miller, R. G.

R. G. Miller, E. K. C. Lee, Chem. Phys. Lett. 41, 52 (1976); J. Chem. Phys. 68, 4448 (1978).
[CrossRef]

Moore, C. B.

E. S. Yeung, C. B. Moore, J. Chem. Phys. 58, 3988 (1973).
[CrossRef]

E. S. Yeung, C. B. Moore, Appl. Phys. Lett. 21, 109 (1972); R. V. Ambartsumyan, V. M. Apatin, V. S. Letokhov, V. I. Mishin, Sov. J. Quantum Electron. 5, 191 (1975); J. Marling, J. Chem. Phys. 66, 4200 (1977).
[CrossRef]

Nakagawa, T.

T. Nakagawa, University of Tokyo, Tokyo, Japan, personal communication (1976).

Oka, T.

T. Oka, J. Chem. Phys. 47, 13 (1967); Adv. At. Mol. Phys. 9, 127 (1973).
[CrossRef]

Okon, M.

G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
[CrossRef]

Oppenheim, U. P.

G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
[CrossRef]

Orr, B. J.

B. J. Orr, Chem. Phys. Lett. 43, 446 (1976).
[CrossRef]

B. J. Orr, Spectrochim. Acta 30A, 1275 (1975).

B. J. Orr, J. W. C. Johns, unpublished infrared absorption spectrum of D2CO vapor, recorded with a resolution of ~0.05 cm−1 in the 9–11-μm spectral region.

Prakash, V.

V. Prakash, J. E. Boggs, J. Chem. Phys. 57, 2599 (1972).
[CrossRef]

Quelly, T. J.

I. Burak, T. J. Quelly, J. I. Steinfeld, J. Chem. Phys. 70, 334 (1979).
[CrossRef]

Shimoda, K.

M. Takami, K. Shimoda, Jpn. J. Appl. Phys. 11, 1648 (1972).
[CrossRef]

Splingard, J. P.

D. Dangoisse, A. Deldalle, J. P. Splingard, J. Bellet, IEEE J. Quantum Electron. Q-E 13, 730 (1977).
[CrossRef]

Steinfeld, J. I.

I. Burak, T. J. Quelly, J. I. Steinfeld, J. Chem. Phys. 70, 334 (1979).
[CrossRef]

J. I. Steinfeld, P. L. Houston, “Double-resonance spectroscopy,” in Laser and Coherence Spectroscopy, J. I. Steinfeld, ed. (Plenum, New York, 1978), pp. 1–123.
[CrossRef]

Takami, M.

M. Takami, K. Shimoda, Jpn. J. Appl. Phys. 11, 1648 (1972).
[CrossRef]

Tal, D.

G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
[CrossRef]

Weil, R.

G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
[CrossRef]

Yamada, C.

D. Coffey, C. Yamada, E. Hirota, J. Mol. Spectrosc. 64, 98 (1977).
[CrossRef]

Yeung, E. S.

E. S. Yeung, C. B. Moore, J. Chem. Phys. 58, 3988 (1973).
[CrossRef]

E. S. Yeung, C. B. Moore, Appl. Phys. Lett. 21, 109 (1972); R. V. Ambartsumyan, V. M. Apatin, V. S. Letokhov, V. I. Mishin, Sov. J. Quantum Electron. 5, 191 (1975); J. Marling, J. Chem. Phys. 66, 4200 (1977).
[CrossRef]

Yogev, A.

A. Yogev, Y Haas, Chem. Phys. Lett. 21, 544 (1973).
[CrossRef]

Appl. Phys. Lett.

E. S. Yeung, C. B. Moore, Appl. Phys. Lett. 21, 109 (1972); R. V. Ambartsumyan, V. M. Apatin, V. S. Letokhov, V. I. Mishin, Sov. J. Quantum Electron. 5, 191 (1975); J. Marling, J. Chem. Phys. 66, 4200 (1977).
[CrossRef]

G. Koren, U. P. Oppenheim, D. Tal, M. Okon, R. Weil, Appl. Phys. Lett. 29, 40 (1976); G. Koren, M. Okon, U. P. Oppenheim, Opt. Commun. 22, 351 (1977); G. Koren, U. P. Oppenheim, “Multiphoton dissociation in formaldehyde,” in Laser-Induced Processes in Molecules, K. L. Kompa, S. D.Smith Smith, eds. (Springer-Verlag, Berlin, 1979), pp. 209–212.
[CrossRef]

Chem. Phys. Lett.

R. G. Miller, E. K. C. Lee, Chem. Phys. Lett. 41, 52 (1976); J. Chem. Phys. 68, 4448 (1978).
[CrossRef]

A. Yogev, Y Haas, Chem. Phys. Lett. 21, 544 (1973).
[CrossRef]

B. J. Orr, Chem. Phys. Lett. 43, 446 (1976).
[CrossRef]

IEEE J. Quantum Electron.

D. Dangoisse, A. Deldalle, J. P. Splingard, J. Bellet, IEEE J. Quantum Electron. Q-E 13, 730 (1977).
[CrossRef]

J. Chem. Phys.

T. Oka, J. Chem. Phys. 47, 13 (1967); Adv. At. Mol. Phys. 9, 127 (1973).
[CrossRef]

V. Prakash, J. E. Boggs, J. Chem. Phys. 57, 2599 (1972).
[CrossRef]

I. Burak, T. J. Quelly, J. I. Steinfeld, J. Chem. Phys. 70, 334 (1979).
[CrossRef]

E. S. Yeung, C. B. Moore, J. Chem. Phys. 58, 3988 (1973).
[CrossRef]

J. Chem. Soc.

J. C. D. Brand, J. Chem. Soc. 858 (1956).

J. Mol. Spectrosc.

D. Coffey, C. Yamada, E. Hirota, J. Mol. Spectrosc. 64, 98 (1977).
[CrossRef]

Jpn. J. Appl. Phys.

M. Takami, K. Shimoda, Jpn. J. Appl. Phys. 11, 1648 (1972).
[CrossRef]

Spectrochim. Acta

B. J. Orr, Spectrochim. Acta 30A, 1275 (1975).

Other

J. I. Steinfeld, P. L. Houston, “Double-resonance spectroscopy,” in Laser and Coherence Spectroscopy, J. I. Steinfeld, ed. (Plenum, New York, 1978), pp. 1–123.
[CrossRef]

T. Nakagawa, University of Tokyo, Tokyo, Japan, personal communication (1976).

B. J. Orr, J. W. C. Johns, unpublished infrared absorption spectrum of D2CO vapor, recorded with a resolution of ~0.05 cm−1 in the 9–11-μm spectral region.

We use the notation JKaKc for the rotational levels of a near-prolate asymmetric rotor.

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Figures (3)

Fig. 1
Fig. 1

Excitation scheme for infrared–ultraviolet double resonance (IRUVDR). Levels 0 and 1 are specific rotational–vibrational levels of the ground electronic state, and level 2 belongs to an excited vibronic state of the molecule.

Fig. 2
Fig. 2

(a) Portion of a high-resolution absorption spectrogram of D2CO vapor in the vicinity of the 365-nm 410 band origin (labeled O). (b) Excitation spectrum of D2CO vapor (pressure ~5 mTorr), showing IRUVDR peaks produced by pumping with the 10.8-μm P(36) The dye-CO2 laser line. laser pulse was delayed by 0.8 ± 0.1 μsec with respect to the CO2 laser pulse in obtaining this trace (c) Background excitation spectrum (infrared laser off), corresponding to (b), that is due to thermal population of the 41 vibrational level. Assignment of the spectral features labeled A, B, C, D, and H is discussed in the text. The wavelength scale applies precisely only to traces (b) and (c), which were obtained with a scan rate of 0.5 nm min−1 and an instrumental time constant of 3 sec.

Fig. 3
Fig. 3

Effect of dye-laser delay time on the 365.62-nm (C + D) IRUVDR feature of D2CO, obtained with the 10.8-μm P(36) CO2 laser line. The delay times between dye-laser pulse and CO2 laser pulse are as indicated on the figure. Other conditions are: D2 CO pressure, 5 mTorr; time delay jitter, ~ ±0.2 μsec; dye-laser scan rate, 1.4 nm min−1; time constant, 3 sec. A background trace (infrared laser off) is shown as a broken curve immediately below the 2.4-μsec trace.

Equations (1)

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A , 9 2 , 8 8 1 , 7 at 27381.650 cm - 1 ( 365.208 nm ) ; B , 8 2 , 6 8 1 , 7 at 27366.947 cm - 1 ( 365.404 nm ) ; C , 7 2 , 6 8 1 , 7 at 27351.998 cm - 1 ( 365.604 nm ) ; D , 8 0 , 8 8 1 , 7 at 27350.498 cm - 1 ( 365.624 nm ) .

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