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Volumn 113, Issue 21, 2000, Pages 9488-9496

Nonlinear wavepacket interferometry for polyatomic molecules

Author keywords

[No Author keywords available]

Indexed keywords

CONFORMATIONS; GROUND STATE; HAMILTONIANS; INTERFEROMETRY; MOLECULAR VIBRATIONS; MOLECULES;

EID: 0034499563     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.1319873     Document Type: Article
Times cited : (44)

References (53)
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    • See Secs. III.B, IV.D, and V of Ref. 2
    • See Secs. III.B, IV.D, and V of Ref. 2.
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    • The discrimination against the A- and B-term three-pulse reference packets relative to those of the C- and D-terms could be made to operate in the opposite way by shifting the carrier frequency for pulses 3 and 4 well to the red of the absorption maximum
    • The discrimination against the A- and B-term three-pulse reference packets relative to those of the C- and D-terms could be made to operate in the opposite way by shifting the carrier frequency for pulses 3 and 4 well to the red of the absorption maximum.
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    • We should be aware, however, that this limit begins to militate against spectral elimination of the A- and B-term overlaps
    • We should be aware, however, that this limit begins to militate against spectral elimination of the A- and B-term overlaps.
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    • note
    • d is the relative optical phase between pulses 3 and 4 at the locking frequency Ωd, and φ is an arbitrary overall phase for those two pulses, which does not affect the interference signal [see Eq. (2)].
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    • Shen and Cina (Ref. 23) recently obtained approximate closed-form expressions for the effect of frequency-chirp on the position and momentum moments of a short-pulse excited wavepacket that will be useful in shaping the preparation pulses
    • Shen and Cina (Ref. 23) recently obtained approximate closed-form expressions for the effect of frequency-chirp on the position and momentum moments of a short-pulse excited wavepacket that will be useful in shaping the preparation pulses.
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    • Equations (3.8) and Eq. (3.13) of Ref. 2 give the interference contribution to photon absorption in terms of the vibronic transition energies and Franck-Condon factors; these equations would apply to either fluorescence excitation or transmission loss
    • Equations (3.8) and Eq. (3.13) of Ref. 2 give the interference contribution to photon absorption in terms of the vibronic transition energies and Franck-Condon factors; these equations would apply to either fluorescence excitation or transmission loss.
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    • note
    • d) to the interference population; the finite spectral range of the pulses prohibits the complete determination of the system's response." The claim inaccurately attributed to the original analysis would also contradict expressions (3.24) and (3.23) of paper 2 for the experimentally derived dispersive and absorptive susceptibility components, both of which contain pulse-envelope-modulated vibronic transition moments. That these two quantities are related by a (formally reciprocal) Kramers-Kronig transformation is evident from their parallel structure with the complete e ← g susceptibilities [(3.20) and (3.19) or Ref. 2]. Each of the susceptibility components assembled from the measured phase-locked transients according to the prescriptions (3.24) and (3.23) has the same form as the corresponding component of the full susceptibility, but with envelope-modulated vibronic transition moments replacing the ordinary Franck-Condon factors.
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    • I. Pastirk, E. J. Brown, B. I. Grimberg, V. V. Lozovoy, and M. Dantus, Faraday Discuss. 113, 401 (1999); E. J. Brown, Q. Zhang, and M. Dantus, J. Chem. Phys. 110, 5772 (1999); and I. Pastirk, V. V. Lozovoy, B. I. Grimberg, E. J. Brown, and M. Dantus, J. Phys. Chem. A 103, 10226 (1999). The effects of pulse timing on homodyne-detected degenerate four-wave mixing signals - proportional to the square of the phase-matched component of the third-order induced polarization - are detailed by V. V. Lozovoy, I. Pastirk, E. J. Brown, B. I. Grimberg, and M. Dantus, Int. Rev. Phys. Chem. (in press).
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    • I. Pastirk, E. J. Brown, B. I. Grimberg, V. V. Lozovoy, and M. Dantus, Faraday Discuss. 113, 401 (1999); E. J. Brown, Q. Zhang, and M. Dantus, J. Chem. Phys. 110, 5772 (1999); and I. Pastirk, V. V. Lozovoy, B. I. Grimberg, E. J. Brown, and M. Dantus, J. Phys. Chem. A 103, 10226 (1999). The effects of pulse timing on homodyne-detected degenerate four-wave mixing signals - proportional to the square of the phase-matched component of the third-order induced polarization - are detailed by V. V. Lozovoy, I. Pastirk, E. J. Brown, B. I. Grimberg, and M. Dantus, Int. Rev. Phys. Chem. (in press).
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    • I. Pastirk, E. J. Brown, B. I. Grimberg, V. V. Lozovoy, and M. Dantus, Faraday Discuss. 113, 401 (1999); E. J. Brown, Q. Zhang, and M. Dantus, J. Chem. Phys. 110, 5772 (1999); and I. Pastirk, V. V. Lozovoy, B. I. Grimberg, E. J. Brown, and M. Dantus, J. Phys. Chem. A 103, 10226 (1999). The effects of pulse timing on homodyne-detected degenerate four-wave mixing signals - proportional to the square of the phase-matched component of the third-order induced polarization - are detailed by V. V. Lozovoy, I. Pastirk, E. J. Brown, B. I. Grimberg, and M. Dantus, Int. Rev. Phys. Chem. (in press).
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    • in press
    • I. Pastirk, E. J. Brown, B. I. Grimberg, V. V. Lozovoy, and M. Dantus, Faraday Discuss. 113, 401 (1999); E. J. Brown, Q. Zhang, and M. Dantus, J. Chem. Phys. 110, 5772 (1999); and I. Pastirk, V. V. Lozovoy, B. I. Grimberg, E. J. Brown, and M. Dantus, J. Phys. Chem. A 103, 10226 (1999). The effects of pulse timing on homodyne-detected degenerate four-wave mixing signals - proportional to the square of the phase-matched component of the third-order induced polarization - are detailed by V. V. Lozovoy, I. Pastirk, E. J. Brown, B. I. Grimberg, and M. Dantus, Int. Rev. Phys. Chem. (in press).
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    • note
    • 2), or vice versa, does not seem to have been noted previously. But some spectral-selection arguments are made in Refs. 38 (see Fig. 5 of the last article listed, for example).
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    • The arguments in the Appendix are reminiscent of conditions for vibrational mode suppression in photo-echo experiments identified by C. J. Bardeen and C. V. Shank, Chem. Phys. Lett. 203, 535 (1993).
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    • It is worth noting, however, that if nonlinear wavepacket interferometry experiments were used to monitor excited-state intramolecular vibrational wavefunctions of solvated species, inhomogeneous broadening could help suppress the D-(and A-) terms relative to C (and B); see Chap. 10 of Ref. 20
    • It is worth noting, however, that if nonlinear wavepacket interferometry experiments were used to monitor excited-state intramolecular vibrational wavefunctions of solvated species, inhomogeneous broadening could help suppress the D-(and A-) terms relative to C (and B); see Chap. 10 of Ref. 20.
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    • See also J. A. Cina and R. A. Harris, Ultrafast Phenomena IX, edited by W. Knox and P. Barbara (Springer-Verlag, Berlin, 1994), p. 486; C. S. Maierle and R. A. Harris, J. Chem. Phys. 109, 3713 (1998). For an up-to-date survey of work addressing the preparation and measurement of molecular superposition states, see C. S. Maierle, Ph.D. dissertation, University of California at Berkeley, 1999.
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    • Ph.D. dissertation, University of California at Berkeley
    • See also J. A. Cina and R. A. Harris, Ultrafast Phenomena IX, edited by W. Knox and P. Barbara (Springer-Verlag, Berlin, 1994), p. 486; C. S. Maierle and R. A. Harris, J. Chem. Phys. 109, 3713 (1998). For an up-to-date survey of work addressing the preparation and measurement of molecular superposition states, see C. S. Maierle, Ph.D. dissertation, University of California at Berkeley, 1999.
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  • 52
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    • Forthcoming numerical calculations by R. P. Duarte-Zamorano and V. Romero-Rochín explore the effects of nonzero pulse duration in the model of Ref. 6 and quantify the limits of validity of various approximations used in that study
    • Forthcoming numerical calculations by R. P. Duarte-Zamorano and V. Romero-Rochín explore the effects of nonzero pulse duration in the model of Ref. 6 and quantify the limits of validity of various approximations used in that study.
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    • and references therein
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