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Volumn 108, Issue 7, 2004, Pages 1275-1289

Hydrogen bond dynamics in water and ultrafast infrared spectroscopy: A theoretical study

Author keywords

[No Author keywords available]

Indexed keywords

GROUND STATE; HYDROGEN BONDS; INFRARED SPECTROSCOPY; MOLECULAR VIBRATIONS; SOLVENTS; ULTRAFAST PHENOMENA; WATER;

EID: 1442312825     PISSN: 10895639     EISSN: None     Source Type: Journal    
DOI: 10.1021/jp035935r     Document Type: Article
Times cited : (249)

References (109)
  • 21
    • 1442280243 scopus 로고    scopus 로고
    • note
    • These considerations are over and above the point that the experiments of refs 5 and 6 represent average measurements, rather than, e.g., single molecule experiments.
  • 27
    • 0037035158 scopus 로고    scopus 로고
    • note
    • In this connection it is of interest to note that underdamped H-bond motion is assumed in the theoretical work of one of us on proton-transfer reactions, in solution (see e.g.: Kiefer, P. M.; Hynes, J. T. J. Phys. Chem. A 2002, 106, 1850)
    • (2002) J. Phys. Chem. A , vol.106 , pp. 1850
    • Kiefer, P.M.1    Hynes, J.T.2
  • 30
    • 1442353665 scopus 로고    scopus 로고
    • note
    • For reasons that will become evident in Section 4.1, we do not analyze the velocity correlation function in Figure 2 in terms of any model such as a Brownian oscillator model. We will comment on such models for a different correlation function in Section 4.2.
  • 53
    • 1442304813 scopus 로고    scopus 로고
    • note
    • In using this Coulombic terminology, we are of course here dealing with the given description in terms of short range and Coulombic forces, and not the more fundamental issue of the electronic character of the H bond (see e.g. refs 44 and 45 and references therein)
  • 56
    • 1442353663 scopus 로고    scopus 로고
    • note
    • More precisely, the appropriate combination of the electric fields at the charge sites for OH.
  • 62
    • 1442329239 scopus 로고    scopus 로고
    • note
    • Indeed, this approach has been followed in ref 49 for the frequency correlation function; we comment further on this in Sections 4.2 and 5.
  • 63
    • 0141432008 scopus 로고    scopus 로고
    • note
    • Fecko, C. J.; Eaves, J. D.; Loparo, J. J.; Tokmakoff, A.; Geissler, P. L. Science 2003, 301, 1698. We thank the authors for sending us a preprint of this paper, received after the work described in the present article was completed.
    • (2003) Science , vol.301 , pp. 1698
    • Fecko, C.J.1    Eaves, J.D.2    Loparo, J.J.3    Tokmakoff, A.4    Geissler, P.L.5
  • 65
    • 1442280238 scopus 로고    scopus 로고
    • note
    • -1).
  • 72
    • 1442353669 scopus 로고    scopus 로고
    • note
    • A related conclusion from a different perspective has been reached in ref 49.
  • 73
    • 1442329232 scopus 로고    scopus 로고
    • note
    • The numbers quoted here are slightly different from those reported in ref 16 due to a changed fitting procedure.
  • 75
    • 1442353670 scopus 로고    scopus 로고
    • note
    • eq is the equilibrium separation for an intact H-bonded species, is divergent on longer time scales for the same reason.
  • 78
    • 1442329238 scopus 로고
    • Ratajczak, H., Orville-Thomas, W. J., Eds.; John Wiley and Sons: New York
    • Bratos, S.; Lascombe, J.; Novak, A. In The Hydrogen Bond; Ratajczak, H., Orville-Thomas, W. J., Eds.; John Wiley and Sons: New York, 1980.
    • (1980) The Hydrogen Bond
    • Bratos, S.1    Lascombe, J.2    Novak, A.3
  • 84
    • 33751500687 scopus 로고
    • note
    • Klippenstein, S. K.; Hynes, J. T. J. Phys. Chem. 1991, 95, 4651. In view of our results concerning the OO distance for H-bonded pairs in Section 4 and our remarks concerning the electric field in Section 2.5.2, a more orthogonal partitioning than was employed in this reference might prove useful.
    • (1991) J. Phys. Chem. , vol.95 , pp. 4651
    • Klippenstein, S.K.1    Hynes, J.T.2
  • 88
    • 1442329234 scopus 로고    scopus 로고
    • note
    • R′(t) restricted to H-bonded pairs is invalid. We also note here that the reason that no such modeling for the OO velocity correlation func tion in Figure 2 was done (see ref 24) is that this function has longer time contributions from dissociating trajectories; thus, a bound oscillator should have zero time area for this correlation function, but that of Figure 2 has a finite area.
  • 89
    • 1442280240 scopus 로고    scopus 로고
    • note
    • 2O, see ref 69.
  • 96
    • 1442353673 scopus 로고    scopus 로고
    • note
    • -1 has been reported in ref 7. We emphasize that we are here examining the hole dynamics governed exclusively by the ground OH vibrational state dynamics. The Stokes shift would involve investigation of the difference of the average O → 1 bleaching frequency and the 1 → 0 emission frequency after the pump, with the latter occurring with the vibrationally excited OH state dynamics. While one could consider assorted models for this exploiting the analogy between vibrational states and electronic states and adopting models for e.g., different average OH dipole moments in the ground and excited vibrational states to make contact with treatments of electronic Stokes shifts, we do not pursue this here.
  • 101
    • 1442304809 scopus 로고    scopus 로고
    • note
    • Lawrence and Skinner, in an examination of the four point and two point correlation functions of the fluctuating OH frequency, conclude that while the OH frequency is not Gaussian, "this approximation could still lead to fairly accurate results".
  • 102
    • 1442304811 scopus 로고    scopus 로고
    • note
    • -2, but this only applies for about 15 fs, during which C(t) has decayed by only about 15%.
  • 103
    • 1442304814 scopus 로고    scopus 로고
    • note
    • On the other hand, the Gaussian spectrum shown in Figure 19 is a good representation of the density-of-states histogram in Figure 6.
  • 104
    • 1442329231 scopus 로고    scopus 로고
    • note
    • The distinction between thermal H-bond breaking and vibrational predissociation is evidently not always appreciated.
  • 105
    • 33947462781 scopus 로고
    • note
    • Thus, attention to the various H-bonding issues discussed within might prove of value in analyzing e.g. time-dependent fluorescence solvation dynamics in aqueous systems. In this connection, see also: Pimentel, G. C. J. Am. Chem. Soc. 1957, 79, 3323.
    • (1957) J. Am. Chem. Soc. , vol.79 , pp. 3323
    • Pimentel, G.C.1


* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.