Frequency shifts in the hydrogen-bonded OH stretch in halide - water clusters. The importance of charge transfer

Journal of the American Chemical Society

Volumn 122, Issue 26, 2000, Pages 6278-6286

  Thompson, Ward H ^a   Hynes, James T ^a,b  

^a UNIVERSITY OF COLORADO   (United States)

^b ECOLE NORMALE SUPÉRIEURE   (France)

Author keywords

[No Author keywords available]

Indexed keywords

HALIDE; WATER;

ARTICLE; BINDING AFFINITY; CHEMICAL BINDING; HYDROGEN BOND; MATHEMATICAL MODEL; PHASE TRANSITION; STRUCTURE ANALYSIS;

EID: 0034608960     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja993058q     Document Type: Article

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60. All ab initio calculations reported in this paper, with the exception of the natural bond orbital analysis, were carried out using the GAMESS package. Schmidt, M. W.; Baldridge, K. K.; Boatz, J. A.; Elbert, S. T.; Gordon, M. S.; Jensen, J. H.; Koseki, S.; Matsunaga, N.; Nguyen, K. A.; Su., S. J.; Windus, T. L.; Dupuis, M.; Montgomery, J. A. J. Comput. Chem. 1993, 14, 1347-1363. The natural bond orbital analysis (NBO Version 3.1, Glendening, E. D.; Reed, A. E.; Carpenter, J. E.; Weinhold, F.) was carried out using Gaussian 98, Revision A.6, (Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Zakrzewski, V. G.; Montgomery, J. A., Jr.; Stratmann, R. E.; Burant, J. C.; Dapprich, S.; Millam, J. M.; Daniels, A. D.; Kudin, K. N.; Strain, M. C.; Farkas, O.; Tomasi, J.; Barone, V.; Cossi, M.; Cammi, R.; Mennucci, B.; Pomelli, C.; Adamo, C.; Clifford, S.; Ochterski, J.; Petersson, G. A.; Ayala, P. Y.; Cui, Q.; Morokuma, K.; Malick, D. K.; Rabuck, A. D.; Raghavachari, K.; Foresman, J. B.; Cioslowski, J.; Ortiz, J. V.; Stefanov, B. B.; Liu, G.; Liashenko, A.; Piskorz, P.; Komaromi, I.; Gomperts, R.; Martin, R. L.; Fox, D. J.; Keith, T.; Al-Laham, M. A.; Peng, C. Y.; Nanayakkara, A.; Gonzalez, C.; Challacombe, M.; Gill, P M. W.; Johnson, B.; Chen, W.; Wong, M. W.; Andres, J. L.; Gonzalez, C.; Head-Gordon, M.; Replogle, E. S.; Pople, J. A. Gaussian 98, Revision A.6; Gaussian, Inc.: Pittsburgh, PA, 1998).
61. All ab initio calculations reported in this paper, with the exception of the natural bond orbital analysis, were carried out using the GAMESS package. Schmidt, M. W.; Baldridge, K. K.; Boatz, J. A.; Elbert, S. T.; Gordon, M. S.; Jensen, J. H.; Koseki, S.; Matsunaga, N.; Nguyen, K. A.; Su., S. J.; Windus, T. L.; Dupuis, M.; Montgomery, J. A. J. Comput. Chem. 1993, 14, 1347-1363. The natural bond orbital analysis (NBO Version 3.1, Glendening, E. D.; Reed, A. E.; Carpenter, J. E.; Weinhold, F.) was carried out using Gaussian 98, Revision A.6, (Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Zakrzewski, V. G.; Montgomery, J. A., Jr.; Stratmann, R. E.; Burant, J. C.; Dapprich, S.; Millam, J. M.; Daniels, A. D.; Kudin, K. N.; Strain, M. C.; Farkas, O.; Tomasi, J.; Barone, V.; Cossi, M.; Cammi, R.; Mennucci, B.; Pomelli, C.; Adamo, C.; Clifford, S.; Ochterski, J.; Petersson, G. A.; Ayala, P. Y.; Cui, Q.; Morokuma, K.; Malick, D. K.; Rabuck, A. D.; Raghavachari, K.; Foresman, J. B.; Cioslowski, J.; Ortiz, J. V.; Stefanov, B. B.; Liu, G.; Liashenko, A.; Piskorz, P.; Komaromi, I.; Gomperts, R.; Martin, R. L.; Fox, D. J.; Keith, T.; Al-Laham, M. A.; Peng, C. Y.; Nanayakkara, A.; Gonzalez, C.; Challacombe, M.; Gill, P M. W.; Johnson, B.; Chen, W.; Wong, M. W.; Andres, J. L.; Gonzalez, C.; Head-Gordon, M.; Replogle, E. S.; Pople, J. A. Gaussian 98, Revision A.6; Gaussian, Inc.: Pittsburgh, PA, 1998).
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65. 12
66. -.
67. 2O and the strong Coulomb forces imposed in the electrostatic model (recall that we have constrained the charges to be the same for all the clusters). Thus, the Lennard-Jones potential must be more repulsive (in this model) than one would expect on the basis of anion size. This is actually an initial indication of the shortcomings of the non-CT model for this cluster.
68. 18,19 Thus, it is not unreasonable to use our calculated binding energies as a substitute for binding enthalpies for these systems.
69. 12 have been adjusted to remove the effects due to a Fermi resonance between the hydrogen-bonded OH stretch and the overtone of the intramolecular bend.
70. 2O cluster. It is important to note that the neglect of these two effects will not alter the fundamental conclusions presented in this paper regarding the role of charge transfer in the frequency shifts.
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81. At some point, vibrational predissociation will complicate the analysis, but this is itself an interesting phenomenon (cf.: Staib, A.; Hynes, J. T. Chem. Phys. Lett. 1993, 204, 197-205. Heilweil, E. J. Science 1999, 283, 1467-1468. Woutersen, S.; Emmerichs, U.; Nienhuys, H.-K.; Bakker, H. J. Phys. Rev. Lett. 1998, 81, 1106-1109. Nienhuys, H.-K.; Woutersen, S.; van Santen, R. A.; Bakker, H. J. J. Chem. Phys. 1999, 111, 1494- 1500).
82. At some point, vibrational predissociation will complicate the analysis, but this is itself an interesting phenomenon (cf.: Staib, A.; Hynes, J. T. Chem. Phys. Lett. 1993, 204, 197-205. Heilweil, E. J. Science 1999, 283, 1467-1468. Woutersen, S.; Emmerichs, U.; Nienhuys, H.-K.; Bakker, H. J. Phys. Rev. Lett. 1998, 81, 1106-1109. Nienhuys, H.-K.; Woutersen, S.; van Santen, R. A.; Bakker, H. J. J. Chem. Phys. 1999, 111, 1494- 1500).
83. At some point, vibrational predissociation will complicate the analysis, but this is itself an interesting phenomenon (cf.: Staib, A.; Hynes, J. T. Chem. Phys. Lett. 1993, 204, 197-205. Heilweil, E. J. Science 1999, 283, 1467-1468. Woutersen, S.; Emmerichs, U.; Nienhuys, H.-K.; Bakker, H. J. Phys. Rev. Lett. 1998, 81, 1106-1109. Nienhuys, H.-K.; Woutersen, S.; van Santen, R. A.; Bakker, H. J. J. Chem. Phys. 1999, 111, 1494-1500).
84. This view is at odds with that of Giguere for HF [Giguere, P. A. J. Chem. Educ. 1979, 56, 571-575. Giguere, P. A. Chem. Phys. 1981, 60, 421-423], as is discussed in ref 39.
85. This view is at odds with that of Giguere for HF [Giguere, P. A. J. Chem. Educ. 1979, 56, 571-575. Giguere, P. A. Chem. Phys. 1981, 60, 421-423], as is discussed in ref 39.
86. -. It would be of interest in future work to examine this behavior in the context of the present type of analysis.
87. Scheiner, S.; Cuma, M. J. Am. Chem. Soc. 1996, 118, 1511-1521.