Density Functional Study of 17O NMR Chemical Shift and Nuclear Quadrupole Coupling Tensors in Oxyheme Model Complexes

Journal of Physical Chemistry B

Volumn 104, Issue 21, 2000, Pages 5200-5208

  Kaupp, Martin ^a,c   Rovira, Carme ^b   Parrinello, Michele ^a  

^a MAX PLANCK INSTITUT FÜR FESTKÖRPERFORSCHUNG   (Germany)

^b UNIVERSITY OF BARCELONA   (Spain)

^c UNIVERSITY OF WÜRZBURG   (Germany)

Author keywords

[No Author keywords available]

Indexed keywords

EID: 0000901899     PISSN: 15206106     EISSN: None     Source Type: Journal    
DOI: 10.1021/jp994234k     Document Type: Article

References (70)

1. See, e.g.: Perutz, M. F.; Fermi, G.; Luisi, B.; Shaanan, B.; Liddington, R. C. Acc. Chem. Res. 1987, 20, 309. Shaanan, B. J. Mol. Biol. 1983, 171, 31. Olson, J. S.; Phillips, G. N. J. Mol. Biol. 1996, 271, 17593.
2. See, e.g.: Perutz, M. F.; Fermi, G.; Luisi, B.; Shaanan, B.; Liddington, R. C. Acc. Chem. Res. 1987, 20, 309. Shaanan, B. J. Mol. Biol. 1983, 171, 31. Olson, J. S.; Phillips, G. N. J. Mol. Biol. 1996, 271, 17593.
3. See, e.g.: Perutz, M. F.; Fermi, G.; Luisi, B.; Shaanan, B.; Liddington, R. C. Acc. Chem. Res. 1987, 20, 309. Shaanan, B. J. Mol. Biol. 1983, 171, 31. Olson, J. S.; Phillips, G. N. J. Mol. Biol. 1996, 271, 17593.
4. Springer, B. A.; Sligar, S. G.; Olson, J. S.; Philips, G. N. Chem. Rev. 1994, 94, 699. Schlichting, I.; Berendzen, J.; Philips, G. N.; Sweet, R. M. Nature 1994, 371, 808. Lim, M.; Jackson, T. A.; Anfirud, P. A. Science 1995, 269, 962. Slebodnik, C.; Ibers, J. A. J. Biol. Inorg. Chem. 1997, 2, 521.
5. Springer, B. A.; Sligar, S. G.; Olson, J. S.; Philips, G. N. Chem. Rev. 1994, 94, 699. Schlichting, I.; Berendzen, J.; Philips, G. N.; Sweet, R. M. Nature 1994, 371, 808. Lim, M.; Jackson, T. A.; Anfirud, P. A. Science 1995, 269, 962. Slebodnik, C.; Ibers, J. A. J. Biol. Inorg. Chem. 1997, 2, 521.
6. Springer, B. A.; Sligar, S. G.; Olson, J. S.; Philips, G. N. Chem. Rev. 1994, 94, 699. Schlichting, I.; Berendzen, J.; Philips, G. N.; Sweet, R. M. Nature 1994, 371, 808. Lim, M.; Jackson, T. A.; Anfirud, P. A. Science 1995, 269, 962. Slebodnik, C.; Ibers, J. A. J. Biol. Inorg. Chem. 1997, 2, 521.
7. Springer, B. A.; Sligar, S. G.; Olson, J. S.; Philips, G. N. Chem. Rev. 1994, 94, 699. Schlichting, I.; Berendzen, J.; Philips, G. N.; Sweet, R. M. Nature 1994, 371, 808. Lim, M.; Jackson, T. A.; Anfirud, P. A. Science 1995, 269, 962. Slebodnik, C.; Ibers, J. A. J. Biol. Inorg. Chem. 1997, 2, 521.
8. Momenteau, M.; Reed, C. A. Chem. Rev. 1994, 94, 659.
9. See, e.g.: Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E.; Barrie, P. J. J. Am. Chem. Soc. 1993, 115, 9796. Gerothanassis, I. P.; Barrie, P. J.; Momenteau, M.; Hawkes, G. E. J. Am. Chem. Soc. 1994, 116, 11944. Barrie, P. J.; Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E. J. Magn. Reson. 1995, 108, 185. Kaladomidous, C. G.; Gerothanassis, I. P.; Rose, E.; Hawkes, G. E.; Pieratelli, R. J. Am. Chem. Soc. 1999, 121, 2903 and references therein.
10. See, e.g.: Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E.; Barrie, P. J. J. Am. Chem. Soc. 1993, 115, 9796. Gerothanassis, I. P.; Barrie, P. J.; Momenteau, M.; Hawkes, G. E. J. Am. Chem. Soc. 1994, 116, 11944. Barrie, P. J.; Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E. J. Magn. Reson. 1995, 108, 185. Kaladomidous, C. G.; Gerothanassis, I. P.; Rose, E.; Hawkes, G. E.; Pieratelli, R. J. Am. Chem. Soc. 1999, 121, 2903 and references therein.
11. See, e.g.: Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E.; Barrie, P. J. J. Am. Chem. Soc. 1993, 115, 9796. Gerothanassis, I. P.; Barrie, P. J.; Momenteau, M.; Hawkes, G. E. J. Am. Chem. Soc. 1994, 116, 11944. Barrie, P. J.; Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E. J. Magn. Reson. 1995, 108, 185. Kaladomidous, C. G.; Gerothanassis, I. P.; Rose, E.; Hawkes, G. E.; Pieratelli, R. J. Am. Chem. Soc. 1999, 121, 2903 and references therein.
12. See, e.g.: Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E.; Barrie, P. J. J. Am. Chem. Soc. 1993, 115, 9796. Gerothanassis, I. P.; Barrie, P. J.; Momenteau, M.; Hawkes, G. E. J. Am. Chem. Soc. 1994, 116, 11944. Barrie, P. J.; Gerothanassis, I. P.; Momenteau, M.; Hawkes, G. E. J. Magn. Reson. 1995, 108, 185. Kaladomidous, C. G.; Gerothanassis, I. P.; Rose, E.; Hawkes, G. E.; Pieratelli, R. J. Am. Chem. Soc. 1999, 121, 2903 and references therein.
13. Gerothanassis, I. P. Prog. Nucl. Magn. Reson. Spectrosc. 1994, 26, 239.
14. Gerothanassis, I. P.; Momenteau, M. J. Am. Chem. Soc. 1987, 109, 6944.
15. Gerothanassis, I. P.; Momenteau, M.; Loock, B. J. Am. Chem. Soc. 1989, 111, 7006.
16. Oldfield, E.; Lee, H. C.; Coretsopoulos, C.; Adebodun, F.; Park, K. D.; Yang, S.; Chung, J.; Phillips, B. J. Am. Chem. Soc. 1991, 113, 8680.
17. Godbout, N.; Sanders, L. K.; Salzmann, R.; Havlin, R. H.; Wojdelski, M.; Oldfield, E. J. Am. Chem. Soc. 1999, 121, 3829.
18. (a) Pauling, L.; Coryell, C. D. Proc. Natl. Acad. Sci. U.S.A. 1936, 22, 210.
19. (b) Pauling, L. Nature 1964, 203, 182.
20. (c) Pauling, L. Proc. Natl. Acad. Sci. 1977, 74, 2612.
21. Weiss, J. J. Nature 1964, 202, 83.
22. Kaupp, M.; Malkina, O. L.; Malkin, V. G. NMR of Transition Metal Compounds. In Encyclopedia of Computational Chemistry; Schleyer, P. v. R., Ed.; Wiley-Interscience, New York, 1998; pp 1857-1866.
23. Bühl, M.; Kaupp, M.; Malkin, V. G.; Malkina, O. L. J. Comput. Chem. 1999, 20, 91.
24. Schreckenbach, G.; Ziegler, T. Theor. Chem. Acc. 1998, 2, 71.
25. Godbout, N.; Havlin, R. H.; Salzmann, R.; Debrunner, P. G.; Oldfield, E. J. Phys. Chem. A 1998, 102, 2342. McMahon, M. T.; deDios, A. C.; Godbout, N.; Salzmann, R.; Laws, D. D.; Havlin, R. H.; Oldfield, E. J. Am. Chem. Soc. 1998, 120, 4787.
26. Godbout, N.; Havlin, R. H.; Salzmann, R.; Debrunner, P. G.; Oldfield, E. J. Phys. Chem. A 1998, 102, 2342. McMahon, M. T.; deDios, A. C.; Godbout, N.; Salzmann, R.; Laws, D. D.; Havlin, R. H.; Oldfield, E. J. Am. Chem. Soc. 1998, 120, 4787.
27. Salzmann, R.; Ziegler, C. J.; Godbout, N.; McMahon, M. T.; Suslick, K. S.; Oldfield, E. J. Am. Chem. Soc. 1999, 121, 11323.
28. Rovira, C.; Kunc, K.; Hutter, J.; Ballone, P.; Parrinello, M. J. Phys. Chem. A 1997, 101, 8914. Rovira, C.; Parrinello, M. Int. J. Quantum Chem. 1998, 70, 387.
29. Rovira, C.; Kunc, K.; Hutter, J.; Ballone, P.; Parrinello, M. J. Phys. Chem. A 1997, 101, 8914. Rovira, C.; Parrinello, M. Int. J. Quantum Chem. 1998, 70, 387.
30. Rovira, C.; Parrinello, M. Chem. Eur. J. 1999, 5, 250.
31. Rovira, C.; Parrinello, M. Biophys. J. 2000, 78, 93.
32. -4 au for the ionic gradients. Structure optimizations were performed with no constraints starting from nonsymmetric structures. See refs 18 and 19 for further details.
33. (a) Salahub, D. R.; Fournier, R.; Mlynarski, P.; Papai, I.; St-Amant, A.; Ushio, J. In Density Functional Methods in Chemistry, Labanowski, J., Andzelm, J., Eds.; Springer: New York, 1991.
34. (b) St-Amant, A.; Salahub, D. R. Chem. Phys. Lett. 1990, 169, 387.
35. Becke, A. D. Phys. Rev. A 1988, 38, 3098. Perdew, J. P.; Wang, Y. Phys. Rev. B 1986, 33, 8822.
36. Becke, A. D. Phys. Rev. A 1988, 38, 3098. Perdew, J. P.; Wang, Y. Phys. Rev. B 1986, 33, 8822.
37. Bergner, A.; Dolg, M.; Küchle, W.; Stoll, H.; Preuss, H. Mol. Phys. 1993, 80, 1431.
38. d-Functions from: Huzinaga, S., Ed. Gaussian Basis Sets for Molecular Calculations; Elsevier: New York, 1984.
39. Godbout, N.; Salahub, D. R.; Andzelm, J. Wimmer, E. Can. J. Chem. 1992, 70, 560.
40. For such small molecules, the use of localized basis sets rather than plane waves is more efficient. Otherwise the computational level is consistent with the CPMD calculations. The deMon optimizations made use of an extra SCF iteration without fit of the exchange-correlation potential.
41. Malkin, V. G.; Malkina, O. L.; Casida, M. E.; Salahub, D. R. J. Am. Chem. Soc. 1994, 116, 5898.
42. Malkin, V. G.; Malkina, O. L.; Eriksson, L. A.; Salahub, D. R. In Modern Density Functional Theory: A Tool for Chemistry: Theoretical and Computational Chemistry; Seminario, J. M., Politzer, P., Eds.; Vol. 2; Elsevier: Amsterdam, 1995; Vol. 2.
43. See, e.g.: Malkin, V. G.; Malkina, O. L.; Salahub, D. R. Chem. Phys. Lett. 1993, 204, 80.
44. Olsson, L.; Cremer, D. J. Chem. Phys. 1996, 105, 8995.
45. Kaupp, M.; Malkina, O. L.; Malkin, V. G. J. Chem. Phys. 1997, 106, 9201.
46. See, e.g.: Perdew, J. P. Phys. B 1992, 172, 1. Perdew, J. P. In Electronic Structure of Solids '91; Ziesche, P., Eschring, H.. Eds.; Akademie Verlag: Berlin, 1991. Perdew, J. P.; Wang, Y. Phys. Rev. B 1992, 45, 13244.
47. See, e.g.: Perdew, J. P. Phys. B 1992, 172, 1. Perdew, J. P. In Electronic Structure of Solids '91; Ziesche, P., Eschring, H.. Eds.; Akademie Verlag: Berlin, 1991. Perdew, J. P.; Wang, Y. Phys. Rev. B 1992, 45, 13244.
48. See, e.g.: Perdew, J. P. Phys. B 1992, 172, 1. Perdew, J. P. In Electronic Structure of Solids '91; Ziesche, P., Eschring, H.. Eds.; Akademie Verlag: Berlin, 1991. Perdew, J. P.; Wang, Y. Phys. Rev. B 1992, 45, 13244.
49. Daul, C. A.; Goursot, A.; Salahub, D. R. In NATO ARW Proceedings on Grid Methods in Atomic and Molecular Quantum Calculation; Cerjan, C., Ed.; Kluwer: Dordrecht, 1993; Vol. C412.
50. Kutzelnigg, W.; Fleischer, U.; Schindler, M. In NMR-Basic Principles and Progress; Springer: Heidelberg 1990; Vol. 23, pp 165ff.
51. Dolg, M.; Wedig, U.; Stoll, H.; Preuss, H. J. Chem. Phys. 1987, 86, 866.
52. Sundholm, D.; Gauss, J.; Schäfer, A. J. Chem. Phys. 1996, 105, 11051.
53. See, e.g.: Fedotov, M. A.; Malkina, O. L.; Malkin, V. G. Chem. Phys. Lett. 1996, 258, 330.
54. See, e.g.: Salzmann, R.; Kaupp, M.; McMahon, M.; Oldfield, E. J. Am. Chem. Soc. 1998, 120, 4771.
55. For early qualitative theoretical considerations, cf.: Maricic, S.; Leigh, J. S., Jr.; Sunko, D. E. Nature 1967, 214, 3017. Velenic, A.; Lynden- Bell, R. M. Croat. Chim. Acta 1969, 41, 205. Velenic, A.; Lynden-Bell, R. M. Mol. Phys. 1970, 19, 371.
56. For early qualitative theoretical considerations, cf.: Maricic, S.; Leigh, J. S., Jr.; Sunko, D. E. Nature 1967, 214, 3017. Velenic, A.; Lynden-Bell, R. M. Croat. Chim. Acta 1969, 41, 205. Velenic, A.; Lynden-Bell, R. M. Mol. Phys. 1970, 19, 371.
57. For early qualitative theoretical considerations, cf.: Maricic, S.; Leigh, J. S., Jr.; Sunko, D. E. Nature 1967, 214, 3017. Velenic, A.; Lynden- Bell, R. M. Croat. Chim. Acta 1969, 41, 205. Velenic, A.; Lynden-Bell, R. M. Mol. Phys. 1970, 19, 371.
58. Goddard, W. A.; Olafson, B. D. Proc. Natl. Acad. Sci. U.S.A. 1975, 72, 2335. Olafson, B. D.; Goddard, W. A. Proc. Natl. Acad. Sci. U.S.A. 1977, 74, 1315.
59. Goddard, W. A.; Olafson, B. D. Proc. Natl. Acad. Sci. U.S.A. 1975, 72, 2335. Olafson, B. D.; Goddard, W. A. Proc. Natl. Acad. Sci. U.S.A. 1977, 74, 1315.
60. See also: Bytheway, I.; Hall, M. B. Chem. Rev. 1994, 94, 639 and references therein.
61. See, e.g.: Huynh, B.; Case, D. A.; Karplus, M. J. Am. Chem. Soc. 1977, 99, 6103 and references therein.
62. Spartalian, K.; Lang, G.; Collman, J. P.; Gagne, R. R.; Reed, O. J. Chem. Phys. 1975, 63, 5375.
63. Schindler, M.; Kutzelnigg, W. Mol. Phys. 1983, 48, 781. These calculations did not include electron correlation, and thus the quantitative agreement with experiment was poor.
64. Cohen, E. A.; Pickett, H. M. J. Mol. Struct. 1983, 97, 97.
65. A significant contribution of the shift anisotropy to the line widths might be determined from measurements at different field strengths.
66. See also: Summerville, D. A.; Jones, R. D.; Hoffman, B. M.; Basolo, F. J. Chem. Educ. 1979, 50, 157 and references therein.
67. e is the free electron g-factor, S is the total spin, k is Boltzmann's constant, and T is the absolute temperature. Inserting our computed spin densities into eq 1 leads to contact shifts for the triplet state (S = 1) of ca. +5220 ppm and ca. -3790 ppm for bridging and terminal oxygen positions, respectively, at T = 298 K. At T = 11 K, the contact shifts are computed to be ca. +20190 ppm and ca. -14680 ppm, respectively.
68. e is the free electron g-factor, S is the total spin, k is Boltzmann's constant, and T is the absolute temperature. Inserting our computed spin densities into eq 1 leads to contact shifts for the triplet state (S = 1) of ca. +5220 ppm and ca. -3790 ppm for bridging and terminal oxygen positions, respectively, at T = 298 K. At T = 11 K, the contact shifts are computed to be ca. +20190 ppm and ca. -14680 ppm, respectively.
69. Noodleman, L. J. Chem. Phys. 1981, 74, 5737.
70. Tsai, T. E.; Groves, J. L.; Wu, C. S. J. Chem. Phys. 1981, 74, 4306.