Excited-state contributions to ground-state properties of mixed-valence dimers: Spectral and electronic-structural studies of [Fe2(OH)3(tmtacn)2]2+ related to the [Fe2S2]+ active sites of plant-type ferredoxins

Journal of the American Chemical Society

Volumn 118, Issue 34, 1996, Pages 8085-8097

  Gamelin, Daniel R ^a   Bominaar, Emile L ^b   Kirk, Martin L ^a   Wieghardt, Karl ^c   Solomon, Edward I ^a  

^a STANFORD UNIVERSITY   (United States)

^b CARNEGIE MELLON UNIVERSITY   (United States)

^c MAX PLANCK INSTITUTE FOR CHEMICAL ENERGY CONVERSION   (Germany)

Author keywords

[No Author keywords available]

Indexed keywords

FERREDOXIN; IRON COMPLEX;

ARTICLE; DRUG STRUCTURE; MODEL; MOLECULAR DYNAMICS; RAMAN SPECTROMETRY; THERMODYNAMICS; X RAY DIFFRACTION;

EID: 0029816180     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja9536633     Document Type: Article

References (71)

1. Mixed Valency Systems: Applications in Chemistry, Physics, and Biology; Prassides, K., Ed.; Kluwer Academic Publishers: Dordrecht, The Netherlands, 1991.
2. Mechanistic Aspects of Inorganic Reactions: Rorabacher, D. B., Endicott, J. F., Eds.; ACS Symposium Series; American Chemical Society: Washington, DC, 1982; Vol. 198.
3. Mixed-Valence Compounds; Brown, D. B., Ed.; Reidel: Dordrecht, The Netherlands, 1980.
4. Iron-Sulfur Proteins; Cammack, R., Ed.; Adv. Inorg. Chem., Vol. 38; Academic Press, Inc.: San Diego, 1992.
5. Iron-Sulfur Proteins; Spiro, T. G., Ed.; Wiley and Sons: New York, 1982.
6. Que, L., Jr.; True, A. E. Prog. Inorg. Chem. 1990, 38, 97-200.
7. Solomon, E. I. In Metal Clusters in Proteins; Que, L., Jr., Ed.: ACS Symposium Series; American Chemical Society: Washington, DC, 1988; Vol. 372, pp 116-150.
8. Bioinorganic Chemistry of Copper; Karlin, K. D., Tyeklár, Z., Eds.; Chapman & Hall Inc.: New York, 1993.
9. Ramirez, B. E.; Malmström, B. G.; Winkler, J. R.; Gray, H. B. Proc. Natl. Acad. Sci. U.S.A. 1995, 92, 11949-11951.
10. Manganese Redox Enzymes; Pecoraro, V. L., Ed.; VCH Publishers: New York, 1992.
11. Robin, M. B.; Day, P. Adv. Inorg. Chem. Radiochem. 1967, 10, 247-403.
12. Zener, C. Phys. Rev. 1951, 82, 403-405.
13. Andersen, P. W.; Hasegawa, H. Phys. Rev. 1955, 100, 675.
14. Girerd, J.-J. J. Chem. Phys. 1983, 79, 1766-1775.
15. Noodleman, L.; Baerends, E. J. J. Am. Chem. Soc. 1984, 106, 2316-2327.
16. Blondin, G.; Girerd, J.-J. Chem. Rev. 1990, 90, 1359-1376.
17. Bominaar, E. L.; Hu, Z.; Münck, E.; Girerd, J.-J.; Borshch, S. A. J. Am. Chem. Soc. 1995, 117, 6976-6989.
18. Borshch, S. A.; Bominaar, E. L.; Blondin, G.: Girerd, J.-J. J. Am. Chem. Soc. 1993, 115, 5155-5168.
19. Noodleman, L.; Case, D. A. Adv. Inorg. Chem. 1992, 38, 423-470.
20. Ross, P. K.; Allendorf, M. D.; Solomon, E. I. J. Am. Chem. Soc. 1989, 111, 4009-4021.
21. Tuczek, F.; Solomon, E. I. Inorg. Chem. 1993, 32, 2850-2862.
22. Brown, C. A.; Remar, G. J.; Musselman, R. L.; Solomon, E. I. Inorg. Chem. 1995, 34, 688-717.
23. Drüeke, S.; Chaudhuri, P.; Pohl, K.; Wieghardt, K.; Ding, X.-Q.; Bill, E.; Sawaryn, A.; Trautwein, A. X.: Winkler, H.; Gurman, S. J. J. Chem. Soc., Chem. Commun. 1989, 59-62.
24. Ding, X.-Q.; Bominaar, E. L.; Bill, E.; Winkler, H.; Trautwein, A. X.; Drüeke, S.; Chaudhuri, P.; Wieghardt, K. J. Chem. Phys. 1990, 92, 178-186.
25. Peng, G.; van Elp, J.; Jang, H.: Que, L., Jr.; Armstrong, W. H.; Cramer, S. P. J. Am. Chem. Soc. 1995, 117, 2515-2519.
26. Sheldrick, G. M. SHELX-76; University of Cambridge: Cambridge, England, 1976.
27. International Tables for X-Ray Crystallography, Kynoch Press: Birmingham, England, 1974; Vol. IV, pp 99-149.
28. Walker, N.; Stuart, D. Acta Crystallogr. 1983, A39, 158-166.
29. Weller, R. R.: Hatfield, W. E. J. Chem. Educ. 1979, 56, 652.
30. Modern Coordination Chemistry; Figgis, B. N., Lewis, J., Eds.; Interscience: New York, 1960; p 403.
31. König, E. Magnetic Properties of Transition Metal Compounds; Springer-Verlag: Berlin, 1966.
32. Cook, M.; Case, D. A. QCPE Program #465 1991, 23, 21-22.
33. Kittel, C. Introduction to Solid Slate Physics; 6th ed.; Wiley & Sons: New York, 1986; pp 400-402.
34. Gamelin, D. R.; Bominaar, E. L.; Mathonière, C.; Kirk, M. L.; Girerd, J.-J.; Wieghardt, K.; Solomon, E. I. Inorg. Chem. 1996, 35, 4323-4335.
35. Vermaas, A.; Groeneveld, W. L. Chem. Phys. Lett. 1974, 27, 583-585.
36. Scarborough, J. P. Numerical Mathematical Analysis; Oxford University Press: New York, 1971; p 159.
37. Marathe, V. R.; Mitra, S. Chem. Phys. Lett. 1974, 27, 103-106.
38. Medley, G. A.; Stranger, R. Inorg. Chem. 1994, 33, 3976-3985.
39. Natkaniec, L. Bul. Acad. Pol. Sc. 1978, 26, 633-640.
40. Summerville, R. H.; Hoffmann, R. J. Am. Chem. Soc. 1979, 101, 3821-3831.
41. Leuenberger, B.; Güdel, H. U. Inorg. Chem. 1986, 25, 181-184.
42. Natkaniec, L. Bull. Acad. Pol. Sci. 1978, 26, 625-631.
43. Hush, N. S.; Beattie, J. K.; Ellis, V. M. Inorg. Chem. 1984, 23, 3339-3342.
44. Riesen, H.; Reber, C.; Güdel, H. U.; Wieghardt, K. Inorg. Chem. 1987, 26, 2747-2750.
45. Stranger, R.; Moran, G.; Krausz, E.; Medley, G. Inorg. Chem. 1993, 32, 4555-4560.
46. Ballhausen, C. J. Introduction to Ligand Field Theory; McGraw-Hill: New York, 1962.
47. Trogler, W. C. Inorg. Chem. 1980, 19, 697-700.
48. Mortensen, O. S.; Hassing, S. In Advances in Infrared and Roman Spectroscopy; Clark, R. J., Hester, R. E., Eds.; Heyden: London, 1979; Vol. 6. pp 1-60.
49. Piepho, S. B.; Schatz, P. N. Group Theory in Spectroscopy; Wiley-Interscience: New York, 1983.
50. Dubicki, L.; Ferguson, J. Chem. Phys. Lett. 1984, 109, 128-131.
51. Gerstman, B. S.; Brill, A. S. J. Chem. Phys. 1985, 82, 1212-1230.
52. Schläfer, H. L.; Glieman, G. Basic Principles of Ligand Field Theory; Wiley-Interscience: London, 1969; p 78.
53. This overestimation is reflected in the hybridization of the two e′ dimer orbitals (Table 2), which deviate from the trigonal limit of eq 6 and approach the axial limit in which metal-metal π-bonding is optimized.
54. Anderson, P. W. Solid State Phys. 1963, 14, 99-214.
55. Hay, P. J.; Thibeault, J. C.; Hoffmann, R. J. Am. Chem. Soc. 1975, 97, 4884-4899.
56. 2+ on the basis of orbital-overlap considerations.
57. McCormick, J. M.; Reem, R. C.; Solomon, E. I. J. Am. Chem. Soc. 1991, 113, 9066-9079.
58. (a) Dunham, W. R.; Bearden, A. J.; Salmeen, I. T.; Palmer, G.; Sands, R. H.; Orme-Johnson, W. H.; Beinert, H. Biochim. Biophvs. Acta 1971, 253, 134-152.
59. (b) Mascharak, P. K.; Papaefthymiou, G. C.; Frankel, R. B.; Holm, R. H. J. Am. Chem. Soc. 1981, 103, 6110-6116.
60. Indeed, S = 9/2 ground-state magnetic properties have very recently been reported for two mutants of C. pasteurianum ferredoxin, and although Mössbauer studies are still needed to determine their degree of valence delocalization, this ferromagnetism is likely a manifestation of double exchange. Crouse, B. R.; Meyer, J.; Johnson, M. K. J. Am. Chem. Soc. 1995, 117, 9612-9613.
61. Petersson, L.; Cammack, R.; Rao, K. K. Biochim. Biophys. Acta 1980, 622, 18-24.
62. Palmer, G. In Iron-Sulfur Proteins; Lovenberg, W., Ed.; Academic Press: New York, 1973; pp 285-325.
63. Norman, J. G., Jr.; Kalbacher, B. J.; Jackels, S. C. J. Chem. Soc., Chem. Commun. 1978, 1027-1029.
64. Summerville, R. H.; Hoffmann, R. J. Am. Chem. Soc. 1976, 98, 7240-7254.
65. -1.
66. Lane, R. W.; Ibers, J. A.; Frankel, R. B.; Papaefthymiou, G. C.; Holm, R. H. J. Am. Chem. Soc. 1977, 99, 84-98.
67. Hair, N. J.; Beattie, J. K. Inorg. Chem. 1977, 16, 245-250.
68. Snyder, B. S.; Patterson, G. S.: Abrahamson, A. J.; Holm, R. H. J. Am. Chem. Soc. 1989, 111, 5214-5223.
69. Han, S.; Czernuszewicz, R. S.; Kimura, T.; Adams, M. W. W.; Spiro, T. G. J. Am. Chem. Soc. 1989, 111, 3505-3511.
70. Fu, W.; Drozdzewski, P. M.; Davies, M. D.; Sugar, S. G.; Johnson, M. K. J. Biol. Chem. 1992, 267, 15502-15510.
71. Note Added in Proof: Very recent Mössbauer studies demonstrate that the S = 9/2 ground states observed in ref 59 are valence delocalized. Achim, C.; Golinelli, M. P.; Bominaar, E. L.; Meyer, J.; Münck, E. J. Am. Chem. Soc., in press.