Long-distance magnetic interaction between a MnIIIMnIV (S = 1/2) core and an organic radical: A spectroscopic model for the S2Y2 · state of photosystem II

Angewandte Chemie - International Edition

Volumn 41, Issue 24, 2002, Pages 4775-4779

  Marlin, Dana S ^a   Bill, Eckhard ^a   Weyhermüller, Thomas ^a   Rentschler, Eva ^a   Wieghardt, Karl ^a  

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

Author keywords

EPR spectroscopy; Magnetic properties; Manganese; Photosystem II; Radicals

Indexed keywords

ETHANE; FREE RADICALS; SPECTROSCOPIC ANALYSIS;

EXCHANGE REACTIONS;

MANGANESE COMPOUNDS;

1,2 BIS(4,7 DIMETHYL 1,4 TRIAZACYCLONON 1 YL)ETHANE; 2 (4 CARBOXYPHENYL) 4,4,5,5 TETRAMETHYL 3 OXYIMIDAZOLIDIN 1 OXIDE; ETHANE; MANGANESE; OXIDE; UNCLASSIFIED DRUG;

ARTICLE; CHEMICAL STRUCTURE; CHEMISTRY; ELECTRON SPIN RESONANCE; MAGNETISM; PHOTOSYNTHESIS; PHOTOSYSTEM II; SPECTROSCOPY;

MAGNETICS; MANGANESE; MODELS, MOLECULAR; PHOTOSYNTHETIC REACTION CENTER COMPLEX PROTEINS; PHOTOSYSTEM II PROTEIN COMPLEX; SPECTRUM ANALYSIS;

EID: 0037122142     PISSN: 14337851     EISSN: None     Source Type: Journal    
DOI: 10.1002/anie.200290045     Document Type: Article

References (33)

1. A.-F. Miller, G. W. Brudwig, Biochim. Biophys. Acta 1991, 1056, 1.
2. J. Stubbe, W. A. van der Donk, Chem. Rev. 1998, 98, 705.
3. V. K. Yachandra, K. Sauer, M. P. Klein, Chem. Rev. 1996, 96, 2927.
4. B. Kok, B. Forbush, M. McGloin, Photochem. Photobiol. 1970, 11, 457.
5. G. C. Dismukes, Y. Siderer, Proc. Natl. Acad. Sci. USA 1981, 78, 274.
6. K.-O. Schäfer, R. Bittl, W. Zweygart, F. Lendzian, G. Haselhorst, T. Weyhermüller, K. Wieghardt, W. Lubitz, J. Am. Chem. Soc. 1998, 120, 13104.
7. a) J. M. Peloquin, K. A. Campbell, D. W. Randall, M. A. Evanchik, V. L. Pecoraro, W. H. Armstrong, R. D. Britt, J. Am. Chem. Soc. 2000, 122, 10926;
8. b) D. H. Kim, R. D. Britt, M. P. Klein, K. Sauer, J. Am. Chem. Soc. 1990, 112, 9389.
9. R.J. Debus, Biochim. Biophys. Acta 1992, 1102, 269.
10. P. Dorlet, A. Bossac, W. Rutherford, S. Un, J. Phys. Chem. B 1998, 102, 10945.
11. V. A. Szalai, H. Kühne, K. V. Lakshmi, G. W. Brudvig, Biochemistry 1998, 37, 13594.
12. W. Lubitz, F. Lendzian, R. Bittl, Acc. Chem. Res. 2002, 35, 313.
13. M. L. Gilchrist, Jr., J. A. Ball, D. W. Randall, R. D. Britt, Proc. Natl. Acad. Sci. USA 1995, 92, 9545.
14. P. Dorlet, M. Di Valentin, G.T. Babcock, J. L. McCracken, J. Phys. Chem. B 1998, 102, 8239.
15. K.V. Lakshmi, S. S. Eaton, G. R. Eaton, G. W. Brudvig, Biochemistry 1999, 38, 12758.
16. C. W. Hoganson, G. T. Babcock, Science 1997, 277, 1953.
17. X.-S. Tang, D. W. Randall, D. A. Force, B. A. Diner, R. D. Britt, J. Am. Chem. Soc. 1996, 118, 7638.
18. Y. Kodera, S. A. Dzuba, H. Hara, A. Kawamori, Biochim. Biophys. Acta 1994, 1186, 91.
19. A. Zouni, H.-T. Witt, J, Kern, P. Fromme, N, Krauß, W. Saenger, P. Orth, Nature 2001, 409, 739.
20. 4dtne=1,2-bis(4,7-dimethyl-1,4,7-triazacyclonon-1-yl)ethane was synthesized according to reference [6].
21. 2CPhNIT=2-(4-carboxyphenyl)-4,4,5,5- tetramethyl-3-oxyimidazolidin-1-oxide was prepared according to: C. Bätz, P, Amann, H.-J. Deiseroth, L. Dulog, Liebigs Ann. Chem. 1994, 739.
22. 14:C40.13, H 5.86, N 11.71; found: C 38.80, H 5.77, N 11.71.
23. -1, F(000)=2000; 56074 reflections collected at 100(2)K; 9213 independent reflections; GOF= 1.079; R=0.0448, wR2=0.0827. CCDC-192780 contains the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/conts/retrieving.html (or from the Cambridge Crystallographic Data Centre, 12, Union Road, Cambridge CB2 1EZ, UK; fax: (+44)1223-336-033; or deposit@ccdc.cam.ac.uk).
24. Early synthetic attempts at 1 and variants under less mild conditions resulted in complexes wherein decomposition of the NIT moiety took place yielding the imidazolidin-1-oxide radical product, which was evident from inequivalent thermal parameters of O(42) and O(39).
25. -1). The routine JULIUS was used for spin Hamiltonian simulations of the data (C. Krebs, E. Bill, F. Birkelbach, V. Staemmler, unpublished results).
26. EPR spectra were measured for solutions of 1-3 in acetonitrile with a Bruker ELEXSYS E300 spectrometer with standard or dual-mode cavity and Oxford Instruments ESR910 flow cryostat. Spin-Hamiltonian simulations were performed with the XSOPHE program by G. Hanson et al. that is distributed by Bruker Biospin GmbH.
27. 3+ is observed. The "impurity" spectra are similar to those in Figure 3 a and b and may be easily subtracted from that of intact 1 (shown in Figure 3c). The amount subtracted, integrated to less than 1 % by area.
28. E. Ullman, J. H. Osiecki, D. G. B. Boocock, R. Darcy, J. Am. Chem. Soc. 1972, 94, 7049.
29. a) J. E. Wertz, J. R. Bolton, Electron Spin Resonance, McGraw-Hill, New York, 1972;
30. b) P. J. Hore in Advanced EPR: Applications in Biology and Biochemistry (Ed.: A. J. Hoff), Elsevier, Amsterdam, 1977, pp. 405-440.
31. a) N. M. Atherton, C. J. Winscom, Inorg. Chem. 1973, 12, 383;
32. b) T. D. Smith, J. R. Pilbrow, Coord. Chem. Rev. 1974, 13, 173;
33. A. Bencini, D. Gatteschi, EPR of Exchange Coupled Systems, Springer, Berlin, 1990.