Dynamics of wild-type HiPIPs: A Cys77Ser mutant and a partially unfolded HiPIP

被引:11
作者
Dilg, AWE
Grantner, K
Iakovleva, O
Parak, FG
Babini, E
Bertini, I
Capozzi, F
Luchinat, C
Meyer-Klaucke, W
机构
[1] Tech Univ Munich, Phys Dept E17, D-85747 Garching, Germany
[2] Univ Florence, Magnet Resonance Ctr, I-50019 Florence, Italy
[3] DESY, EMBL, D-22603 Hamburg, Germany
来源
JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY | 2002年 / 7卷 / 7-8期
关键词
high-potential iron proteins; Chromatium vinosum; iron-sulfur cluster; Mossbauer; extended X-ray absorption fine structure;
D O I
10.1007/s00775-002-0344-4
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
The temperature dependence of the mean square displacement of the Fe-57 nuclei due to motion faster than 100 ns are measured by temperature-dependent Mossbauer spectroscopy for oxidized and reduced HiPIPs from Ectothiorhodospira halophila, Chromatium vinosum WT and a Cys77Ser mutant. The behaviour is interpretable in the frame of the general model of protein dynamics distinguishing two temperature intervals. The character of harmonic and quasi-diffusional modes in HiPIPs is discussed. Dynamic information obtained from Mossbauer spectroscopy and Fe K-edge EXAFS are compared. Structure dynamics of the iron-sulfur cluster in the partially unfolded reduced HiPIP from C. vinosum was investigated by Mossbauer spectroscopy and EXAFS, indicating an intact metal centre and a protein backbone with a largely collapsed secondary structure. The role of the cofactor during protein folding is discussed. Differences in the dynamics between the native protein and the molten globule are found at physiological temperatures only. The structure and dynamic behaviour of the [Fe4S4]Cys(3)Ser cluster in the Cys77Ser mutant of the HiPIP from C. vinosum are analysed. The temperature dependence of electron relaxation in oxidized HiPIPs is investigated by Mossbauer spectroscopy and analysed theoretically, considering spin-spin and spin-lattice relaxation. The latter consists of contributions from direct phonon bottleneck and Orbach mechanisms. The data agree with former pulsed EPR results. Orbach relaxation is interpreted as due to transitions between electronic isomers of oxidized HiPIPs. With this interpretation, the energetic difference between both isomers equals the energy gap estimated from the temperature dependence of the Orbach relaxation.
引用
收藏
页码:691 / 703
页数:13
相关论文
共 69 条
[41]  
GUTLICH P, 1978, INORGANIC CHEM CONCE, P56
[42]  
JENSEN LH, 1987, IRON SULFUR PROTEIN, P3
[43]   SOME APPLICATIONS OF STATISTICAL TESTS IN ANALYSIS OF EXAFS AND SEXAFS DATA [J].
JOYNER, RW ;
MARTIN, KJ ;
MEEHAN, P .
JOURNAL OF PHYSICS C-SOLID STATE PHYSICS, 1987, 20 (25) :4005-4012
[44]   Probing structural and electronic properties of the oxidized [Fe4S4]3+ cluster of Ectothiorhodospira halophila iso-II high-potential iron-sulfur protein by ENDOR spectroscopy [J].
Kappl, R ;
Ciurli, S ;
Luchinat, C ;
Hüttermann, J .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1999, 121 (09) :1925-1935
[45]   NEW METHOD FOR CALCULATION OF ATOMIC PHASE-SHIFTS - APPLICATION TO EXTENDED X-RAY ABSORPTION FINE-STRUCTURE (EXAFS) IN MOLECULES AND CRYSTALS [J].
LEE, PA ;
BENI, G .
PHYSICAL REVIEW B, 1977, 15 (06) :2862-2883
[46]  
Makinen MW, 1987, MET IONS BIOL SYST, P129
[47]   STRUCTURAL DYNAMICS OF HUMAN DEOXYHEMOGLOBIN AND HEMOCHROME INVESTIGATED BY NUCLEAR GAMMA-RESONANCE ABSORPTION (MOSSBAUER) SPECTROSCOPY [J].
MAYO, KH ;
KUCHEIDA, D ;
PARAK, F ;
CHIEN, JCW .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA-BIOLOGICAL SCIENCES, 1983, 80 (17) :5294-5296
[48]   LOW-POTENTIAL IRON SULFUR CENTERS IN PHOTOSYSTEM-I - AN X-RAY ABSORPTION-SPECTROSCOPY STUDY [J].
MCDERMOTT, AE ;
YACHANDRA, VK ;
GUILES, RD ;
BRITT, RD ;
DEXHEIMER, SL ;
SAUER, K ;
KLEIN, MP .
BIOCHEMISTRY, 1988, 27 (11) :4013-4020
[49]   Structural fluctuations of myoglobin from normal-modes, Mossbauer, Raman, and absorption spectroscopy [J].
Melchers, B ;
Knapp, EW ;
Parak, F ;
Cordone, L ;
Cupane, A ;
Leone, M .
BIOPHYSICAL JOURNAL, 1996, 70 (05) :2092-2099