Observation of Terahertz Vibrations in the Nitrogenase FeMo Cofactor by Femtosecond Pump-Probe Spectroscopy

被引：8
作者：
Delfino, Ines
Cerullo, Giulio [3 ]
Cannistraro, Salvatore
Manzoni, Cristian [3 ]
Polli, Dario [3 ]
Dapper, Christie [4 ]
Newton, William E. [4 ]
Guo, Yisong [1 ]
Cramer, Stephen P. [1 ,2 ]
机构：
[1] Univ Calif Davis, Dept Appl Sci, Davis, CA 95616 USA
[2] Univ Calif Berkeley, Lawrence Berkeley Lab, Phys Biosci Div, Berkeley, CA 94720 USA
[3] Politecn Milan, IFN CNR, Dipartimento Fis, Milan, Italy
[4] Virginia Polytech Inst & State Univ, Dept Biochem, Blacksburg, VA 24061 USA
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2010年 / 49卷 / 23期
关键词：
bioinorganic chemistry; nitrogenases; pump-probe spectroscopy; vibrational spectroscopy; IRON-MOLYBDENUM COFACTOR; CHARGE-TRANSFER DYNAMICS; PYROCOCCUS-FURIOSUS RUBREDOXIN; RESONANCE RAMAN-SPECTROSCOPY; NORMAL-MODE ANALYSIS; COHERENCE SPECTROSCOPY; N-2; REDUCTION; ACTIVE-SITE; STATE; PLASTOCYANIN;
D O I：
10.1002/anie.200906787
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Pump it upl The FeMo cofactor (see picture) has resisted characterization by resonance Raman spectroscopy. Impulsive coherent vibrational spectroscopy may be an alternative probe of its dynamics. A 15 fs visible laser pulse pumped the sample to an excited electronic state, and a second < 10 fs pulse probed the change in transmission as a function of the time delay. (Figure Presented) © 2010 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
引用
收藏
页码：3912 / 3915
页数：4
相关论文
共 37 条
[21]  
NEWTON WE, 2004, NITROGEN FIXATION OR, V1
[22]   Fertilized to death [J].
Nosengo, N .
NATURE, 2003, 425 (6961) :894-895
[23]   Exploring new frontiers of nitrogenase structure and mechanism [J].
Peters, JW ;
Szilagyi, RK .
CURRENT OPINION IN CHEMICAL BIOLOGY, 2006, 10 (02) :101-108
[24]   Electron-transfer chemistry of the iron-molybdenum cofactor of nitrogenase: Delocalized and localized reduced states of FeMoco which allow binding of carbon monoxide to iron and molybdenum [J].
Pickett, CJ ;
Vincent, KA ;
Ibrahim, SK ;
Gormal, CA ;
Smith, BE ;
Best, SP .
CHEMISTRY-A EUROPEAN JOURNAL, 2003, 9 (01) :76-87
[25]   High-time-resolution pump-probe system with broadband detection for the study of time-domain vibrational dynamics [J].
Polli, Dario ;
Lueer, Larry ;
Cerullo, Giulio .
REVIEW OF SCIENTIFIC INSTRUMENTS, 2007, 78 (10)
[26]   Structural basis of biological nitrogen fixation [J].
Rees, DC ;
Tezcan, FA ;
Haynes, CA ;
Walton, MY ;
Andrade, S ;
Einsle, O ;
Howard, JB .
PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES, 2005, 363 (1829) :971-984
[27]   Wavelength selective modulation in femtosecond pump-probe spectroscopy and its application to heme proteins [J].
Rosca, F ;
Kumar, ATN ;
Ionascu, D ;
Sjodin, T ;
Demidov, AA ;
Champion, PM .
JOURNAL OF CHEMICAL PHYSICS, 2001, 114 (24) :10884-10898
[28]   ISOLATION OF AN IRON-MOLYBDENUM COFACTOR FROM NITROGENASE [J].
SHAH, VK ;
BRILL, WJ .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1977, 74 (08) :3249-3253
[29]   Normal-mode analysis of FeCl4- and Fe2S2Cl42- via vibrational Mossbauer, resonance Raman, and FT-IR spectroscopies [J].
Smith, MC ;
Xiao, YM ;
Wang, HX ;
George, SJ ;
Coucouvanis, D ;
Koutmos, M ;
Sturhahn, W ;
Alp, EE ;
Zhao, JY ;
Cramer, SP .
INORGANIC CHEMISTRY, 2005, 44 (16) :5562-5570
[30]   Observation of terahertz vibrations in Pyrococcus furiosus rubredoxin via impulsive coherent vibrational spectroscopy and nuclear resonance vibrational spectroscopy -: interpretation by molecular mechanics [J].
Tan, Ming-Liang ;
Bizzarri, Anna Rita ;
Xiao, Yuming ;
Cannistraro, Salvatore ;
Ichiye, Toshiko ;
Manzoni, Cristian ;
Cerullo, Giulio ;
Adams, Michael W. W. ;
Jenney, Francis E., Jr. ;
Cramer, Stephen P. .
JOURNAL OF INORGANIC BIOCHEMISTRY, 2007, 101 (03) :375-384
1234