Fluctuating enzymes: Lessons from single-molecule studies

被引:316
作者
Min, W
English, BP
Luo, GB
Cherayil, BJ
Kou, SC
Xie, XS [1 ]
机构
[1] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA
[2] Harvard Univ, Dept Stat, Cambridge, MA 02138 USA
关键词
D O I
10.1021/ar040133f
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Recent single-molecule enzymology measurements with improved statistics have demonstrated that a single enzyme molecule exhibits large temporal fluctuations of the turnover rate constant at a broad range of time scales (from 1 ms to 100 s). The rate constant fluctuations, termed as dynamic disorder, are associated with fluctuations of the protein conformations observed on the same time scales. We discuss the unique information extractable from these experiments and the reconciliation of these observations with ensemble-averaged Michaelis-Menten equation. A theoretical model based on the generalized Langevin equation (GLE) treatment of Kramers' barrier crossing problem for chemical reactions accounts naturally for the observation of dynamic disorder and highly dispersed kinetics.
引用
收藏
页码:923 / 931
页数:9
相关论文
共 59 条
[1]   Kinesin moves by an asymmetric hand-over-hand mechanism [J].
Asbury, CL ;
Fehr, AN ;
Block, SM .
SCIENCE, 2003, 302 (5653) :2130-2134
[2]   DYNAMICS OF LIGAND-BINDING TO MYOGLOBIN [J].
AUSTIN, RH ;
BEESON, KW ;
EISENSTEIN, L ;
FRAUENFELDER, H ;
GUNSALUS, IC .
BIOCHEMISTRY, 1975, 14 (24) :5355-5373
[3]   Multitime correlation functions for single molecule kinetics with fluctuating bottlenecks [J].
Barsegov, V ;
Chernyak, V ;
Mukamel, S .
JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (10) :4240-4251
[4]   A perspective on enzyme catalysis [J].
Benkovic, SJ ;
Hammes-Schiffer, S .
SCIENCE, 2003, 301 (5637) :1196-1202
[5]   CLASSICAL AND MODERN METHODS IN REACTION-RATE THEORY [J].
BERNE, BJ ;
BORKOVEC, M ;
STRAUB, JE .
JOURNAL OF PHYSICAL CHEMISTRY, 1988, 92 (13) :3711-3725
[6]   Examining noise sources at the single-molecule level:: 1/f noise of an open maltoporin channel [J].
Bezrukov, SM ;
Winterhalter, M .
PHYSICAL REVIEW LETTERS, 2000, 85 (01) :202-205
[7]   Escape through a bottleneck undergoing non-Markovian fluctuations [J].
Bicout, DJ ;
Szabo, A .
JOURNAL OF CHEMICAL PHYSICS, 1998, 108 (13) :5491-5497
[8]   Ten years of tension: single-molecule DNA mechanics [J].
Bustamante, C ;
Bryant, Z ;
Smith, SB .
NATURE, 2003, 421 (6921) :423-427
[9]   Multiple time scale dynamics of distance fluctuations in a semiflexible polymer: A one-dimensional generalized Langevin equation treatment [J].
Debnath, P ;
Min, W ;
Xie, S ;
Cherayil, BJ .
JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (20)
[10]   The fluctuating enzyme:: a single molecule approach [J].
Edman, L ;
Földes-Papp, Z ;
Wennmalm, S ;
Rigler, R .
CHEMICAL PHYSICS, 1999, 247 (01) :11-22