Fast enzyme dynamics at the active site of formate dehydrogenase

被引：69

作者：

Bandaria, Jigar N. ^{[1
,2
]}

Dutta, Samrat ^{[1
,2
]}

Hill, Sarah E. ^{[1
,2
]}

Kohen, Amnon ^{[1
,2
]}

Cheatum, Christopher M. ^{[1
,2
]}

机构：

[1] Univ Iowa, Dept Chem & Opt Sci, Iowa City, IA 52242 USA

[2] Univ Iowa, Ctr Technol, Iowa City, IA 52242 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2008年 / 130卷 / 01期

关键词：

D O I：

10.1021/ja077599o

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The role of femtosecond-picosecond structural dynamics of proteins in enzyme-catalyzed reactions is a hotly debated topic. We report infrared photon echo measurement of the formate dehydrogenase-NAD(+)-azide ternary complex. In contrast to earlier studies of protein dynamics, the data show complete spectral diffusion on the femtosecond-picosecond time scale with no static heterogeneity. This result indicates that this transition-state analogue complex completely samples the distribution of structures that determine the distribution of azide vibrational frequencies within a few picoseconds and that there are no slower motions that perturb the H-bond network at the active site.

引用

页码：22 / +

页数：3

共 19 条

[1] A perspective on enzyme catalysis [J].

Benkovic, SJ ;

Hammes-Schiffer, S .

SCIENCE, 2003, 301 (5637) :1196-1202

[2] KINETIC AND CHEMICAL MECHANISMS OF YEAST FORMATE DEHYDROGENASE [J].

BLANCHARD, JS ;

CLELAND, WW .

BIOCHEMISTRY, 1980, 19 (15) :3543-3550

[3] Fast protein dynamics probed with infrared vibrational echo experiments [J].

Fayer, MD .

ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2001, 52 :315-356

[4] Ultrafast dynamics of myoglobin without the distal histidine: Stimulated vibrational echo experiments and molecular dynamics simulations [J].

Finkelstein, IJ ;

Goj, A ;

McClain, BL ;

Massari, AM ;

Merchant, KA ;

Loring, RF ;

Fayer, MD .

JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (35) :16959-16966

[5] Substrate binding and protein conformational dynamics measured by 2D-IR vibrational echo spectroscopy [J].

Finkelstein, Ilya J. ;

Ishikawa, Haruto ;

Kim, Seongheun ;

Massari, Aaron M. ;

Fayer, M. D. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2007, 104 (08) :2637-2642

[6] Hydrogen tunneling and protein motion in enzyme reactions [J].

Hammes-Schiffer, S .

ACCOUNTS OF CHEMICAL RESEARCH, 2006, 39 (02) :93-100

[7] VARIATION OF TRANSITION-STATE STRUCTURE AS A FUNCTION OF THE NUCLEOTIDE IN REACTIONS CATALYZED BY DEHYDROGENASES .2. FORMATE DEHYDROGENASE [J].

HERMES, JD ;

MORRICAL, SW ;

OLEARY, MH ;

CLELAND, WW .

BIOCHEMISTRY, 1984, 23 (23) :5479-5488

[8]

Kohen A., 2006, ISOTOPE EFFECTS CHEM, P743

[9] Vibrational spectral diffusion of azide in water [J].

Li, Shuzhou ;

Schmidt, J. R. ;

Piryatinski, A. ;

Lawrence, C. P. ;

Skinner, J. L. .

JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (38) :18933-18938

[10] Approaches for the calculation of vibrational frequencies in liquids: Comparison to benchmarks for azide/water clusters [J].

Li, Shuzhou ;

Schmidt, J. R. ;

Corcelli, S. A. ;

Lawrence, C. P. ;

Skinner, J. L. .

JOURNAL OF CHEMICAL PHYSICS, 2006, 124 (20)

← 1 2 →