Experimental free energy surface reconstruction from single-molecule force spectroscopy using Jarzynski's equality

被引:161
作者
Harris, Nolan C. [1 ]
Song, Yang [1 ]
Kiang, Ching-Hwa [1 ]
机构
[1] Rice Univ, Dept Phys & Astron, Houston, TX 77005 USA
关键词
D O I
10.1103/PhysRevLett.99.068101
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
We used the atomic force microscope to manipulate and unfold individual molecules of the titin I27 domain and reconstructed its free energy surface using Jarzynski's equality. The free energy surface for both stretching and unfolding was reconstructed using an exact formula that relates the nonequilibrium work fluctuations to the molecular free energy. In addition, the unfolding free energy barrier, i.e., the activation energy, was directly obtained from experimental data for the first time. This Letter demonstrates that Jarzynski's equality can be used to analyze nonequilibrium single-molecule experiments, and to obtain the free energy surfaces for molecular systems, including interactions for which only nonequilibrium work can be measured.
引用
收藏
页数:4
相关论文
共 31 条
[1]   A simple method for probing the mechanical unfolding pathway of proteins in detail [J].
Best, RB ;
Fowler, SB ;
Toca-Herrera, JL ;
Clarke, J .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2002, 99 (19) :12143-12148
[2]   Mechanical processes in biochemistry [J].
Bustamante, C ;
Chemla, YR ;
Forde, NR ;
Izhaky, D .
ANNUAL REVIEW OF BIOCHEMISTRY, 2004, 73 :705-748
[3]   Mechanical and chemical unfolding of a single protein: A comparison [J].
Carrion-Vazquez, M ;
Oberhauser, AF ;
Fowler, SB ;
Marszalek, PE ;
Broedel, SE ;
Clarke, J ;
Fernandez, JM .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1999, 96 (07) :3694-3699
[4]   Verification of the Crooks fluctuation theorem and recovery of RNA folding free energies [J].
Collin, D ;
Ritort, F ;
Jarzynski, C ;
Smith, SB ;
Tinoco, I ;
Bustamante, C .
NATURE, 2005, 437 (7056) :231-234
[5]   Intrinsic rates and activation free energies from single-molecule pulling experiments [J].
Dudko, OK ;
Hummer, G ;
Szabo, A .
PHYSICAL REVIEW LETTERS, 2006, 96 (10)
[6]   RNA structure - Pulling on hair(pins) [J].
Fernandez, JM ;
Chu, S ;
Oberhauser, AF .
SCIENCE, 2001, 292 (5517) :653-654
[7]   Using nonequilibrium measurements to determine macromolecule free-energy differences [J].
Fox, RF .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2003, 100 (22) :12537-12538
[8]   Biological physics [J].
Frauenfelder, H ;
Wolynes, PG ;
Austin, RH .
REVIEWS OF MODERN PHYSICS, 1999, 71 (02) :S419-S430
[9]   Autoionization in liquid water [J].
Geissler, PL ;
Dellago, C ;
Chandler, D ;
Hutter, J ;
Parrinello, M .
SCIENCE, 2001, 291 (5511) :2121-2124
[10]   Mechanisms of protein folding [J].
Grantcharova, V ;
Alm, EJ ;
Baker, D ;
Horwich, AL .
CURRENT OPINION IN STRUCTURAL BIOLOGY, 2001, 11 (01) :70-82