Single-molecule dynamics of semiflexible Gaussian chains

被引:24
作者
Yang, SL [1 ]
Witkoskie, JB [1 ]
Cao, JS [1 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
关键词
D O I
10.1063/1.1521156
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A semiflexible Gaussian chain model is used to determine the statistics and correlations of single-molecule fluorescence resonant energy transfer (FRET) experiments on biological polymers. The model incorporates a persistence length in a Rouse chain and describes single-chain dynamics with normal modes. The hydrodynamic interaction is included in the dynamics of the semiflexible Gaussian chain on the preaveraging level. The distribution functions of the fluorescence lifetime and the FRET efficiency provide direct measures of the chain stiffness, and their correlation functions probe the intrachain dynamics at the single-molecule level. When measured with finite time resolution, the instantaneous diffusion coefficient for FRET is much smaller in the collapsed structure than in the coiled structure, and the variation has a quadratic dependence on the donor-acceptor distance. In the fast reaction limit, single-molecule FRET lifetime measurements can be used to map out the equilibrium distribution function of interfluorophore distance. As an example of microrheology, the intrinsic viscoelasticity can be extracted from single-molecule tracking of the Brownian dynamics of polymers in solution. (C) 2002 American Institute of Physics.
引用
收藏
页码:11010 / 11023
页数:14
相关论文
共 51 条
[1]  
[Anonymous], ADV CHEM PHYS, DOI [10.1002/9780470143728, DOI 10.1002/9780470143728.CH1]
[2]  
BACHE T, 1996, SINGLE MOL OPTICAL D
[3]   Theory of single-molecule fluorescence spectroscopy of two-state systems [J].
Berezhkovskii, AM ;
Szabo, A ;
Weiss, GH .
JOURNAL OF CHEMICAL PHYSICS, 1999, 110 (18) :9145-9150
[4]   The speed limit for protein folding measured by triplet-triplet energy transfer [J].
Bieri, O ;
Wirz, J ;
Hellrung, B ;
Schutkowski, M ;
Drewello, M ;
Kiefhaber, T .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1999, 96 (17) :9597-9601
[5]   DYNAMICS OF POLYMER MOLECULES IN DILUTE-SOLUTIONS [J].
BIXON, M .
JOURNAL OF CHEMICAL PHYSICS, 1973, 58 (04) :1459-1466
[6]   HYDRODYNAMIC INTERACTION AND DYNAMIC INTRINSIC-VISCOSITY OF A FLEXIBLE POLYMER [J].
BIXON, M ;
ZWANZIG, R .
JOURNAL OF CHEMICAL PHYSICS, 1978, 68 (04) :1890-1895
[7]   Two-point microrheology of inhomogeneous soft materials [J].
Crocker, JC ;
Valentine, MT ;
Weeks, ER ;
Gisler, T ;
Kaplan, PD ;
Yodh, AG ;
Weitz, DA .
PHYSICAL REVIEW LETTERS, 2000, 85 (04) :888-891
[8]   Single-molecule protein folding: Diffusion fluorescence resonance energy transfer studies of the denaturation of chymotrypsin inhibitor 2 [J].
Deniz, AA ;
Laurence, TA ;
Beligere, GS ;
Dahan, M ;
Martin, AB ;
Chemla, DS ;
Dawson, PE ;
Schultz, PG ;
Weiss, S .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2000, 97 (10) :5179-5184
[9]   Time-dependent optical linewidth in fluctuating environments: Stochastic models [J].
Diezemann, G .
JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (04) :1647-1657
[10]  
Doi M., 1986, The Theory of Polymer Dynamics