Santo K P, Sebastian K L
Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore, India.
Phys Rev E Stat Nonlin Soft Matter Phys. 2006 Mar;73(3 Pt 1):031923. doi: 10.1103/PhysRevE.73.031923. Epub 2006 Mar 29.
The dynamics of contact formation between different parts of a long chain molecule is of considerable interest in biology. The related processes of opening of a loop or closing to form a loop also are of considerable interest and have attracted the attention of experimentalists/theorists. For closing, results are available in the completely flexible limit. However, this limit is not realized in many cases. Recently, there have been investigations for the semiflexible case too. We develop an approach, which leads to an easy description of the dynamics, incorporating semiflexibility rigorously into account. With this approach, the dynamics of a semiflexible polymer ring formed by a weak bond between the two ends can be modeled as the escape of a particle over a barrier in a multidimensional potential energy surface. We then calculate the rate of opening using a multidimensional transition state theory. Effects of friction on the rate are also taken into account using the standard coupling to a bath of harmonic oscillators. We find that for shorter chains (i.e., semiflexible), the rate of opening is strongly length dependent and is well described by the equation A(L/lp)v exp(Blp/L), with L as the length, and lp as the persistence length, A, B as the constants, and v approximately 1.2.
长链分子不同部分之间接触形成的动力学在生物学中具有相当大的研究价值。环的打开或闭合形成环的相关过程也备受关注,并吸引了实验人员/理论学家的注意。对于环的闭合,在完全柔性极限情况下已有相关结果。然而,在许多情况下并未达到这一极限。最近,也有针对半柔性情况的研究。我们开发了一种方法,该方法能轻松描述动力学过程,同时严格考虑了半柔性。通过这种方法,由两端之间的弱键形成的半柔性聚合物环的动力学可被建模为粒子在多维势能面上越过势垒的逃逸过程。然后,我们使用多维过渡态理论计算打开速率。还通过与简谐振子浴的标准耦合考虑了摩擦对速率的影响。我们发现,对于较短的链(即半柔性链),打开速率强烈依赖于链长,并且可以用方程(A(L/l_p)^v \exp(B l_p/L))很好地描述,其中(L)为链长,(l_p)为持久长度,(A)、(B)为常数,(v)约为(1.2)。