Freund L B
Division of Engineering, Brown University, 184 Hope Street, Providence, RI 02912-9104, USA.
Proc Natl Acad Sci U S A. 2009 Jun 2;106(22):8818-23. doi: 10.1073/pnas.0903003106. Epub 2009 Apr 29.
The goal of measurements of the resisting force generated by a molecular bond as it is being forcibly separated under controlled conditions is to determine functional characteristics of the bond. Here, we establish the dependence of force history during unbinding on both those parameters chosen to characterize the bond itself and the controllable loading parameters. This is pursued for the practical range of behavior in which unbinding occurs diffusively rather than ballistically, building on the classic work of Kramers. For a bond represented by a one-dimensional energy landscape, modified by a second time-dependent energy profile representing applied loading, we present a mathematical analysis showing the dependence of the resistance of the bond-on-bond well shape, general time dependence of the imposed loading, and stiffness of the loading apparatus. The quality of the result is established through comparison with full numerical solutions of the underlying Smoluchowski equation.
在可控条件下,当分子键被强行分离时,测量其产生的阻力的目的是确定该键的功能特性。在此,我们确定了在解离过程中力的历史与所选的用于表征键本身的参数以及可控加载参数之间的依赖关系。这是基于克拉默斯的经典工作,针对解离以扩散而非弹道方式发生的实际行为范围进行的研究。对于由一维能量景观表示的键,通过表示施加负载的第二个随时间变化的能量分布进行修改,我们给出了数学分析,展示了键的阻力与键阱形状、施加负载的一般时间依赖性以及加载装置刚度之间的依赖关系。通过与基础的斯莫卢霍夫斯基方程的完整数值解进行比较,确定了结果的质量。