Theory Department, National Institute of Chemistry, Hajdrihova 19, SI-1001 Ljubljana, Slovenia.
Department of Physics, Faculty of Mathematics and Physics, University of Ljubljana, Jadranska 19, SI-1000 Ljubljana, Slovenia.
J Phys Chem B. 2023 Aug 24;127(33):7231-7243. doi: 10.1021/acs.jpcb.3c02324. Epub 2023 Aug 9.
Proteins are natural polymers that play an essential role in both living organisms and biotechnological applications. During certain bioprocessing steps, they can be exposed to significant mechanical stress induced by, for example, shear flow or sonication, resulting in reduced therapeutic efficacy, aggregation, or even a loss of activity. For this reason, there is a need to understand and determine the susceptibility of the protein activity to the experienced mechanical stress. To acquire this knowledge, it is necessary to study the rotational dynamics of the protein. Commonly, the rotational dynamics of soft molecules is interpreted based on a theoretical analysis performed in an inertial laboratory frame. However, the obtained angular velocity mixes pure rotations and vibrations with angular momentum, consequently lacking a clear dynamical interpretation. On the other hand, the use of the noninertial internal Eckart frame allows the determination of pure angular velocity as it minimizes the coupling between the rotational and vibrational degrees of freedom. In the present work, by conducting open-boundary molecular dynamics simulations and exploiting the Eckart frame formalism, we study the rotational dynamics of a small protein under the shear flow of various strengths. Our results show that the angular velocity increases nonlinearly with increasing shear rate. Furthermore, the protein gains vibrational angular momentum at higher shear rates, which is reflected in the higher angular velocity computed by employing the Eckart frame formalism and confirmed by analysis of the contributions to the total kinetic energy of the biomolecule.
蛋白质是天然聚合物,在生物有机体内和生物技术应用中都起着至关重要的作用。在某些生物处理步骤中,它们可能会受到剪切流或超声等因素引起的显著机械应力的影响,从而导致治疗效果降低、聚集甚至失去活性。出于这个原因,有必要了解并确定蛋白质活性对所经历的机械应力的敏感性。为了获得这些知识,需要研究蛋白质的旋转动力学。通常,基于在惯性实验室框架中进行的理论分析来解释软分子的旋转动力学。然而,所得到的角速度混合了纯旋转和振动与角动量,因此缺乏清晰的动力学解释。另一方面,使用非惯性内部 Eckart 框架可以确定纯角速度,因为它最小化了旋转和振动自由度之间的耦合。在本工作中,通过进行开边界分子动力学模拟并利用 Eckart 框架形式主义,我们研究了在各种强度的剪切流下小蛋白的旋转动力学。我们的结果表明,角速度随剪切率的增加呈非线性增加。此外,在较高的剪切率下,蛋白质获得了振动角动量,这反映在通过采用 Eckart 框架形式主义计算的较高角速度中,并通过分析生物分子总动能的贡献得到了证实。