Loverde Sharon M, Velichko Yury S, Olvera de la Cruz Monica
Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208-3108, USA.
J Chem Phys. 2006 Apr 14;124(14):144702. doi: 10.1063/1.2181573.
A binary mixture of oppositely charged components confined to a plane such as cationic and anionic lipid bilayers may exhibit local segregation. The relative strengths of the net short range interactions, which favors macroscopic segregation, and the long range electrostatic interactions, which favors mixing, determine the length scale of the finite size or microphase segregation. The free energy of the system can be examined analytically in two separate regimes, when considering small density fluctuations at high temperatures and when considering the periodic ordering of the system at low temperatures [F. J. Solis, S. I. Stupp, and M. Olvera de la Cruz, J. Chem. Phys. 122, 054905 (2005)]. A simple molecular dynamics simulation of oppositely charged monomers, interacting with a short range Lennard-Jones potential and confined to a two dimensional plane, is examined at different strengths of short and long range interactions. The system exhibits well-defined domains that can be characterized by their periodic length scale as well as the orientational ordering of their interfaces. By adding salt, the ordering of the domains disappears and the mixture macroscopically phase segregates in agreement with analytical predictions.
限制在平面内的带相反电荷的二元混合物,如阳离子和阴离子脂质双层,可能会出现局部分离。有利于宏观分离的净短程相互作用和有利于混合的长程静电相互作用的相对强度,决定了有限尺寸或微相分离的长度尺度。当考虑高温下的小密度涨落以及低温下系统的周期性有序排列时,系统的自由能可以在两个不同的区域进行解析研究[F. J. Solis, S. I. Stupp, and M. Olvera de la Cruz, J. Chem. Phys. 122, 054905 (2005)]。研究了一种简单的分子动力学模拟,其中带相反电荷的单体通过短程 Lennard-Jones 势相互作用,并限制在二维平面内,考察了不同短程和长程相互作用强度下的情况。该系统表现出明确的区域,这些区域可以通过其周期性长度尺度以及界面的取向有序性来表征。通过添加盐,区域的有序性消失,混合物宏观相分离,这与解析预测一致。