Martínez-Fernández Daniel, Pedrosa Clara, Herranz Miguel, Foteinopoulou Katerina, Karayiannis Nikos Ch, Laso Manuel
Institute for Optoelectronic Systems and Microtechnology (ISOM) and Escuela Técnica Superior de Ingenieros Industriales (ETSII), Universidad Politécnica de Madrid (UPM), C/ Jose Gutierrez Abascal 2, 28006 Madrid, Spain.
J Chem Phys. 2024 Jul 21;161(3). doi: 10.1063/5.0216436.
Through extensive Monte Carlo simulations, we systematically study the effect of chain stiffness on the packing ability of linear polymers composed of hard spheres in extremely confined monolayers, corresponding effectively to 2D films. First, we explore the limit of random close packing as a function of the equilibrium bending angle and then quantify the local and global order by the degree of crystallinity and the nematic or tetratic orientational order parameter, respectively. A multi-scale wealth of structural behavior is observed, which is inherently absent in the case of athermal individual monomers and is surprisingly richer than its 3D counterpart under bulk conditions. As a general trend, an isotropic to nematic transition is observed at sufficiently high surface coverages, which is followed by the establishment of the tetratic state, which in turn marks the onset of the random close packing. For chains with right-angle bonds, the incompatibility of the imposed bending angle with the neighbor geometry of the triangular crystal leads to a singular intra- and inter-polymer tiling pattern made of squares and triangles with optimal local filling at high surface concentrations. The present study could serve as a first step toward the design of hard colloidal polymers with a tunable structural behavior for 2D applications.
通过广泛的蒙特卡罗模拟,我们系统地研究了链刚度对由硬球组成的线性聚合物在极度受限的单层(有效对应于二维薄膜)中的堆积能力的影响。首先,我们探索了随机密堆积极限作为平衡弯曲角的函数,然后分别通过结晶度和向列或四方取向序参数量化局部和全局有序度。观察到了丰富的多尺度结构行为,这在无热单个单体的情况下是固有的,并且令人惊讶地比其在本体条件下的三维对应物更丰富。作为一般趋势,在足够高的表面覆盖率下观察到从各向同性到向列相的转变,随后是四方态的建立,这反过来又标志着随机密堆积的开始。对于具有直角键的链,所施加的弯曲角与三角晶体的相邻几何形状不兼容,导致在高表面浓度下由正方形和三角形组成的奇异的聚合物内和聚合物间平铺图案,具有最佳的局部填充。本研究可作为设计具有可调结构行为的硬胶体聚合物以用于二维应用的第一步。