Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
J Phys Chem B. 2011 Mar 3;115(8):1792-7. doi: 10.1021/jp1114527. Epub 2011 Feb 3.
We present large-scale calculations of electronic structure of strongly disordered conjugated polymers. The calculations have been performed using the density functional theory based charge patching method for the construction of single-particle Hamiltonian and the overlapping fragments method for the efficient diagonalization of that Hamiltonian. We find that the hole states are localized due to the fluctuations of the electrostatic potential and not by the breaks in the conjugation of the polymer chain. The tail of the density of hole states exhibits an exponentially decaying behavior. The main features of the electronic structure of the system can be described by an one-dimensional nearest neighbor tight-binding model with a correlated Gaussian distribution of on-site energies and constant off-site coupling elements.
我们呈现了强无序共轭聚合物的电子结构的大规模计算。这些计算是使用基于密度泛函理论的电荷补丁方法来构建单粒子哈密顿量，并使用重叠片段方法来有效地对角化该哈密顿量。我们发现，空穴态由于静电势的涨落而局域化，而不是由于聚合物链的共轭中断。空穴态密度的尾部表现出指数衰减行为。该系统的电子结构的主要特征可以用一个一维最近邻紧束缚模型来描述，该模型具有局域能的相关高斯分布和常数的非局域耦合元素。
