Polaron States in Fullerene Adducts Modeled by Coarse-Grained Molecular Dynamics and Tight Binding.
Polaron States in Fullerene Adducts Modeled by Coarse-Grained Molecular Dynamics and Tight Binding.
复制标题
通过粗粒分子动力学和紧结合建模的富勒烯加合物中的极化子态。
DOI：
10.1021/acs.jpclett.8b02320
复制
发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Rice B
中科院分区：
文献类型：
--
作者：
Rice B
强电子-声子耦合导致分子半导体材料中的极化子局域化并影响电荷传输，但原子计算成本昂贵。在这里，我们提出了一个简单而有效的模型来确定无序分子膜的粗粒度表示内极化子态的能量和空间范围。我们使用紧束缚哈密顿量计算分子组装体的电子结构，并通过周围介质对电荷的介电响应扰动位点能量来自洽地确定极化子状态。当应用于富勒烯衍生物时，该方法表明，由于堆积无序和极性侧链，极化子在 C60 中延伸到多个分子，但在苯基-C61-丁酸甲酯 (PCBM) 的高级加合物中局限于单个分子。在 PCBM 中，仅当包含能量无序或富勒烯分散在混合物中时，极化子才会定位在单个分子上。该方法有助于建立跳跃传输模型合理性的条件。
Strong electron–phonon coupling leads to polaron localization in molecular semiconductor materials and influences charge transport, but it is expensive to calculate atomistically. Here, we propose a simple and efficient model to determine the energy and spatial extent of polaron states within a coarse-grained representation of a disordered molecular film. We calculate the electronic structure of the molecular assembly using a tight-binding Hamiltonian and determine the polaron state self-consistently by perturbing the site energies by the dielectric response of the surrounding medium to the charge. When applied to fullerene derivatives, the method shows that polarons extend over multiple molecules in C60 but localize on single molecules in higher adducts of phenyl-C61-butyric-acid-methyl-ester (PCBM) because of packing disorder and the polar side chains. In PCBM, polarons localize on single molecules only when energetic disorder is included or when the fullerene is dispersed in a blend. The method helps to establish the conditions under which a hopping transport model is justified.
影响因子：
5.7
作者：
Gajdos, Fruzsina;Oberhofer, Harald;Blumberger, Jochen
通讯作者：
Blumberger, Jochen
DOI：
10.1021/acs.jpclett.8b01112
发表时间：
2018-06-07
期刊：
The journal of physical chemistry letters
影响因子：
--
作者：
Giannini S;Carof A;Blumberger J
通讯作者：
Blumberger J
影响因子：
3.3
作者：
Oberhofer, Harald;Blumberger, Jochen
通讯作者：
Blumberger, Jochen